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Theory of intense laser-matter interaction

D. Bauer

**Max-Planck-Institut für Kernphysik, Heidelberg, Germany
**

dieter.bauer@mpi-hd.mpg.de

June 22, 2006

2

Contents

1 2 Introduction Classical motion in electromagnetic ﬁelds 2.1 The nonrelativistic ponderomotive force . . . . . . . . . 2.1.1 The ponderomotive force of a standing wave . . 2.2 Relativistic dynamics in an electromagnetic wave . . . . 2.2.1 The oscillation center frame . . . . . . . . . . . . . 2.2.2 The adiabatically ramped pulse in the lab frame 2.3 The relativistic ponderomotive force . . . . . . . . . . . . 2.3.1 Example: sin2 -pulse . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 5 9 9 11 14 17 19 21 24 27 27 32 37 42 42 47 50 56 61 62 67 71 76 81 82 84 86 89 95

3

Atoms in external ﬁelds 3.1 Atomic units . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 3.2 Time-dependent perturbation theory . . . . . . . . . . . . . . . . . . . . . . . 3.2.1 Dyson series, S-matrix, Green’s functions, propagators, and resolvents . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 3.3 Important models . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 3.3.1 Discrete level coupled to the continuum . . . . . . . . . . . . . . . . 3.3.2 Resonantly coupled discrete levels: Rabi-oscillations . . . . . . . . 3.4 Atoms in strong, static electric ﬁelds . . . . . . . . . . . . . . . . . . . . . . . 3.4.1 Tunneling ionization . . . . . . . . . . . . . . . . . . . . . . . . . . . . 3.5 Atoms in strong laser ﬁelds . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 3.5.1 Floquet formalism . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 3.5.2 Non-Hermitian Floquet theory . . . . . . . . . . . . . . . . . . . . . 3.5.3 High-frequency Floquet theory and stabilization . . . . . . . . . . 3.6 Strong ﬁeld approximation . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 3.6.1 Circular polarization and long pulses . . . . . . . . . . . . . . . . . . 3.6.2 Channel closing in above-threshold ionization . . . . . . . . . . . . 3.6.3 Linear polarization and long pulses . . . . . . . . . . . . . . . . . . . 3.6.4 Few-cycle above-threshold ionization . . . . . . . . . . . . . . . . . . 3.6.5 “Simple man’s theory” . . . . . . . . . . . . . . . . . . . . . . . . . . . 3.6.6 High harmonic generation . . . . . . . . . . . . . . . . . . . . . . . .

3

4

CONTENTS

Chapter 1 Introduction

In this lecture we shall try to answer the questions — “What happens if we put electrons, atoms, molecules, clusters, solids, plasmas etc. in an intense laser pulse?” — “What is the new physics there?” — “What are the new theoretical methods to deal with the problem?” — “What is it good for?” Theoretical research in this area has been strongly motivated by the rapid progress in laser technology over the last twenty years, and there are good reasons to believe that this progress continues. The main goals are to achieve 1. higher laser pulse peak intensities, 2. shorter pulses, 3. shorter wavelengths. The demand for higher and higher laser pulse intensities is driven by, e.g., inertial conﬁnement fusion (i.e., nuclear fusion using lasers), “table top” particle acceleration, or particle physics (e.g., particle creation in vacuum using lasers). Shorter pulses are needed to study fast atomic processes directly in the time domain. Just as femtosecond (1 fs = 10−15 = 0.000 000 000 000 001 s) laser technology revolutionized chemistry, the hope is that attosecond (1 as = 10−18 s) laser pulses give a new twist on good old atomic physics. First, successful “proof of principle”-like experiments have been already carried out. The shortness of these kind of laser pulses is impressively illustrated by the comparison 8 min 1 fs . (1.1) 1s age of the universe 5

6

CHAPTER 1. INTRODUCTION

Table 1.1: Comparison between a strong laser and sunlight.

ﬁeld strength [V/m] intensity [W/cm2 ] excursion [Å] ponderom. [eV] potential (at 800 nm) 2169.2 8 · 10−15

strong laser sun

5.14 · 1011 1000

3.51 · 1016 0.13

163 3.3 · 10−7

Finally, shorter wavelength lasers are desirable to complement (or to offer a cheaper alternative to) synchrotron radiation sources with a vast amount of applications in material and biological sciences. Moreover, shorter wavelengths λ and shorter pulse durations are related since a lower limit for the pulse duration is the laser period 2π/ω where ω = 2πc/λ is the laser frequency. What do we mean by strong or intense when we talk about laser pulses? Whether a laser pulse has to be considered strong or not depends on the force it exerts as compared to other, competing forces. These other forces are typically the binding forces that prevents the target from falling apart (even without laser). A good example is the force that is “seen” by an electron on its ﬁrst Bohr orbit in the hydrogen atom. This force is F = −eEH (1.2)

where |EH | = 5.14 · 1011 V/m is the electric ﬁeld due to the attraction of electron and proton. This electric ﬁeld can be directly compared with the electric ﬁeld of a laser pulse ˆ E (r , t ) = E ei(ωt −k·r ) , (1.3)

and the latter is at latest to be considered strong if it equals the binding force. The laser intensity is deﬁned as the cycle-averaged modulus of the Poynting vector, 1 ˆˆ I = c 2 0 |E (t ) × B(t )| = c 0 E E ∗ . 2 (1.4)

Here we use SI units and the relation between the electric ﬁeld and the magnetic ﬁeld B for an electromagnetic wave in vacuum. The unit of the intensity I is that of an energy ﬂux, namely W/cm2 , which is energy passing through an area per time. Plugging in EH yields I = 3.51 · 1016 Wcm−2 . This sounds a lot, especially if compared to sunlight on earth (cf. Table 1.1). However, for current laser technology it is rather peanuts, for 1017 Wcm−2 are routinely achieved in many laboratories around the world while 1022 Wcm−2 seems to be the maximum achieved so far. The other entries in Table 1.1 will be referred to later on. The shortest pulses generated so far consist of only a few cycles in the “full width half maximum” (FWHM) of the pulse at λ = 800 nm. The laser period for this TitaniumSapphire laser wavelength is T 2.7 fs so that the pulse duration is about 5 fs for these

7 shortest laser pulses. During such a short time light travels only a distance of 1.5 µm in vacuum so that these pulses are not laser beams but rather laser light bullets of a few wavelengths width. The pulse duration determines the time scale which can be resolved directly in the time domain. Since atomic processes occur on the attosecond time scale (except phenomena involving mainly Rydberg states), 5 fs pulses are still too long do resolve them. However, in combination with shorter wavelength pulses of attosecond duration which can be generated by the 800 nm pulse itself via high harmonic generation, femtosecond laser pulses have been already used to study experimentally attosecond atomic processes such as the Auger decay. So far, few-cycle laser pulses were only generated at rather modest laser intensities below 1018 Wcm−2 . The most intense pulses with an intensity of 1020 Wcm−2 or higher are of picosecond (1 ps = 10−12 s) duration or longer. It is instructive to calculate the power and the energy of such a, e.g., 10 ps pulse if it is focused down to, say, (10 µm)2 : 1020 Wcm−2 · (10 µm)2 = 0.1 PW where PW stands for petawatt (1015 W), and 0.1 PW · 10 ps = 1 kJ. (1.6) (1.5)

Currently, megajoule lasers are being constructed in several laboratories around the world. The light pressures such pulses exert are enormous. From Eq. (1.7) below we estimate pressures of the order of 10 Gigabar. Since dimensionally, pressure is an energy density, another way of estimating the pressure is 1 kJ/[(10 µm)2 · c ·10 ps], which yields the same answer. Such pressures even exceed those in the interior of stars and may offer the opportunity to study the equation of state of various materials under extreme conditions. At this point we do not want to hide that such research is of interest to military, and, in fact, was previously carried out (with limited success) employing underground nuclear explosions. The newly constructed “national ignition facility” (NIF) in the US aims at those aspects of intense laser-matter interaction. Coming back from “boom-boom”-physics to theory, experience shows that standard, quantum mechanical, perturbative approaches start to fail already around 1013 Wcm−2 when applied to the ionization of atomic hydrogen in a laser ﬁeld, for instance. The new analytical techniques that have been developed (as well as those still lacking) will be topics of this lecture. Many things become more complicated in strong laser ﬁelds, however, some others are getting simpler. There is, for instance, no need to quantize the electromagnetic ﬁeld. Moreover, many of the new effects observed, such as the plateaus in photoelectron or harmonics spectra and nonsequential double ionization, although utterly unaccessible in terms of standard perturbation theory, turned out to have rather simple, almost classical explanations. These effects and their theoretical explanation will be also part of this lecture. Finally, there is the relativistic domain which separates the strong laser ﬁelds from the ultra-strong ones. In the case of a free electron in a laser pulse there is no binding

8

CHAPTER 1. INTRODUCTION

force to compete with. However, there are strong ﬁeld effects as well. Already at moderate laser intensities the so-called ponderomotive force is appreciable, depending on the pulse shape. Ponderomotive effects will be discussed in quite some detail and reappear frequently during the course of this lecture; in brief: the ponderomotive force in general pushes charged particles out of regions of high intensity (i.e., the laser focus) and exerts pressure on the target. In fact, the light pressure pl = (1 + R) I c (1.7)

(where R is the reﬂectivity and c is the velocity of light in vacuum) can be linked to the ponderomotive force. The ponderomotive force is related to the breakdown of the so-called dipole approximation ˆ E (r , t ) = E e−i(ωt −k·r ) ˆ E e−iωt = E (t ) (1.8)

where the spatial dependence of the ﬁeld is neglected because the wavelength is so much larger than the excursion r (t ) of, say, an electron in the ﬁeld. The classical motion of the electron is governed by the Lorentz force (SI units) ˙ p = −e[E (r , t ) + v × B(r , t )] (1.9)

(where p, v are the electron momentum and velocity, respectively). Making the dipole approximation implies the omittance of the magnetic ﬁeld so that there is no v × Bforce. Hence, the electron is assumed to just oscillate in laser polarization direction (or in the plane of polarization directions if elliptically polarized light is used). However, the velocity of this oscillatory motion increases with the laser intensity and, since the v × B-force is a v/c-effect, from a certain laser intensity on there is no excuse anymore for neglecting it. This threshold intensity depends on the laser wavelength, and for the commonly used 800 nm it turns out to be of the order of 1018 Wcm−2 . The v × B-force is a v/c effect and as such not yet relativistic. Truly relativistic effects are of order (v/c)2 or higher and will be discussed in the last part of this lecture.

**Chapter 2 Classical motion in electromagnetic ﬁelds
**

In this Chapter we shall derive the non-relativistic ponderomotive force and the relativistic equations of motion for a charged particle in a laser pulse of arbitrary intensity. For the case of a travelling wave we also derive the relativistic ponderomotive force.

**2.1 The nonrelativistic ponderomotive force
**

The Lorentz-force on a particle of charge q is given by (SI units) F = q[E (r , t ) + v × B(r , t )]. (2.1)

This force is also relativistically correct. In our case we have in mind E and B making up the electromagnetic ﬁeld of a laser pulse, that is, ˆ E (r , t ) = E (r , t )eiωt and, because of ∇ × E = −∂ t B, B(r , t ) = i ω ∇ × E (r , t ), (2.3) (2.2)

but the derivation also holds for longitudinal waves as they occur in plasmas. The derivation of the ponderomotive force relies on the possibility to separate the relevant time scales: the “fast” motion on the time scale of the laser period 2π/ω and a “secular” ˆ one due to the ponderomotive force. Hence we assume that E (r , t ), apart from containing e−ik·r , describes the laser ﬁeld envelope, having only a “slow” time dependence so that ∂ t B = iωB to high accuracy. In lowest order the particle just oscillates around its current position r0 due to the ˆ electric ﬁeld (the possible slow time-dependence in E is suppressed for notational convenience): ˆ ¨ m r1 = q E (r0 )eiωt . (2.4) 9

10

CHAPTER 2. CLASSICAL MOTION IN ELECTROMAGNETIC FIELDS

The corresponding velocity and position are ˙ r1 = − iq mω ˆ E (r0 )eiωt , r1 = − q mω 2 ˆ E (r0 )eiωt . (2.5)

In the next higher order one has ¨ ˙ m r2 = q[(r1 · ∇)E (r0 , t ) + r1 × B(r0 , t )] (2.6)

where the electric ﬁeld has been expanded around r0 . So far we used complex ﬁelds and implicitly understood that the real part has to be taken. Now the calculation becomes nonlinear and this trick is not applicable anymore. Hence we write ¨ m r2 = q − + q 4mω q

2

ˆ ˆ ˆ ˆ (E e+ + E ∗ e− ) · ∇(E e+ + E ∗ e− )

(2.7)

4mω q2 ˆ ˆ ˆ ˆ [E · ∇E ∗ + E × ∇ × E ∗ + c.c. + Ω2ω ] = − 2 4mω

2

ˆ ˆ ˆ ˆ (−iE e+ + iE ∗ e− ) × ∇ × (iE e+ − iE ∗ e− ) (2.8)

with e± = e±iωt and Ω2ω collecting all terms ∼ e±i2ωt which disappear upon averaging over a laser period, ¨ m r2 = − Using the identity C × ∇ × D + D × ∇ × C + C · ∇D + D · ∇C = ∇C · D we ﬁnally obtain the nonrelativistic ponderomotive force ¨ Fp = m r2 = − q2 4mω

2

q2 4mω 2

ˆ ˆ ˆ ˆ [E · ∇E ∗ + E × ∇ × E ∗ + c.c.].

(2.9)

(2.10)

ˆ ∇|E (r , t )|2 .

(2.11)

ˆ In E (r , t ) the position r now refers to the so-called oscillation center. We remind that the time dependence of the envelope must be “slow” as compared to the laser period because otherwise the separation of time-scales used in the derivation makes no sense. The ponderomotive force (2.11) can obviously be derived from the ponderomotive potential Φp (r , t ) = q2 4mω

2

ˆ |E (r , t )|2

(2.12)

which is proportional to the laser intensity and independent of the sign of the particle’s charge: it is always repulsive. Hence all charged particles are expelled from regions

2.1. THE NONRELATIVISTIC PONDEROMOTIVE FORCE

11

of high laser intensity (e.g., the laser focus). However, owing to the mass m in the denominator the immediate effect on electrons is much larger than on ions. The ponderomotive force is inverse proportional to the square of the laser frequency, meaning that its signiﬁcance increases with increasing laser wavelength. In order for the derivation being valid, the particle must not oscillate “too much” around r0 . More precisely, the conditions read |˙1 | r c, k · r1 1 (2.13)

for an electromagnetic wave and a longitudinal wave, respectively. The condition for the electromagnetic wave is exactly the same indicating the breakdown of the dipole approximation (1.8). As a consequence, (2.12) is not applicable to relativistically intense laser pulses. We shall derive in the subsequent Section the relativistic expression for the ponderomotive force of a laser pulse. The ponderomotive potential (at a certain position r ) equals the average quiver en˙ ergy of the charged particle in the laser ﬁeld (at that position). In fact, taking r1 from (2.5) yields 1 q2 ˆ ˙ Up = m r1 2 = |E |2 . (2.14) 2 2 4mω Is there a connection between this mere number Up and the potential Φp ? Consider a spatially ﬁnite ﬁeld structure which leads to Φp . Now, think of a particle injected into this structure with some kinetic energy W0 . While strolling through the ﬁeld structure the particle will encounter regions of varying Φp . In regions of high Φp it will oscillate with larger amplitude (high Up ) than in regions of low Φp (low Up ). After averaging out the fast time scales, the whole system is conservative so that W + Up = W0 . This means that the local Up indeed serves as a potential and is just the Φp derived above.

**2.1.1 The ponderomotive force of a standing wave
**

Let us consider the standing wave ˆ ˆ E (r , t ) = E eiωt (e−i k·r + ei k·r ) = 2E eiωt cos(k · r ). Comparing this with (2.2) we identify ˆ ˆ E (r , t ) = 2E cos(k · r ) and can immediately use expressions (2.11) and (2.12) to give Φp (r , t ) = ˆ q 2 |E |2 mω 2 cos (k · r ),

2

(2.15)

(2.16)

Fp (r , t ) =

ˆ q 2 |E |2 mω 2

k sin(2k · r ).

(2.17)

The ponderomotive force will push the particle towards the nodes of the standing wave where the ﬁeld vanishes. Depending on its initial velocity, the particles may be trapped

12

CHAPTER 2. CLASSICAL MOTION IN ELECTROMAGNETIC FIELDS

Figure 2.1: Trajectories of an electron in a standing laser wave (2.15) (polarized along ey , propagation directions along e x ) that starts at t = 0 from y = 0 and k x = π/40. The amplitudes were ˆ ˆ e A/mc = −e E/mωc = −0.1 (upper left), −0.2 (upper right), and −0.5 (lower). With increasing laser intensity, the electron is able to escape from the “valley” in which it is released. It can then be trapped temporarily in other valleys (upper right and lower plot), and the dynamics can be shown to become chaotic.

inside the “valleys” of the standing wave. If we assume that the propagation direction is e x and expand the force around the position of a node, we obtain a ponderomotive force of the form ˆ 2q 2 |E|2 . (2.18) Fp“valley −Ω2 x, Ω2 = mc 2 The trapped particle will thus undergo harmonic secular motion with a frequency Ω that is proportional to the electric ﬁeld (which reminds of the Rabi-frequency in resonant laser-atom interaction, to be discussed later on). However, since the frequency increases with the ﬁeld strength, the whole idea of separation of time scales breaks down at some point. In fact, the numerical solution of the (relativistic) equations of motion shows that for sufﬁciently high ﬁeld strengths the particle may leave the valley in which it was trapped. The motion can be shown to be chaotic then. The particle may be temporarily trapped in other valleys, leaving them again, and strolling around erratically (cf. Fig. 2.1). It is clear from the ponderomotive force (2.17) that a standing wave pattern may be used as a grating with a separation of “slits” that is half a laser wavelength (Kapitza-Dirac

2.1. THE NONRELATIVISTIC PONDEROMOTIVE FORCE

13

effect). Particles injected perpendicular to the propagation direction of the two laser beams will be deﬂected. If the de Broglie wavelength is chosen properly, a detector on the opposite side will measure an interference pattern.

Some remarks

In the physics of laser-matter interaction, the importance of the ponderomotive potential is hard to overestimate. In many effects it sets the relevant energy scale, as we shall see later on. In laser-atom interaction, for instance, Φp (r , t ) determines not only the cut-offs of photoelectron and harmonics spectra but also equals the AC Stark-shift of the continuum. In laser-plasma physics, instabilities can be understood in terms of the ponderomotive force. As a historical side remark it should be mentioned that the ponderomotive force has been re-invented several times in the literature although it is derived already in Landau & Lifshitz’s Mechanics volume. Ponderomotive forces can be also derived for more complex systems than classical, point-like particles. An instructive example (and a good exercise) is to calculate the ponderomotive force on two charged particles bound together by a linear force (i.e., a harmonic oscillator). Such particles with internal degrees of freedom may display ˆ counter-intuitive behavior, for instance, acceleration into regions of high |E |2 rather than repulsion from them. Such kind of ponderomotive forces are used to trap neutral atoms in standing laser ﬁelds or other electromagnetic ﬁelds (“optical traps”) or for “optical tweezers”. What we did in this Section in order to obtain a potential for the oscillation center is done in the physics of magnetized plasmas for the so-called guiding center. In the same way we got rid of the fast but uninteresting oscillations on the time scale of a laser period (and twice the laser period), the fast cyclotron motion around the ﬁeld lines of a strong magnetic ﬁeld is eliminated, and what remains is the equation of motion of the “guiding center”. The method of separation of time scales was originally invented for the study of celestial mechanics. This is also where the term secular motion comes from. The effect of Jupiter on the earth’s motion around the sun, for instance, is negligible on the time scale of a few years but may have to be taken into account on longer time scales. One practical advantage of the separation of time scales is for numerical simulations. Imagine you want to simulate one second of the laser plasma dynamics using a ﬂuid code. All effects you are interested in happen on the time scale of, say, microseconds or longer. However, there is this oscillatory motion in the laser ﬁeld on a ten order of magnitude shorter time scale. Resolving this with the ﬂuid code would lead to run-times of years. However, all you need are the secular effects generated by the laser pulse. The ponderomotive potential comes to your rescue: there only the laser pulse envelope enters while the time scales of the laser period (and faster) are eliminated.

14

CHAPTER 2. CLASSICAL MOTION IN ELECTROMAGNETIC FIELDS

Problem 1.1 Calculate the ponderomotive force of an elliptically polarized laser pulse.

2.2

Relativistic dynamics of a charged particle in an electromagnetic wave

Let us consider the motion of a particle of charge q and mass m in an electromagnetic ﬁeld of the form ˆ A(r , t ) = Aσ(η) (η), η = ωt − k · r = k µ xµ , A · k = 0. (2.19)

ˆ Here, A(r , t ) is the vector potential of amplitude A, σ(η) carries the fast timedependence, and (η) is the slowly varying envelope. The phase η is a relativistic invariant, as it is evident from η = k µ xµ where we use common relativistic notation (µ = 0, 1, 2, 3), x µ = (c t , r ), k µ = (ω/c, k), the sum convention, and the metric g = diag(1, −1, −1, −1). The ﬁelds are E = −∂ t A, B = ∇ × A. (2.20)

There are various ways to solve the equations of motion for a charged particle in the ﬁeld (2.19). A particularly elegant method is used in Landau & Lifshitz’s Classical Theory of Fields, based on the relativistic Hamilton-Jacobi equation. The relativistic Hamiltonian governing the motion of a charged particle in an electromagnetic ﬁeld given by the scalar potential φ and the vector potential A reads H = c2 m 2 c 2 + (P − qA)2 + qφ. (2.21)

Here, P is the canonical momentum (while p = P − qA is the kinetic momentum). As in the derivation of the Klein-Gordon equation we square (2.21) and obtain 1 c2 (H − qφ)2 = m 2 c 2 + (P − qA)2 . (2.22)

The goal of the Hamilton-Jacobi method is to ﬁnd a generating function S, called action, for a canonical transformation to new, constant variables. These constant variables are

2.2. RELATIVISTIC DYNAMICS IN AN ELECTROMAGNETIC WAVE

15

then used to fulﬁll the initial conditions. The action S, depending on the “old” positions (+ time) and the new canonical momenta (+ energy) has to be chosen such that = H = −∂ t S, Plugging this into (2.22) yields (∂c t S + qφ/c)2 = m 2 c 2 + (∇S − qA)2 . (2.24) P = ∇S. (2.23)

This expression can be written in a covariant manner. Introducing the four vectors ∂ µ S = (∂c t S, −∇S) = (− /c, −P) =: −P µ and Aµ = (φ/c,A), eq. (2.24) can be written as gµν (∂ µ S + qAµ )(∂ ν S + qAν ) = m 2 c 2 . (2.27) (2.26) (2.25)

We are interested in the dynamics of a charged particle in an electromagnetic wave and therefore have Aµ = (0,A), Aµ kµ = 0. (2.28) With the Ansatz S = Sfree + Sfield (η) = βµ x µ + Sfield (η) where the βµ play the role of the new, constant momenta (+ energy), we obtain ∂µ S = βµ + ∂µ Sfield = βµ + ∂µ η ∂ Sfield ∂η = βµ + kµ Sfield (2.30) (2.29)

where Sfield = ∂η Sfield . The Ansatz with Sfield depending only on the invariant phase η but not on space and time separately is crucial. The fact that it works makes the problem soluble at all. Plugging (2.30) into (2.27) leads to (βµ + kµ Sfield + qAµ )(βµ + k µ Sfield + qAµ ) = m 2 c 2 . Making use of kµ k µ = 0 and Aµ k µ = 0, this equation can be solved for Sfield : Sfield (η) = 1 2βµ k µ

η

(2.31)

dη

η0

m 2 c 2 − [βµ + qAµ (η )][βµ + qAµ (η )]

(2.32)

16

CHAPTER 2. CLASSICAL MOTION IN ELECTROMAGNETIC FIELDS

**and the total action thus is S = βµ x + = βµ x µ +
**

µ

1 2βµ k µ 1 2βµ k µ

η

dη

η0 η

m 2 c 2 − [βµ + qAµ (η )][βµ + qAµ (η )]

(2.33)

dη

η0

m 2 c 2 − βµ βµ − 2qβµ Aµ (η ) − q 2 Aµ (η )Aµ (η ) .

The new, constant four-momentum fulﬁlls βµ βµ = m 2 c 2 (2.34)

and is given through the initial conditions. The canonical four-momentum is given by [making use also of (2.34)] P = −∂ S = −β +

µ µ µ

2qβ · A(η) + q 2 A(η) · A(η) 2β · k

kµ

(2.35)

with a·b = aµ b µ . The derivatives of the action (2.33) with respect to the βs are constant and give us the trajectory: ∂S ∂ βµ = xiniµ = xµ − dη m 2 c 2 − β · β − 2qβ · A(η ) − q 2 A(η ) · A(η ) 2(β · k)2 η0 η 1 − dη βµ + qAµ (η ) (2.36) β · k η0 η 1 = xiniµ + dη βµ + qAµ (η ) (2.37) β · k η0 η kµ − dη 2qβ · A(η ) + q 2 A(η ) · A(η ) . 2 2(β · k) η0 kµ

η

⇒

xµ

In the last line we used (2.34) again. We shall now specialize on an electromagnetic wave ˆ A(η) = Aey sin η, i.e., ˆ Aµ = (0, 0, Asin η, 0), In this case we have ˆ β · A = −β2 Asin η, ˆ A · A = −A2 sin2 η, β · k = k(β0 − β1 ), (2.40) k µ = (ω/c, k, 0, 0) = (k, k, 0, 0). (2.39) k = ke x , (2.38)

2.2. RELATIVISTIC DYNAMICS IN AN ELECTROMAGNETIC WAVE

17

**(the reader should be careful not to mix up upper indices with powers!) and (2.35) becomes explicitly P =
**

0

c

= −β −

0

ˆ ˆ 2qβ2 Asin η + q 2 A2 sin2 η 2(β0 − β1 ) ˆ ˆ 2qβ2 Asin η + q 2 A2 sin2 η 2(β0 − β1 )

, ,

(2.41) (2.42) (2.43) (2.44)

**P 1 = p x = −β1 − ˆ P 2 = py + q Asin η = −β2 , P = p z = −β .
**

3 3

Clearly, the canonical momenta in y- and z-direction are conserved, and the relation between canonical and kinetic momentum is included in (2.43).

**2.2.1 The oscillation center frame
**

We are still free to choose the initial conditions βµ . This is equivalent to choose a certain reference frame in which we want to study the dynamics. The only restriction is β · β = m 2 c 2 . Let us choose the βs in such a way that the oscillation center of the particle is at rest: p x = py = p z = 0. From eqs. (2.43) and (2.44) follows β2 = β3 = 0 so that with β · β = m2 c 2 ⇒ β0 = − m 2 c 2 + (β1 )2 (2.47) ˆ (minus sign because in (2.41) must be positive in the free particle case where A = 0). From p x = 0 and (2.42) we have 2β1 β1 + ˆ ˆ m 2 c 2 + (β1 )2 = 2qβ2 Asin η + q 2 A2 sin2 η. (2.48) (2.46)

!

(2.45)

The cycle average of sin η vanishes while sin2 η = 1/2. Equation (2.48) can then be solved for β1 , ˆ q 2 A2 1 . (2.49) |β1 | = 4 m 2 c 2 + q 2 A2 /2 ˆ The sign will be chosen later. The trajectory in the oscillation center frame can be calculated from (2.37) and reads c t = c tini + β0 k(β − β )

0 1

(η − η0 ) +

ˆ q 2 A2 2k(β − β )

0 1 2

η

dη sin2 η ,

η0

(2.50)

18

**CHAPTER 2. CLASSICAL MOTION IN ELECTROMAGNETIC FIELDS
**

x x

1

= xini + = xini +

2

1

β1 k(β0 − β1 ) ˆ qA k(β0 − β1 )

(η − η0 ) +

η

ˆ q 2 A2 2k(β0 − β1 )2

η

dη sin2 η ,

η0

(2.51) (2.52) (2.53)

2

dη sin η ,

η0

**x 3 = xini 3 . The difference of (2.50) and (2.51) yields c t − x 1 = c tini − xini 1 + so that η = ωt − k x, η0 = ωtini − k xini ,
**

1

η − η0 k

(2.54)

(2.55)

as it should. Since in the oscillation center x should only oscillate but not drift, the term ∼ (η − η0 ) has to be canceled by the ﬁrst term of the integral 1 1 dη sin2 η = η − sin 2η. 2 4 This is the case if we choose the positive sign in (2.49), β = Explicitly, we have β =−

0 1

(2.56)

1 4

ˆ q 2 A2 ˆ m c + q A2 /2

2 2 2

.

(2.57)

ˆ m 2 c 2 + q 2 A2 /4 ˆ m c + q A2 /2

2 2 2

,

β0 − β1 = −

ˆ m 2 c 2 + q 2 A2 /2,

(2.58)

and the trajectory is given by [setting rini appropriately and x µ = (c t , x, y, z)] x = − sin 2η, ˆ 8k(m 2 c 2 + q 2 A2 /2) ˆ qA y = cos η, ˆ k m 2 c 2 + q 2 A2 /2 z = 0. ˆ q 2 A2 (2.59) (2.60) (2.61)

This describes a ﬁgure-eight motion in the plane deﬁned by the polarization vector (ey in our case) and the propagation direction k/k (e x in our case), as shown in Fig. 2.2. If we deﬁne the dimensionless vector potential amplitude as a= ˆ qA mc (2.62)

2.2. RELATIVISTIC DYNAMICS IN AN ELECTROMAGNETIC WAVE

19

**Figure 2.2: Figure-eight dynamics of a charged particle in an electromagnetic wave, as seen in
**

the oscillation center frame. The trajectory in the xy-plane, where x is the propagation direction of the laser pulse, and y is the polarization direction, is shown for a = 0.5 (solid), a = 1 (dotted), ˆ ˆ a = 10 (dashed), and a = 100 (dashed-dotted). As a increases, the amplitudes k x and k y approach the calculated values 1/4 and 2, respectively.

we have kx = − a2 8(1 + a 2 /2)

ˆ kx

sin 2η,

ky =

a 1 + a 2 /2

ˆ ky

cos η,

k z = 0.

(2.63)

The size of the ﬁgure-eight does not increase inﬁnitely as the laser intensity goes to inﬁnity: ˆ 1 x 1 ˆ ˆ 0.177. (2.64) lim k x = , lim k y = 2, lim = a→∞ a→∞ a→∞ y ˆ 4 2 4 Note that we only have the orbit parameterized with the invariant phase η (which is proportional to the proper time). We do not know the explicit expressions for x and y as functions of t . Parameterized with η, the trajectory looks extremely simple. In fact, only η and 2η shows up. If η were just ωt we could talk about the fundamental and the second harmonic and nothing else. However, since η = ωt − k x and x itself depends on t (or η), all frequencies, that is, all multiples of the laser frequency enter. This has consequences for the radiation emitted by such a particle. We neglect the emitted radiation in this Chapter but will come back to it later on.

**2.2.2 The adiabatically ramped pulse in the lab frame
**

We shall now investigate the same situation in the lab frame. We assume that the laser pulse has been ramped up adiabatically from = 0 at η → −∞ to = 1, and that the

20

CHAPTER 2. CLASSICAL MOTION IN ELECTROMAGNETIC FIELDS

Figure 2.3: Particle motion in the lab frame for a = 1. While oscillating in polarization direction, the particle is drifting in propagation direction. The laser pulse is adiabatically ramped up and of constant amplitude afterwards. The particle was initially at rest. Note that there is no backward motion in x-direction (no loops but spikes).

particle starts from rest. Equations (2.41)–(2.44) hold in the lab frame as well. However, note that four-vectors such as k µ change if we switch from one frame to the other (relativistic Doppler effect). Since it should be clear from the context in which frame we are working, we suppress explicit indices indicating the frame. The initial condition p = 0 for η → −∞ implies that β1 = β2 = β3 = 0 and β0 = −mc. For the trajectory one ﬁnds x = a2 1 η − sin 2η , 2 (2.65) (2.66) (2.67)

4k a y = cos η, k z = 0,

where we used the previously introduced dimensionless vector potential amplitude a [cf. (2.62)]. One sees that in polarization direction the particle just oscillates as before while in laser propagation direction it is drifting. An example of such an orbit is shown in Fig. 2.3. There seems to be a contradiction as far as the excursion of the particle in polarization direction is concerned: in the lab frame this excursion is just proportional to a and thus is, in principle, unlimited. In the oscillation center frame the excursion was limited to 2k, despite the fact that a is the same in both frames. The resolution, of course, lies in k. With respect to the lab, the laser pulse is red-shifted in the oscillation center frame. Finally, we shall calculate the velocity of the oscillation center frame with respect to

**2.3. THE RELATIVISTIC PONDEROMOTIVE FORCE
**

the lab frame. In the latter, eqs. (2.41)–(2.44) can be written as P0 mc = =1+ a2 2 sin2 η, P1 mc = px mc = a2 2 sin2 η, P 2 = P 3 = p z = 0.

21

mc

2

(2.68)

It is obvious that for our choice of the vector potential, the Lorentz transformation has to be performed parallel to e x so that γoc −voc γoc /c 0 0 γoc 0 0 −voc γoc /c Λµ = (2.69) ν 0 0 1 0 0 0 0 1 with voc the oscillation center velocity we are looking for and γoc = (1 − voc 2 /c 2 )−1/2 . Applying this transformation to (2.68), i.e., P µ = Λµ P ν gives us ν P

1

γoc mc

1

=−

voc c

1+

a2 2

sin η +

2

a2 2

sin2 η.

(2.70)

The condition P = p x = 0 yields voc = a2 4 + a2 c. (2.71)

This is the velocity of the oscillation center of the particle in the lab frame if it was at rest before the pulse arrived.

**2.3 The relativistic ponderomotive force
**

We shall now derive the relativistic orbit of the oscillation center for a vector potential of the form (2.19). It is desirable to consider the oscillation center as a relativistic pseudo particle. However, it is a priori not given for granted that the oscillation center coordinates and momenta automatically “behave” in a relativistic, proper way. The correct averaging over a laser period is crucial here. The situation is somewhat similar to the relativistic center of mass, which is ill-deﬁned if one naively extends the nonrela2 2 −1/2 , tivistic expression and writes R = i γi mi , where γi = (1 − vi /c ) i ri γi mi / without specifying in which system this expression should be evaluated. This is easily illustrated by the following example: Imagine two particles of equal rest mass moving with velocities ±ve x in the lab frame, and v very close to c. The observer in the lab frame will come to the conclusion that the center of mass (as deﬁned above) is half way between both particles and stationary. Let us now transform to the reference frame in which one of the two particles is at rest. In this frame the other particle will have a so much higher “effective mass” γ m m that the center of mass will be effectively at

22

CHAPTER 2. CLASSICAL MOTION IN ELECTROMAGNETIC FIELDS

the position of this second particle. The two centers of mass measured by the two observers will not transform properly into each other by a Lorentz transformation. The ambiguity can be circumvented by deﬁning the center of mass in the system in which it is at rest. Once determined it can then be transformed to any other system by a Lorentz transformation. In the case of the relativistic oscillation center of a charged particle in a laser ﬁeld such as (2.19) we are in the fortunate situation to have an invariant phase η = k · k over which we can average in an invariant manner. Already in a standing wave there is not such a single invariant η anymore. In the lab frame, for instance, the two phases η1 = ωt − k · r and η2 = ωt + k · r show up. In a reference frame moving along k one of the two waves will be red-shifted while the other will be blue-shifted, i.e., in this frame there will be no standing wave at all. As in the center of mass-problem, in such a situation the oscillation center — if existing — has to be deﬁned in the system where it is at rest, and averaging has to be done over the proper time. In this lecture we will restrict ourselves to the relativistic ponderomotive force in the travelling laser pulse where averaging over the invariant phase η can be done in any frame. Averaging of (2.35) and (2.37) yields [with βµ = (β0 , β)] roc = r (η) = rini + β η − η0 β·k −k , q2 2(β · k)2

η

dη A · A,

η0

(2.72) (2.73) (2.74)

poc = P(η) = −β + k

oc

q 2A · A 2β · k .

c

=

c

= −β0 + k

q 2A · A 2β · k

Here, the averaged phase η is given by η = ωt − k · roc . The rest mass of the new pseudoparticle called oscillation center is given through poc µ poc µ = M 2 c 2 , For consistency, this mass has also to fulﬁll poc = γoc M voc , For the velocity one ﬁnds voc = (ω − k · voc ) droc dη = (ω − k · voc ) β − kΓ β·k (2.78) ˙ voc = roc , γoc = 1 − voc 2 c2

−1/2

(2.75)

poc µ = (

oc /c, poc ).

(2.76)

.

(2.77)

**2.3. THE RELATIVISTIC PONDEROMOTIVE FORCE
**

where the abbreviation Γ= q 2A · A 2β · k

23

(2.79)

has been introduced. In order to solve (2.78) for voc we decompose the oscillation center velocity and β in components parallel and perpendicular to k, voc = voc This yields voc = ω and γoc = − In the same way we decompose poc , poc = poc with (2.73) leading to poc = −β + kΓ, We then obtain poc ⊥ = −β⊥ .

!

k k

+ voc ⊥ ,

β=β

k k

+ β⊥ .

(2.80)

β − kΓ β0 k − k 2 Γ

,

voc ⊥ = ω β0 − kΓ

β⊥ β0 k − k 2 Γ .

,

(2.81)

m 2 c 2 − 2kΓ(β0 − β )

(2.82)

k k

+ poc ⊥

(2.83)

(2.84) (2.85)

poc µ poc µ = β · β − q 2 A · A = M 2 c 2 so that, using β · β = m 2 c 2 , the mass of the oscillation center is given by M= 1 c m 2 c 2 − q 2 A · A.

(2.86)

It is left as an exercise to the interested reader to check that this mass is indeed consistent with poc = γoc M voc . Another check is the following: if we transform to the system moving with voc , the energy oc in this system should be simply M c 2 . The transformation reads

oc

c

= γoc

oc

c

−

voc · poc c

.

(2.87)

Using (2.74), (2.82), and the decompositions for voc and poc above, one readily checks that indeed = M c 2. (2.88) oc

24

CHAPTER 2. CLASSICAL MOTION IN ELECTROMAGNETIC FIELDS

The relativistic oscillation center pseudo particle possesses a rest mass which is not a constant but depends on the phase η and thereby on space and time, that is, a mass ﬁeld. What remains to be calculated is the ponderomotive force ˙ Fp = poc = (ω − k voc ) Using (2.73) and (2.79) one obtains Fp = The Minkowski force

M Fp =

d dη

poc .

(2.89)

k

ωq 2

d

k 2(β0 − kΓ) dη d

A · A.

(2.90)

poc = γoc Fp (2.91) dτ (where τ is the proper time) assumes a particularly simple form. Using (2.82) (note that the denominator of γoc is proportional to M ) and 1 =− ∇ dη k one obtains

M Fp = −∇ oc

d

(2.92)

= −c 2 ∇M .

(2.93)

The phase-dependent rest mass is the origin of the oscillation center motion. In the nonrelativistic case we saw already that the local quiver motion gives rise to the ponderomotive potential. Relativistically, this quiver motion is included in the rest mass of the oscillation center.

**2.3.1 Example: sin2 -pulse
**

Let us consider a pulse envelope of the form (η) = sin2 (εη), 0<ε 1 (2.94)

which may describe a pulsed laser beam in which one pulse lasts from η = nπ/ε to η = (n + 1)π/ε with n = 0, 1, 2, . . .. At time t = 0 the particle is assumed to be at rest at r = 0 so that β = 0, β0 = −mc. (2.95) Equations (2.72) and (2.73) become in this case roc = poc ˆ q 2 A2

2 2

3

4ε 4m c k 8 ˆ q 2 A2 4 k = sin (εη) . 4mc k

η−

1

sin(2εη) +

1 32ε

sin(4εη)

k k

,

(2.96) (2.97)

2.3. THE RELATIVISTIC PONDEROMOTIVE FORCE

25

Figure 2.4: Electron trajectory for a = −0.5 and ε = 0.01. Polarization and propagation directions are ey and e x , respectively. The displacement after the ﬁrst pulse agrees with formula (2.99) (which yields k · roc 1 = 7.36 in this case).

**The relativistic ponderomotive force (2.90) is
**

sin2 Fp

=

ωmc a 2 a sin (εη) + 4

2 4

d dη

sin4 (εη)

(2.98)

ˆ where a = q A/mc has been used again. In the nonrelativistic limit |a| 1 the nonrelˆ ˆ ativistic ponderomotive force (2.11) is recovered (using (2.92) and A2 = E 2 /ω 2 ). From (2.96) we can immediately infer the displacement of the particle after the ﬁrst pulse: k π η1 , η1 = . (2.99) 4k 8 k ε Figure 2.4 shows the trajectory of an electron for a = −0.5 and ε = 0.01 during the ﬁrst pulse, conﬁrming formula (2.99). roc 1 = a2 3

Problem 2.1 Check that poc = γoc M voc . Further reading: An excellent paper on the subject (including references to important previous work) is E. S. SARACHIK and G. T. SCHAPPERT, “Classical Theory of the Scattering of Intense Laser Radiation by Free Electrons”, Phys. Rev. D 1, 2738 (1970).

26

CHAPTER 2. CLASSICAL MOTION IN ELECTROMAGNETIC FIELDS

**Chapter 3 Atoms in external ﬁelds
**

In this Chapter we shall ﬁrst introduce atomic units and remind the reader of basic quantum mechanical techniques and atomic phenomena such as time-dependent perturbation theory, resonant interaction (Rabi ﬂopping), Stark-effect etc., before we come to the actual topic of this lecture, i.e., the strong ﬁeld effects and the new theoretical approaches that have been developed in this context.

3.1 Atomic units

We will introduce the atomic units in a somewhat formal way. For beginners, the use of atomic units is sometimes confusing because dimensional checks are not possible in a straightforward way once ħ , me , e have been set “equal to unity”. Another practical h problem for beginners is to convert the result of a calculation performed using atomic units back to SI units. If one sticks to SI units and the result of a calculation is, say, 42, one knows that the result is dimensionless. If in atomic units the result is 42 it could be as well 42 ħ , 42 e, 42 me , 42 · 4π 0 , 42 ħ me /e, . . .. A good example is the expression for h h the nonrelativistic eigenenergies of hydrogen-like ions, which in atomic units is simply given by Z2 , n = 0, 1, 2, . . . (atomic units) (3.1) n =− 2n 2 where Z is the nuclear charge. The right-hand-side appears to be dimensionless. Hence, without knowing that the left-hand-side is an energy, there would be no way back to SI units. If one performs the entire calculation (i.e., the solution of the Schrödinger equation) in SI units, one obtains

n =−

Z2

me e 4

2n 2 ħ 2 (4π 0 )2 h

,

n = 0, 1, 2, . . .

(SI units).

(3.2)

Even without knowing the left-hand-side we can recover from the right-hand-side alone that the result is an energy, provided we know the SI units of ħ , me , e, and 0 . This h 27

28

CHAPTER 3. ATOMS IN EXTERNAL FIELDS

seeming asymmetry between the unit systems arise from the fact that “setting ħ , me , e, h and 4π 0 equal to unity” is more than a change of units. It is like setting kg, m, s, and C to unity. Let us denote mass, length, time, and charge by M, L, T, and C, respectively. In atomic units we wish to use the action ħ , the electron mass me , the modulus of the h electron charge e, and 4π times the permittivity of vacuum 4π 0 as the basic units. The relation between both system of units is established by (“[...]” meaning “units of ...”) [ħ ] h [me ] [e] [4π 0 ] = = = = Ma11 La12 Ta13 Ca14 , Ma21 La22 Ta23 Ca24 , Ma31 La32 Ta33 Ca34 , Ma41 La42 Ta43 Ca44 . (3.3) (3.4) (3.5) (3.6)

The exponents a41 , . . . , a44 , for instance, are determined by noticing that in SI units the dimension of 0 is Coulomb per Volt and meter. Volt is a derived unit. Because Coulomb times Volt is an energy one has V= and hence [4π 0 ] = M−1 L−3 T2C2 . Similarly, the remainder of the dimensional matrix is easily calculated and reads a 11 a A = 21 a31 a41 a12 a22 a32 a42 a13 a23 a33 a43 a14 a24 a34 a44 = 1 2 −1 0 1 0 0 0 . 0 0 0 1 −1 −3 2 2 (3.8) ML2 CT2 , (3.7)

(3.9)

Now we want to know the values (in SI units) of one atomic mass, length, time, and charge unit, denoted by , , , and , respectively. Those are later needed for the transformation back to SI units. Mass and charge are trivial: = me , = e. (3.10)

Let us calculate the value of the atomic length unit: = ħ b21 meb22 e b23 (4π 0 ) b24 . h Plugging in (3.3)–(3.6)and using the values for the as in (3.9) lead to = M b21 +b22 −b24 L2b21 −3b24 T−b21 +2b24 C b23 +2b24 , (3.12) (3.11)

3.1. ATOMIC UNITS

29

giving us four equations for the four b s. Since is a length, 2b21 − 3b24 = 1, and the exponents of mass, time, and charge must be zero. One ﬁnds b21 = 2, b22 = −1, b23 = −2, b24 = 1 so that = ħ 2 4π h me e

2 0

= 0.5292 · 10−10 m,

(3.13) is left as an exercise.

which is the Bohr radius a0 . The corresponding calculation for The inverse dimensional matrix is then established through = ħ b11 meb12 e b13 (4π 0 ) b14 , h = ħ b21 meb22 e b23 (4π 0 ) b24 , h = ħ b31 meb32 e b33 (4π 0 ) b34 , h = ħ h with b 11 b B = 21 b31 b41

b41

(3.14) (3.15) (3.16) (3.17) .

meb42 e b43 (4π 0 ) b44 0 1 0 2 −1 −2 = 3 −1 −4 0 0 1 0 1 2 0

b12 b22 b32 b42

b13 b23 b33 b43

b14 b24 b34 b44

(3.18)

It is readily checked that A · B = B · A = 1. (3.19) As an example for the transition from SI to atomic units, let us now formally rewrite the time-dependent Schrödinger equation in position space representation iħ h ∂ ∂t Ψ(r , t ) = H Ψ(r , t ) (3.20)

**in atomic units. We have that (with the values of primed symbols in atomic units)
**

2

ħ = ħ h h t = t Ψ = Ψ H = H =t

−3/2

=ħ ħ h h ħ 3 (4π 0 )2 h me e 4 =Ψ

2 2

⇒ ,

ħ = 1, h

(3.21) (3.22)

ħ 2 4π h me e 2

−3/2 0

, .

(3.23) (3.24)

=H

me e 4 ħ 2 (4π 0 )2 h

30

CHAPTER 3. ATOMS IN EXTERNAL FIELDS

Plugging this into (3.20) (and taking the primed wavefunction as a function of the primed variables) simply yields iħ h ∂ ∂t Ψ (r , t ) = H Ψ (r , t ), (3.25)

i.e., the same equation primed. However, since ħ = 1 [cf. (3.21)] this simpliﬁes to h i ∂ ∂t Ψ (r , t ) = H Ψ (r , t ). (3.26)

The ħ effectively disappeared or, more precisely, is hidden in the units. This is what h is actually meant by “setting ħ = me = e = 1”. In the same way ħ disappeared in this h h example, me , e, and 4π 0 are effectively removed. If, for instance, H= p2 2me − Z e2 4π 0 r + eE · r , (3.27)

that is, the Hamiltonian governing the electron of a hydrogen-like ion in an electric ﬁeld E , in atomic units p2 Z (3.28) H = − +E · r 2 r holds. Finally, we give an example how to return to SI units after a busy calculation employing atomic units. Let us suppose the result of this calculation is a an electric ﬁeld strength E = f (α , β , . . .) ei(ω t −p ·r ) (3.29) and f is some function of the entities α , β , . . . which can be converted to the SI values α, β, . . ., giving rise to some overall factor K = ħ σ me e ξ (4π 0 )ζ . Since an electric ﬁeld h η strength in SI units is Volt per meter, and Volt is related to mass, length, etc. through (3.7) we have m2 e 5 E =E =E 4 e . (3.30) 2 ħ (4π 0 )3 h Hence 2 2 me e 5 me e 5 E =E 4 =K 4 f (α, β, . . .) ei(ω t −p ·r ) . (3.31) 3 3 ħ (4π 0 ) h ħ (4π 0 ) h Obviously ω t − p · r is dimensionless in atomic units, as is ωt in SI units, so that ωt = ω t (3.32)

**but what about p · r ? In SI units p · r is not dimensionless but an action. Well, we have p=p =p me e 2 ħ 4π h
**

0

,

r=r

=r

ħ 2 4π h me e

2

0

(3.33)

3.1. ATOMIC UNITS

so that p ·r = p·r ħ h

31

,

(3.34)

**which, in fact, is dimensionless. Hence the expression (3.29) reads in SI units E=
**

2+η me e 5+ξ h f (α, β, . . .) ei(ωt −p·r /ħ ) .

ħ 4−σ (4π 0 )3−ζ h

(3.35)

We conclude this section by giving the explicit expressions and values for frequently occurring entities in laser-atom interaction: atomic mass unit atomic length unit atomic time unit atomic charge unit atomic action unit atomic permittivity unit atomic energy unit atomic velocity unit atomic el. field strength unit atomic intensity unit = me = 9.1094 · 10−31 kg, = = = = = = = = = ħ 4π h e me

4 2 2 0

(3.36) (3.37)

= a0 = 0.5292 · 10−10 m,

ħ 3 (4π 0 )2 h

me e e = 1.6022 · 10−19C, ħ = 1.0546 · 10−34 J, h 4π 0 = 4π · 8.8542 · 10−12CV−1 m−1 , me e 4 = 4.3598 · 10−19 J = 27.21 eV, 2 2 ħ (4π 0 ) h e2 = 2.1877 · 106 ms−1 = αc, ħ 4π 0 h 2 me e 5 = 5.1422 · 1011Vm−1 , 4 3 ħ (4π 0 ) h 4 e 12 me = 3.5095 · 1020Wm−2 9 6 8παħ (4π 0 ) h = 3.5095 · 1016Wcm−2 .

= 2.4189 · 10−17 s = 0.024 fs, (3.38) (3.39) (3.40) (3.41) (3.42) (3.43) (3.44) (3.45)

Here, the ﬁne structure constant α= e2 ħ 4π 0 c h = 1 137.04 (3.46)

has been introduced. The value of the light velocity in vacuum in atomic units equals the inverse ﬁne structure constant. Note that with ħ , e, me , and 0 alone it is not h possible to construct a dimensionless entity (as it is impossible with kg, m, s, and C). One needs a ﬁfth building brick, which is c in the case of the ﬁne structure constant.

32

CHAPTER 3. ATOMS IN EXTERNAL FIELDS

A useful formula to convert the ﬁeld strength E in atomic units (a.u.) to a laser intensity I in the commonly used Wcm−2 is (I in Wcm−2 ) = 3.51 · 1016 × (E 2 in a.u.). (3.47)

Problem 3.1 Calculate the value of the atomic frequency unit in Hz. Problem 3.2 Calculate the value of the atomic magnetic ﬁeld unit in Tesla.

3.2

Time-dependent perturbation theory

In this Section we brieﬂy review time-dependent perturbation theory. We consider a quantum mechanical system such as an atom, for instance, interacting with a timedependent ﬁeld, e.g., an electromagnetic ﬁeld. In lowest order perturbation theory we expect transitions between the unperturbed states to occur. The Hamiltonians of interest are of the form ˆ ˆ ˆ ˆ H (t ) = H0 + W (t ), W (t ≤ 0) = 0. (3.48) Here we assume that the perturbation W (t ) is switched off for times t ≤ 0. We further assume that the solution of the unperturbed problem is known, that is, ˆ H0 |φn 〉 =

n |φn 〉

(3.49)

with given eigenenergies n and eigenstates |φn 〉. The unperturbed states (including the continuum states, if present) form a complete basis so that the full solution of the time-dependent Schrödinger equation (TDSE) ˆ i∂ t |ψ(t )〉 = H (t )|ψ(t )〉 can be expanded as |ψ(t )〉 =

n

(3.50)

cn (t )|φn 〉 e−i

nt

.

(3.51)

Here we use atomic units and factor the unperturbed time-evolution ∼ e−i n t out of cn (t ) (interaction picture). If at time t = 0 the system is in a single, unperturbed state we have |ψ(0)〉 = |φi 〉 ⇒ cn (0) = δni . (3.52) ˆ At later times, the probability for ﬁnding the system in the state |φf 〉 of H0 is wi→f (t ) = |cf (t )|2 . (3.53)

3.2. TIME-DEPENDENT PERTURBATION THEORY

33

**Inserting the expansion (3.51) in the TDSE (3.50) and multiplying from the left by 〈φ m | yields i dc m dt =
**

n

W mn (t )cn (t ) ei(

m − n )t

,

ˆ W mn (t ) = 〈φ m |W (t )|φn 〉.

(3.54)

**Formal integration of (3.54) gives c m (t ) = c m (0) + 1 i
**

0 t

dt

n

W mn (t ) ei(

m − n )t

cn (t ),

(3.55)

which is an integral equation because the coefﬁcient c m for a certain m also appears under the integral within the sum over n. Such integral equations may be solved iteratively by replacing the cn s under the integral by the expression (3.55) itself. If the perturbation is small (i.e., the W mn s are small on the relevant energy scale), the series converges and one can stop at some sufﬁciently high order. In ﬁrst order one simply has c m (t ) = c m (0) + 1 i

0 t

dt

n

W mn (t ) eiωmn t cn (0),

ω mn =

m

−

n.

(3.56)

**In second order we have c m (t ) = c m (0) + 1 i
**

0 t

dt

n

W mn (t ) eiωmn t × cn (0) + 1 i

0 t

(3.57)

dt

u

Wnu (t ) eiωnu t c u (0) .

If the ﬁnal state of interest was not populated at time t = 0 and ci = 1, the ﬁrst order expression (3.56) becomes cf (t ) = 1 i

0 t

dt Wfi (t ) eiωfi t .

(3.58)

Now let us assume that the perturbation is of the form ˆ ˆ W (t ) = V sin ωt In the sin-case, for instance, one has Wfi (t ) = Vfi sin ωt = so that cfsin (t ) = Vfi 2i Vfi 2i eiωt − e−iωt , ˆ Vfi = 〈φf |V |φi 〉 (3.60) or ˆ ˆ W (t ) = V cos ωt . (3.59)

1 − ei(ωfi +ω)t ωfi + ω

−

1 − ei(ωfi −ω)t ωfi − ω

,

(3.61)

34 and

sin wi→f (t ) =

**CHAPTER 3. ATOMS IN EXTERNAL FIELDS
**

2

|Vfi |2 1 − ei(ωfi +ω)t 4 ωfi + ω

−

1 − ei(ωfi −ω)t ωfi − ω

.

(3.62)

**In the same way one ﬁnds for the cos-expression in (3.59)
**

cos wi→f (t ) =

|Vfi |2 1 − ei(ωfi +ω)t 4 ωfi + ω

+

1 − ei(ωfi −ω)t ωfi − ω

2

.

(3.63)

**The case of a constant perturbation can be obtained by setting ω = 0:
**

const wi→f (t ) =

|Vfi |2

2 ωfi

1−e

iωfi t

2

= |Vfi | F (t , ωfi ),

2

F (t , ωfi ) =

sin(ωfi t /2) ωfi /2

2

. (3.64)

The results for the sin and cos-like perturbations can be written as (upper sign for sin, lower for cos) |Vfi |2 2 sin,cos A+ A− (3.65) wi→f (t ) = 4 where 1 − ei(ωfi ±ω)t sin[(ωfi ± ω)t /2] A± = = −i ei(ωfi ±ω)t /2 . (3.66) ωfi ± ω (ωfi ± ω)/2 If we assume that ω, ωfi > 0 and t ω −1 , only the resonant term A− is important and the highly oscillatory and small anti-resonant term A+ can be neglected. This is the so-called rotating wave approximation (RWA). We then obtain

RWA wi→f (t ) =

|Vfi |2 4

F (t , ωfi − ω).

(3.67)

The function F is deﬁned in (3.64). It is illustrated in Fig. 3.1 for ωfi = 1 and different times. One sees that the maximum increases in time as t 2 while the resonance width ∆ω = 4π/t (3.68)

decreases in time. The resonance width deﬁnes the energy resolution with which we can determine a transition frequency ∆ using a sinusoidal perturbation, t∆ 1. (3.69)

This is the time-energy uncertainty relation. Note that it is of completely different origin compared to uncertainty relations for noncommuting operators (such as the positionmomentum uncertainty relation, for instance). Let us now discuss the validity of our ﬁrst order perturbation theory results. On one hand, the time t must not be too big, because at resonance one has

res wi→f (t ) =

|Vfi |2 4

t 2.

(3.70)

3.2. TIME-DEPENDENT PERTURBATION THEORY

35

(a)

(b)

(c)

**t = 100. The maximum value t 2 occurs at resonance ω = ωfi , the width of the central peak is ∆ω = 4π/t .
**

res Since wi→f (t ) is a probability (i.e., a number between zero and one) and the perturbation is supposed to be small

Figure 3.1: The function F (t , ωfi − ω) vs ω for ωfi = 1 and (a) t = 10, (b) t = 30, and (c)

|Vfi |2 4

t2

1

⇒

t

1 |Vfi |

(3.71)

must hold. On the other hand, the RWA to be valid requires t 1 |ωfi | 1 ω (3.72)

because at early times A+ and A− are of the same magnitude (transient dynamics). Hence, 1 1 t ⇒ |ωfi | |Vfi | (3.73) |ωfi | |Vfi | which conﬁrms our statement above, that “small perturbation” means that the values of the relevant matrix elements W mn are small compared to the “relevant energy scale”, which here is the transition energy ωfi . If the ﬁnal state lies in the continuum and is characterized by a set of parameters α (e.g., quantum numbers , m, wave vector k or energy etc.) one has to integrate over all the possible ﬁnal states to obtain the transition probability, wi→f (t ) =

α∈Df

dα |〈α|ψ(t )〉|2 .

(3.74)

36

CHAPTER 3. ATOMS IN EXTERNAL FIELDS

We now choose the energy as one of these parameters describing the ﬁnal state, and the set β comprises the remaining parameters. Introducing the density of states ρ(β, ) we can write dα = ρ(β, ) dβ d , (3.75) and (3.74) turns into wi→f (t ) =

(β, )∈Df

dβ d ρ(β, ) |〈β, |ψ(t )〉|2 .

(3.76)

**In the case of a constant perturbation, for instance, we obtain wi→f (t ) =
**

(β, )∈Df

ˆ dβ d ρ(β, ) 〈β, |V |φi 〉 F (t , − i ).

2

2

(3.77)

ˆ If t is sufﬁciently large, and ρ(β, ) 〈β, |V |φi 〉 varies much slower over an energy interval 4π/t than F , the integration over energy in (3.77) can be performed using

t →∞

lim F (t , − i ) = πt δ[( − i )/2] = 2πt δ( − i )

(3.78)

**so that wi→f (t ) = 2πt
**

β∈Df

dβ 〈β,

f

=

i |V |φi 〉

ˆ

2

ρ(β,

f

=

i)

if

i

∈ Df

(3.79)

and zero otherwise. The transition probability per unit time (i.e., the rate) is given by Γi→f = dwi→f dt (3.80)

and is time-independent in the case of a constant perturbation. If we suppress the other parameters β to be integrated over, we simply have Γconst. = 2π 〈 i→f

f

=

i |V |φi 〉

ˆ

2

ρ(

f

=

i ).

(3.81)

**In the case of a sinusoidal perturbation we obtain Γsin,cos = 2π 〈 i→f
**

f=

ˆ i + ω|V |φi 〉 ρ(

2

f

=

i

+ ω).

(3.82)

Equations (3.81) and (3.82) are “Fermi’s Golden Rule” applied to a constant perturbation (which conserves energy) and one photon absorption into the continuum, that is, single photon ionization or the photo effect, respectively.

3.2. TIME-DEPENDENT PERTURBATION THEORY

37

**ˆ ˆ ˆ In the case of a laser ﬁeld, V is proportional to r · E where E is the electric ﬁeld amplitude (not an operator!). Hence 〈
**

f

=

i

ˆ + ω|V |φi 〉

2

∼ |E |2 ∼ I ,

(3.83)

i.e., the rate will be proportional to the laser intensity. In nth order n photons may contribute to the ionization process. Because in nth order the matrix elements W mn appear n times in the expression for cf , the nth order ionization rate is proportional to I n and thus fulﬁlls Γi→f = σn I n where the σn are called generalized cross sections.

(n)

(3.84)

Problem 3.3 Calculate the density of states ρ( ) for a free, spinless particle of mass m. Problem 3.4 Calculate the SI units of the generalized cross sections σn in (3.84).

**3.2.1 Dyson series, S-matrix, Green’s functions, propagators, and resolvents
**

ˆ Let us consider the time-evolution operator U corresponding to the TDSE (3.50), ˆ |ψ(t )〉 = U (t , t )|ψ(t )〉. ˆ The operator U fulﬁlls the TDSE, ˆ ˆ ˆ i∂ t U (t , t ) = H (t )U (t , t ), and formal “solutions” of this equation are given by ˆ ˆ U (t , t ) = U0 (t , t ) − i

t t

(3.85)

(3.86)

ˆ ˆ ˆ dt U (t , t )W (t )U0 (t , t ) ˆ ˆ ˆ dt U0 (t , t )W (t )U (t , t )

(3.87) (3.88)

ˆ = U0 (t , t ) − i

t

t

38

CHAPTER 3. ATOMS IN EXTERNAL FIELDS

ˆ ˆ where U0 is the time-evolution operator associated to the unperturbed Hamiltonian H0 . ˆ Equations (3.87) and (3.88) are integral equations since U appears also on the right hand side under the time integrals [cf. (3.55)]. Iteration yields ˆ ˆ U (t , t ) = U0 (t , t ) + (−i)

t t t t

ˆ ˆ ˆ dt U0 (t , t )W (t )U0 (t , t )

(3.89)

+(−i)2

t

dt

t

ˆ ˆ ˆ ˆ ˆ dt U0 (t , t )W (t )U0 (t , t )W (t )U0 (t , t ) + · · · .

ˆ Introducing the perturbation WIP in the interaction picture ˆ ˆ ˆ ˆ ˆ ˆ ˆ WIP (t , t ) = U † (t , t )W (t )U (t , t ) = U (t , t )W (t )U (t , t ), making use of ˆ ˆ ˆ U0 (t , t ) = U0 (t , t )U0 (t , t ) (3.90) (3.91)

**ˆ and multiplying (3.89) by U0 (t , t ) from the left yields ˆ ˆ U0 (t , t )U (t , t ) = 1 + (−i)
**

t t

ˆ dt WIP (t ) + (−i)2

t

t

t

dt

t

ˆ ˆ dt WIP (t )WIP (t ) + · · · .

(3.92) ˆ (which is always t ). We now rewrite Here we suppressed the second time index of WIP this series in the following way: ˆ ˆ U0 (t , t )U (t , t ) = 1 + (−i)

t t t

ˆ dt WIP (t )

t

(3.93) (3.94) (3.95) ˆ ˆ θ(t − t )WIP (t )WIP (t ) (3.96)

+(−i)2

t

dt

t t

ˆ ˆ dt θ(t − t )WIP (t )WIP (t ) + · · ·

= 1 + (−i) + (−i)2 2

t t t

ˆ dt WIP (t )

t

dt

t

dt

ˆ ˆ +θ(t − t )WIP (t )WIP (t ) + · · ·

∞

=

n=0

(−i)n n!

t

t

t

dt1 · · ·

t

ˆ ˆ ˆ dtn T WIP (t1 ) · · · WIP (tn ) .

(3.97)

ˆ In the last line we introduced the time ordering operator T. The expansion of the time evolution operator in terms of integrals over time-ordered products of the perturbation (in interaction picture representation) is called Dyson series. The last expression (3.97) is often written in the form ˆ ˆ ˆ U0 (t , t )U (t , t ) = Te−i

t t

ˆ dt WIP (t )

.

(3.98)

**3.2. TIME-DEPENDENT PERTURBATION THEORY
**

ˆ If the WIP s commute at different times this expression reduces to

t

39

exp −i

t

ˆ dt WIP (t ) ,

t ˆ i.e., the problem is boiled down to the solution of the single integral t dt WIP (t ). ˆ ˆ Unfortunately, in general [WIP (t1 ), WIP (t2 )] = 0 in most of the interesting cases. Let us now deﬁne an initial and a ﬁnal state as

|i〉 = |ψi (−∞)〉,

|f〉 = |ψf (−∞)〉,

(3.99)

ˆ and let us assume that the perturbation W is absent for t → ±∞. The probability for a transition from the initial to the ﬁnal state is wi→f = |Mif |2 with Mif ˆ = 〈ψf (∞)|U (∞, −∞)|ψi (−∞)〉 ˆ ˆ = 〈ψ (−∞)|U † (∞, −∞))U (∞, −∞)|ψ (−∞)〉

f 0 i

(3.100)

(3.101) (3.102) (3.103) (3.104)

ˆ ˆ = 〈f|U0 (−∞, ∞)U (∞, −∞)|i〉 ˆ =: 〈f|S|i〉 = S .

fi

ˆ Sfi is the so-called S-Matrix. Note that S is the left hand side of (3.98) for t → −∞ and t → ∞. ˆ Let us come back to the integral equation for U (3.88). Multiplication by θ(t − t ) and insertion of θ functions under the integral so that the integration limits can be extended to ±∞ yields ˆ ˆ U (t , t )θ(t − t ) = U0 (t , t )θ(t − t )−i Deﬁning the retarded Green’s functions ˆ ˆ K+ (t , t ) = U (t , t )θ(t − t ) , turns (3.105) into ˆ ˆ K+ (t , t ) = K0+ (t , t ) − i

∞ −∞ ∞

ˆ ˆ ˆ dt U0 (t , t )θ(t − t )W (t )U (t , t )θ(t − t ). (3.105) ˆ ˆ K0+ (t , t ) = U0 (t , t )θ(t − t ),

−∞

(3.106)

ˆ ˆ ˆ dt K0+ (t , t )W (t )K+ (t , t ).

(3.107)

ˆ It is easy to show [using (3.86), (3.106), and ∂ t θ(t ) = δ(t )] that K+ fulﬁlls the inhomogeneous TDSE ˆ ˆ (i∂ t − H )K+ (t , t ) = iδ(t − t ). (3.108)

40

CHAPTER 3. ATOMS IN EXTERNAL FIELDS

The advanced Green’s function is deﬁned through ˆ ˆ K− (t , t ) = −U (t , t )θ(t − t ). It fulﬁlls the same Eq. (3.108) (but for different boundary conditions). ˆ Let us now assume that H is time-independent so that

ˆ ˆ K+ (τ) = e−iH τ θ(τ),

(3.109)

τ=t −t .

(3.110)

This assumption may appear strange, especially if we have in mind interactions with strong laser ﬁelds (which are time-dependent electromagnetic ﬁelds). However, if we quantize the electromagnetic ﬁeld, the system atom + ﬁeld becomes conservative, and ˆ H would have no explicit time-dependence. It is always—at least in principle—possible to extend the system under study in such a way that the perturbing driver becomes part of the system, making the total system conservative. In this sense the TDSE is a special case of the time-independent Schrödinger equation and not the other way round. The TDSE arises when we divide bigger, conservative systems into smaller non-conservative systems. The ultimate system would be the entire universe (including parallel ones, of course) with no room for “external” time-dependent drivers whatsoever. ˆ We introduce a new operator G+ which is proportional to the Fourier-transformed Green’s function, ˆ K+ (τ) = − 1 2πi

∞ −∞ ∞ −∞

ˆ d e−i τ G+ ( ),

(3.111) (3.112)

ˆ G+ ( ) = −i

ˆ dτ ei τ K+ (τ).

We can then switch from the time-domain to the energy-domain (or frequency-domain) ˆ ˆ and back by working either with K+ (τ) or G+ ( ), respectively. Using (3.110) we obtain ˆ G+ ( ) = −i

0 ∞

dτ ei(

∞

ˆ −H )τ

(3.113)

ˆ −H +iη)τ

= −i lim

η→0+

dτ ei(

0

,

η≥0

(3.114)

⇒ and in the same way

ˆ G+ ( ) = lim

η→0+

1 ˆ − H + iη

(3.115)

ˆ G− ( ) = lim ˆ G± are called propagators.

η→0+

1 . ˆ − H − iη

(3.116)

**3.2. TIME-DEPENDENT PERTURBATION THEORY
**

ˆ The Fourier-transform of (3.107) for a time-independent W gives us ˆ ˆ G+ ( ) = G0+ ( ) − ˆ = G0+ ( ) − ˆ = G0+ ( ) − The last step follows from τ1 = t − t , We thus have τ2 = t − t ⇒ ∂ (τ, t ) ∂ (τ1 , τ2 ) = 1.

∞ ∞

41

dτ e

−∞ ∞

i τ ∞ −∞

ˆ ˆ ˆ dt K0+ (t , t )W K+ (t , t )

τ1

(3.117) (3.118) (3.119)

dτ

−∞ ∞ −∞ ∞

dt ei dτ2 ei

−∞

ˆ ˆ K0+ (τ1 )W ei ˆ ˆ K0+ (τ1 )W ei

τ2

ˆ K+ (τ2 ) ˆ K+ (τ2 ).

dτ1

−∞

τ1

τ2

(3.120)

ˆ ˆ ˆ ˆ ˆ G+ ( ) = G0+ ( ) + G0+ ( )W G+ ( )

(3.121)

which could have been immediately derived from the identity 1 A = 1 B + 1 (B − A) . B A 1 (3.122)

ˆ Equation (3.121) is an algebraic equation as compared to the integral equations for K+ ˆ and U . Finally, we introduce the resolvent ˆ G(z) = Obviously, as z → 1 ˆ z−H , z∈ . (3.123)

ˆ ˆ G± ( ) = lim G( ± iη).

η→0+

(3.124)

Since θ(x) + θ(−x) = 1 we can write ˆ ˆ ˆ U (τ) = K+ (τ) − K− (τ) ∞ 1 ˆ ˆ = d e−i τ [G− ( ) − G+ ( )] 2πi −∞ 1 ˆ = dz e−izτ G(z). 2πi C+ +C− (3.125) (3.126) (3.127)

The integration contours are depicted in Fig. 3.2. Discrete eigenenergies appear as poles on the real z-axis, continua correspond to cuts.

42

**CHAPTER 3. ATOMS IN EXTERNAL FIELDS
**

z

C+

cuts poles

C−

**Figure 3.2: Illustration of the integration contours C± in (3.127) in the z-plane. For τ > 0 the
**

ˆ contribution from C− is zero, for τ < 0 the contribution from C+ is zero. Eigenenergies of H are located along the real axis (discrete ones indicated by crosses, a continuum by a thick line.

For the resolvent (3.121) becomes ˆ ˆ ˆ ˆ ˆ G(z) = G0 (z) + G0 (z)W G(z) which can be iterated, ˆ ˆ ˆ ˆ ˆ ˆ ˆ ˆ ˆ ˆ G(z) = G0 (z) + G0 (z)W G0 (z) + G0 (z)W G0 (z)W G0 (z) + · · · . (3.129) (3.128)

3.3

Important models

In this Section we will go through two important, exactly soluble models. The ﬁrst one shows how discrete states cease to exist if they are coupled to a continuum. The second one discusses two resonantly (or almost resonantly) coupled discrete states and the population transfer between them (Rabi-oscillations). It is a nice example for a soluble problem where the previously introduced perturbation theory is not applicable.

**3.3.1 Discrete level coupled to the continuum
**

Starting point is the Hamiltonian ˆ ˆ ˆ H = H0 + W . (3.130)

We allow for a single discrete state |ϕ〉 and the continuum states. We now discretize the continuum by introducing a box of length L. The continuum states |k〉 will then be spaced by δ, and the density of states is 1/δ so that Fermi’s Golden Rule (3.81) yields 1 Γ = 2πw 2 , δ Here lim w2 δ = const. (3.131)

δ→0

ˆ wk := 〈k|W |ϕ〉

(3.132)

3.3. IMPORTANT MODELS

and w is the matrix element for which ˆ 〈k|H0 |k〉 =

k ϕ k

43 =

ϕ,

as required by (3.81). We assume k∈ , (3.133) (3.134) (3.135) (3.136)

= kδ, ⇒

−∞ < k < ∞,

ϕ

=0

=

k=0 ,

ˆ ˆ 〈ϕ|W |ϕ〉 = 〈k|W |k 〉 = 0, and that ˆ ˆ wk = 〈k|W |ϕ〉 = 〈ϕ|W |k〉 = w,

that is, all these transition matrix elements are equal and real. We are now looking for the new energies µ and states |ψµ 〉 fulﬁlling ˆ H |ψµ 〉 =

µ |ψµ 〉.

(3.137)

ϕ

**By multiplying from the left with 〈k| and 〈ϕ|, and making use of 1 = |ϕ〉〈ϕ| +
**

k

= 0 and (3.138)

|k〉〈k|,

we obtain

k 〈k|ψµ 〉 + w〈ϕ|ψµ 〉 = µ 〈k|ψµ 〉,

(3.139) (3.140)

w

k

〈k|ψµ 〉 = 〈ϕ|ψµ 〉

µ

µ 〈ϕ|ψµ 〉

so that 〈k|ψµ 〉 = w and

−

,

µ

−

k

=0

(3.141)

k

µ= k

w2

µ− k

,

µ.

(3.142) It can

**which is the desired (although implicit) equation for the new eigenenergies be rewritten
**

µ= k µ

w2 − δk

=

w2 δ

k

1 z−k

=

w2

π

δ tan πz

,

z=

µ

δ

.

(3.143)

Hence, = πw 2 δ tan(π

µ /δ)

µ

⇒

1 tan(π

µ /δ)

=

2

µ

Γ

,

Γ=

2πw 2 δ

.

(3.144)

44

CHAPTER 3. ATOMS IN EXTERNAL FIELDS

Figure 3.3: Graphical determination of the eigenvalues

ˆ of H . The abscissa of each intersection point M k is an eigenvalue. Let M k be the point of intersection whose abscissa is between kδ and (k +1)δ (the abscissa of M−k being between −(k +1)δ and −kδ). The associated eigenvalue is denoted Eκ = µ where the Greek index κ corresponds to the Roman index k of the unperturbed states. The two intersections between −δ and δ arise from the unperturbed states |k = 0〉 and |ϕ〉. [Figure taken from COHEN-TANNOUDJI et al., Atom-Photon Interactions, (Wiley, New York, 1998)].

µ

3.3. IMPORTANT MODELS

45

Finding the new eigenenergies µ amounts to ﬁnd the intersections of y = a x with y = 1/ tan(b x) where a = 2/Γ and b = π/δ, and x = µ . This is shown in Fig. 3.3. The new eigenvalues µ are interspersed between the old ones. The larger |k| the closer are the new eigenvalues to the old ones. If µ Γ one has µ k. Using the normalization condition |〈k|ψµ 〉|2 + |〈ϕ|ψµ 〉|2 = 1

k !

(3.145)

we ﬁnd for the projections of the new states on the unperturbed states 2 −1/2 w 〈ϕ|ψµ 〉 = 1 + , − k µ k 2 −1/2 w w . 〈k|ψµ 〉 = 1 + µ− k µ− k k The square bracket can be rewritten using (z − k)

k −2

(3.146)

(3.147)

=

π2 sin2 πz π δ

(3.148)

and yields 1+

k µ

w −

k

2

=1+

π2 w 2 δ

2

1 + tan−2

µ

.

(3.149)

**With the help of (3.144) this can be recast in the form 1+
**

k µ

w −

k

2

=

1 w

2

w +

2

Γ 2

2

+

2 µ

(3.150)

so that 〈ϕ|ψµ 〉 = w +

2

w

Γ 2 2

+

2 µ

1/2

.

(3.151)

Consider an energy interval [ , + d ] such that δ d Γ (3.152)

so that the probability to ﬁnd the formerly discrete state |ϕ〉 within this interval reads dNϕ =

µ ∈[ , +d ]

|〈ϕ|ψµ 〉|2

d δ

|〈ϕ|ψµ 〉|2 .

(3.153)

46 We thus have

**CHAPTER 3. ATOMS IN EXTERNAL FIELDS
**

dNϕ d Γ/2π w2 +

Γ 2 2

=

+

2

.

(3.154)

**In the continuum limit δ → 0 the probability w 2 has vanishing measure and dNϕ d = Γ/2π
**

Γ 2 2

+

2

(3.155)

which is a Lorentzian of width Γ around the energy = ϕ = 0. We learn from this study that discrete levels cease to exist when they are coupled to a continuum and that the continuum states in the vicinity Γ around the energy of the unperturbed, discrete state |ϕ〉 retain memory of |ϕ〉. We ﬁnally show that the decay in this simple model system in exponential. Let us assume that at time t = 0 the system is prepared to be in the state |ϕ〉, |ψ(0)〉 = |ϕ〉 =

µ

w w +

2 Γ 2 2

+

2 µ

1/2

|ψµ 〉.

(3.156)

**As a consequence, the state at a later time will be |ψ(t )〉 =
**

µ

w e−i w +

2 Γ 2 2

µt

+

2 µ

1/2

|ψµ 〉.

(3.157)

**Using (3.151) yields 〈ϕ|ψ(t )〉 =
**

µ

w 2 e−i w2 + Γ 2π

µ ∞ Γ 2 2

µt

+ e−i

2 µ

µt

(3.158)

=

δ→0

δ

w + d

2

Γ 2 2 t

+

2 µ

(3.159)

= =

Γ 2π

e−i

Γ 2 2

−∞

+

2

(3.160) (3.161)

e−Γt /2 ,

t ≥ 0.

For the last step we used the method of residues. The population of the formerly discrete level thus decays exponentially according |〈ϕ|ψ(t )〉|2 = e−Γt , t ≥ 0. (3.162)

3.3. IMPORTANT MODELS

47

We stop the discussion of the model at this point. We only mention that it can be extended toward more than a single discrete state. If, for instance, the population of the formerly discrete state can either reach the continuum directly or via transition to another (formerly) discrete state, an interference effect arises which leads to spectral shapes (Fano proﬁles) depending on the ratio of the relevant coupling strengths w. The fact that we obtain a simple exponential decay law (3.162) is due to the very simple nature of this model system. In fact, it can be shown that real systems cannot decay exponentially on a time scale shorter than the half-time or much longer than the half-time. The deviation from exponential decay at short time scales offers the possibility to alter the dynamics of the quantum system by repeated measurements (Zeno and anti-Zeno effect).

Further reading: Time-dependent perturbation theory is covered in every reasonable quantum mechanics text book. Dyson series, S-matrix, Green’s functions, propagators etc. are usually covered in books on quantum ﬁeld theory or many-body theory. Models and techniques relevant to (weak) laser-atom interaction are discussed in CLAUDE COHEN-TANNOUDJI, JACQUES DUPONT-ROC, GILBERT GRYNBERG, Atom-Photon Interactions, (Wiley, New-York, 1998) and in FARHAD H. M. FAISAL, Theory of Multiphoton Processes, (Plenum, New York, 1987).

**3.3.2 Resonantly coupled discrete levels: Rabi-oscillations
**

Let us consider the Hamiltonian of a two-level system coupled to a laser ﬁeld in dipole approximation, ˆ ˆ ˆ ˆ H (t ) = H0 + W (t ) = ωa |a〉〈a| + ω b |b 〉〈b | − q E z cos ωt . (3.163)

The charge of the particle in atomic units is q (i.e., q = −1 for an electron), and ωa , ω b are the energies of the states |a〉 and |b 〉, respectively. Plugging the Ansatz |ψ(t )〉 = ca (t )e−iωa t |a〉 + c b (t )e−iωb t |b 〉 into the TDSE ˆ i∂ t |ψ(t )〉 = H (t )|ψ(t )〉 (3.164) (3.165)

and multiplication from the left by 〈a| and 〈b |, respectively, leads to 1 ˆ i˙a (t ) = − E q c b (t ) ei∆t 〈a|z|b 〉, c 2 1 ˆ i˙b (t ) = − E q ca (t ) e−i∆t 〈b |z|a〉. c 2 (3.166) (3.167)

48 Here, we introduced the detuning

CHAPTER 3. ATOMS IN EXTERNAL FIELDS

∆ = ωa − ω b − ω = ωab − ω,

(3.168)

made use of 〈a|z|a〉 = 〈b |z|b 〉 = 0 (assuming that |a〉 and |b 〉 have well-deﬁned parity), and neglected the anti-resonant terms ∼ e±i(ωab +ω)t (RWA, see Sec. 3.2) assuming without loss of generality that ωab > 0 and ω > 0. Setting ˆ ˆ q E〈a|z|b 〉 = E|q〈a|z|b 〉| e−iϕ = ΩR e−iϕ ,

ΩR

ˆ ΩR = E |q〈a|z|b 〉|

(3.169)

(3.166) and (3.167) become 1 ˙ ca (t ) = i ΩR ei∆t −iϕ c b (t ), 2 1 ˙ c b (t ) = i ΩR e−i∆t +iϕ ca (t ). 2 The solutions are ca (t ) = c b (t ) = where Ω= Ω2 + ∆ 2 . R (3.174) a1 eiΩt /2 + a2 e−iΩt /2 ei∆t /2 , b1 eiΩt /2 + b2 e−iΩt /2 e−i∆t /2 (3.172) (3.173) (3.170) (3.171)

The constants a1 , a2 , b1 , b2 are determined through the initial conditions, 1 a1 = (Ω − ∆)ca (0) + ΩR e−iϕ c b (0) , (3.175) 2Ω 1 (Ω + ∆)ca (0) − ΩR e−iϕ c b (0) , (3.176) a2 = 2Ω 1 b1 = (Ω + ∆)c b (0) + ΩR eiϕ ca (0) , (3.177) 2Ω 1 b2 = (Ω − ∆)c b (0) − ΩR eiϕ ca (0) . (3.178) 2Ω We thus have i∆ Ωt Ωt − sin ca (t ) = ca (0) cos (3.179) 2 Ω 2 ΩR Ωt +i e−iϕ c b (0) sin ei∆t /2 , Ω 2 i∆ Ωt Ωt + sin c b (t ) = c b (0) cos (3.180) 2 Ω 2 ΩR Ωt +i eiϕ ca (0) sin e−i∆t /2 , Ω 2

3.3. IMPORTANT MODELS

49

which is remarkably complicated considering the fact that we deal only with two states. In the case of exact resonance ∆ = 0 one has Ω = ΩR. Assuming further that at time t = 0 the system is in state |b 〉 so that c b (0) = 1 and ca (0) = 0, Eqs. (3.179) and (3.180) simplify to ca (t ) = ie−iϕ sin c b (t ) = cos ΩR t 2 ΩR t 2 , (3.181) (3.182)

so that the probability to ﬁnd the system, e.g., in the state |b 〉 is w b (t ) = |c b (t )|2 = cos2 ΩR t 2 = 1 2 [1 + cos ΩR t ] , (3.183)

i.e., it oscillates with the frequency ΩR. These oscillations are called Rabi oscillations (or Rabi ﬂoppings). In ﬁrst order time-dependent perturbation theory we saw that the depopulation of the initial state at resonance goes ∼ t 2 which corresponds to the ﬁrst term of the expansion of cos ΩR t . Obviously, perturbation theory is not adequate to describe the population transfer between the two states. Rabi ﬂoppings are employed experimentally to prepare atoms in a certain desired state using lasers that are tuned to the transition of interest. If the pulse duration Tp is chosen such that ΩRTp = π (so-called π-pulses) the, e.g., ground state population is transferred completely to the desired state. As long as the detuning is small compared to transition energies to other states, the two-level approximation is adequate. In the case of nonvanishing detuning ∆ = 0 the population transfer is not complete (i.e., |ca (t )|2 never reaches unity). The Rabi frequency ΩR is proportional to the dipole matrix element [cf. (3.169)]. Hence, the higher the ﬁeld strength, the faster is the population transfer between the states. However, the so-called AC Stark effect modiﬁes the energies of the two states so that a laser frequency that equals the unperturbed level spacing ωab will be detuned. As an example, we shall ﬁnally calculate the Rabi-frequency ΩR for the resonantly ˆ driven 1s→2p transition in atomic hydrogen for a driving laser of ﬁeld amplitude E = 8 9 · 10 V/m. We have for the dipole matrix element 〈a|z|b 〉 = dr r

2

dΩ

φ∗ 2p r

0

∗ Y10 (Ω) r cos ϑ z 2p0

φ1s r

Y00

(3.184)

1s

where Y m (Ω) are the spherical harmonics and Ω is the solid angle (in this context). Using 1 r 2 −r /2 e , Y00 = , (3.185) φ1s = 2r e−r , φ2p0 = 2 6 4π

50 and

CHAPTER 3. ATOMS IN EXTERNAL FIELDS

z = r cos ϑ = r we obtain 〈a|z|b 〉 = In SI units one has ΩR = 1 3 r4 6

4π 3

Y10 (Ω), 256 2 243

(3.186)

dr

e−3r /2 =

0.7449.

(3.187)

ˆ 256 a0 e E h 2 243 ħ

5.4 · 1013 s−1

(3.188)

(with a0 the Bohr radius). For comparison: one atomic frequency unit corresponds to 4.1 · 1016 s−1 , and the laser frequency at 800 nm is 2.3 × 1015 s−1 . Hence, Rabi-ﬂopping is still “slow” for the considered ﬁeld strength both on the inner-atomic time scale and on the time scale of the laser period. An atom driven resonantly emits at the frequencies ω and ω±ΩR (Mollow-spectrum, ﬂuorescence). Corrections stemming from the anti-resonant terms can be taken into account in a perturbative manner (Bloch-Siegert shifts). It is common to introduce in the context of Rabi-ﬂoppings so called dressed states. These states form a new basis in which the Hamiltonian becomes diagonal at resonance. We postpone the introduction of the dressed states until the discussion of the Floquet approach.

Further reading: Rabi-oscillations are discussed in all Quantum Optics text books. We followed MARLAN O. SCULLY and M. SUHAIL ZUBAIRY, Quantum Optics, (Cambridge University Press, Cambridge, 1997). A historic paper on the subject (employing an interesting application of continued fractions) is S.H. AUTLER AND C.H. TOWNES , Stark Effect in Rapidly Varying Fields, Phys. Rev. 100, 703 (1955). A recent review is ULRICH D. JENTSCHURA and CHRISTOPH H. KEITEL, Radiative corrections in laser-dressed atoms: formalism and applications, Annals of Physics 310, 1 (2004).

3.4

Atoms in strong, static electric ﬁelds

Although we assume the external electric ﬁeld to be static in this Section, the following analysis is useful for atoms in laser ﬁelds too, as will become clear below. The Hamiltonian governing an electron moving in a Coulomb potential −Z/r and a static electric ﬁeld E = Ee z reads ˆ Z p2 ˆ + Veff , Veff = − + E z. (3.189) H= 2 r

3.4. ATOMS IN STRONG, STATIC ELECTRIC FIELDS

51

V Ez

z

"over barrier" "tunneling"

−Z/r

Veff

Figure 3.4: Effective potential Veff in ﬁeld direction. The unperturbed Coulomb potential and

the ﬁeld potential are also shown separately. Depending on the initial (and possibly Stark-shifted) state, the electron may either escape via tunneling or classically via “over-barrier” ionization.

The effective potential Veff describes a tilted Coulomb potential (see Fig. 3.4). A perturbative treatment of the problem can be found in almost all quantum mechanics or atomic physics text books (Stark effect). In ﬁrst order (linear Stark effect) the degeneracy with respect to the angular quantum number is removed while the degeneracy in the magnetic quantum number m is maintained. The non-degenerate ground state is only affected in second order (quadratic Stark effect). It is down-shifted since the potential widens in the presence of the ﬁeld. In the case of the hydrogen atom (Z = 1) this down-shift is given by ∆ = −9E 2 /4. Let us ﬁrst point out that, strictly speaking, there exist no discrete, bound states anymore even for the tiniest electric ﬁeld. This is because even a very small ﬁeld gives rise to a potential barrier (see Fig. 3.4) through which the initially bound electron may tunnel. The electric ﬁeld couples all bound states to the continuum and thus, as we have learnt in Section 3.3.1, all discrete states become resonances with a ﬁnite line width. Mathematically speaking, the spectrum of the Hamiltonian (3.189) is unbound from below. However, since the barrier for small ﬁelds is far out, the probability for tunneling is extremely low (note that the tunneling probability goes exponentially down with the distance to be tunneled) and the states are “quasi-discrete”. A strong increase in the ionization probability is expected when the electron can even escape classically, that is, when it does not have to tunnel. In a zeroth order approximation (which, in fact, is wrong for hydrogen-like ions, as will be discussed below) this so-called critical ﬁeld Ecrit may be estimated as follows: assuming that the initial energy of the electron does not change (i.e., Stark effect negligible), classical over-barrier

52

CHAPTER 3. ATOMS IN EXTERNAL FIELDS

ionization sets in when the barrier maximum coincides with the energy level of the electron. The position of the barrier is (for E > 0) located at zbarr = − and the energy at the barrier maximum is Vbarr = −2 Z E. (3.191) Z E (3.190)

**Hence, if we restrict ourselves to the ground state of hydrogen-like ions, we require that =− Z2 2 = −2 Z Ecrit
**

!

⇒

Ecrit =

Z3 16

.

(3.192)

Because of the strong Z-dependence of the critical ﬁeld even with the most intense lasers available today it is not possible to fully strip heavy elements (see Problem 3.5 below). For hydrogen-like ions Eq. (3.192) even underestimates the critical ﬁeld by more than a factor of two, as will be shown soon. The Schrödinger equation with the Hamiltonian (3.189) separates in parabolic coordinates (ξ , η, ϕ), ξ = r + z, η = r − z, 1 r = (ξ + η), 2 1 z = (ξ − η), 2 0 ≤ ξ , η. (3.193)

Here, r is the radial coordinate, and ϕ is the usual azimuthal angle (as in spherical, polar or cylindrical coordinates). Cuts of contours of constant ξ and η in the x z-plane are shown in Fig. 3.5. The Hamiltonian in parabolic coordinates reads ˆ H =− 2 ξ +η ∂ξ (ξ ∂ξ ) + ∂η (η∂η ) − 1 2ξ η ∂ϕ2 − 2Z ξ +η +E ξ −η 2 . (3.194)

Plugging the Ansatz Ψ = f1 (ξ ) f2 (η)eimϕ (3.195) ˆ into the Schrödinger equation Ψ = H Ψ and multiplying by (ξ + η)/2 leads to an equation that can be decoupled into d dξ d ξ d f1 + + ξ− η− m2 4ξ m2 4η − + E 4 E 4 ξ2 η2 f1 + Z1 f1 = 0, f2 + Z2 f2 = 0 (3.196) (3.197)

dξ d f2 η dη dη

2

2

where Z1 , Z2 are separation constants fulﬁlling Z1 + Z2 = Z. (3.198)

**3.4. ATOMS IN STRONG, STATIC ELECTRIC FIELDS
**

9 8 7 6 5 4 3 2 1 0.1 0.1 1 2 3 4 5 6 7 8 9

53

**Figure 3.5: Illustration of parabolic coordinates. Cuts of contours ξ = const. (dashed, values
**

given next to the lines) and η = const. (solid) in the x z-plane (azimuthal symmetry with respect to the z-axis!).

Division by 2ξ and 2η, respectively, yields the two Schrödinger equations − 1 2 d2 + 1 d − m2 − ξ f1 = 2ξ 8 Z2 E − − η f2 = 2η 8 Z1 + E f1 , f2 (3.199) (3.200)

dξ 2 ξ dξ 4ξ 2 1 d2 1 d m2 − + − 2 dη2 η dη 4η2

4 4

which have the same shape like two Schrödinger equations in cylindrical coordinates and the potentials Z1 E Z2 E Vξ = − + ξ, Vη = − − η. (3.201) 2ξ 8 2η 8 Both potentials have a Coulombic part and a linear contribution, like Veff in (3.189). However, because ξ , η ≥ 0, the potential Vξ has only bound states (we assume E > 0). The potential Vη instead displays a barrier. Hence, in parabolic coordinates ionization happens with respect to the η coordinate while the electron is expected to remain rather conﬁned in ξ . The consequences of this in Cartesian coordinates can be understood with the help of Fig. 3.5: conﬁnement to a region ξ < ξmax implies preferred electron emission toward negative z with a lateral spread that can be estimated by the conﬁning contour ξmax . The potentials Vξ and Vη are called “uphill” and “downhill potential”, respectively. They are illustrated in Fig. 3.6. Given an energy one ﬁnds a sequence of Z1 for which the solution of the Schrödinger equation in ξ , Eq. (3.199), leads to normalizable bound states. This sequence can be labelled by the number of nodes in f1 for ξ > 0, n1 = 0, 1, 2, . . . (note that Z1 < 0 is also possible). The second equation

54

V

CHAPTER 3. ATOMS IN EXTERNAL FIELDS

"uphill" (bound motion)

Vξ

ξ,η

"downhill" (ionization)

Vη

**Figure 3.6: Illustration of the potentials Vξ and Vη [Eqs. (3.201)]. The “uphill potential” Vξ
**

(for E > 0) supports only bound states while the “downhill potential” Vη displays a barrier through which the electron may tunnel.

(3.200) has to be solved for Z2 = Z − Z1 and the same energy . This is possible because ˆ the corresponding Hamiltonian Hη [i.e., the square bracket in (3.200)] is neither bound from below nor from above. In the ﬁeld-free case E = 0 the two Schrödinger equations (3.199) and (3.200) are identical, and the relation between the “usual” principal quantum number n and the parabolic quantum numbers n1 , n2 are as follows: ni + |m| + 1 2 =n Zi Z , n1 + n2 + |m| + 1 = n, i = 1, 2. (3.202)

Instead of working directly with the parabolic coordinates ξ and η, one can perform an additional, simple coordinate transformation u= 2ξ , v= 2η (3.203)

**which, after multiplication of the new Schrödinger equation by (u 2 + v 2 )/4, and plugging in the Ansatz Ψ = Φ u (u)Φv (v)eimϕ yields − 1 1 ∂ u (u∂ u ) − m2
**

2

2 u u m2 1 1 ∂v (v∂v ) − 2 − 2 v v

1 1 + Ω 2 u 2 − g u 4 Φ u = Z1 Φ u , 2 4 1 1 + Ω2 v 2 + g v 4 Φ v = Z 2 Φ v , 2 4

(3.204) (3.205)

**3.4. ATOMS IN STRONG, STATIC ELECTRIC FIELDS
**

where, again, Z = Z1 + Z2 is used, and Ω and g are deﬁned as 1 Ω2 = − , 2 4 ≤ 0, E g =− . 4

55

(3.206)

The Schrödinger equations (3.204) and (3.205) have the shape of two-dimensional oscillators (with radial coordinates u and v, respectively) of frequency Ω and with a quartic perturbation that is proportional to the electric ﬁeld. In the ﬁeld-free case, the Coulomb problem is mapped to two two-dimensional oscillators where, however, the energy assumes the role of the oscillator frequency, and the nuclear charge (splitted into Z1 and Z2 ) assumes the role of the energy. The transformation to the coordinates (u, v, ϕ) corresponds to the Kustaanheimo-Stiefel transformation. Let us now evaluate an improved critical ﬁeld for the case of hydrogen-like ions. As mentioned above, formula (3.192) underestimates the critical ﬁeld by more than a factor of two. In the unperturbed case ( g = 0) and for m = 0 (groundstate) the solutions to (3.204) and (3.205) are Gaussians. We therefore use Φ u (u) = au π e−au u

2 /2

(3.207)

**(and analogous for v) as trial functions with parameters a u and av . The “energy” then is
**

∞

Z1 ( g ) = 2π

0

du

ˆ uΦ∗ H u Φ u u

=

1 au

Ω2 2

−

2 au

2

+ au −

g

2 2a u

.

(3.208)

**Minimizing this energy yields up to ﬁrst order in g au = Ω 1 − The oscillator “energies” are Z1 ( g ) = Ω 1 − g 2Ω3 , Z2 ( g ) = Ω 1 + g 2Ω3 . (3.210) g Ω
**

3

,

av = Ω 1 +

g Ω3

.

(3.209)

Note that this is consistent with the fact that the linear Stark effect vanishes for the ground state since Z1 (g ) + Z2 ( g ) = 2Ω (3.211) is independent of the ﬁeld g . Since Z1 + Z2 = Z we have Z = 2Ω which is [see (3.206)] equivalent to = −Z 2 /2, as it should for the ground states of hydrogen-like ions. In physical coordinates the variationally determined wave function for, e.g., hydrogen (Z = 1) reads 1 − 4E 2 −r −2E ·r e e , (3.212) ΨH (r ) = π

56

CHAPTER 3. ATOMS IN EXTERNAL FIELDS

i.e., the unperturbed wave function is multiplied by a “deformation factor”. If E > 0 we have g < 0 and vice versa. Let us assume g > 0 so that the u-oscillator displays a barrier while the v-oscillator does not. The barrier is located at ubarr = Ω/ g 4 2 and the energy at the barrier maximum is Ω2 ubarr /2− g ubarr /4 = Ω4 /(4 g ). Claiming that at the critical ﬁeld strength the energy of the u-state coincides with the barrier-energy gives us Z1 ( g ) = Ω − g 2Ω

2

=

Ω4 4g

⇒

gcrit = Ω3 (1 − 2−1/2 )

0.3 Ω3

(3.213)

**which translates [using (3.206)] to
**

H−like Ecrit = ( 2 − 1) 3/2

.

(3.214)

H−like = 0.147 instead of the 0.0625 preIn the case of atomic hydrogen one obtains Ecrit dicted by (3.192). The wrong prediction of (3.192) is due to the erroneous assumption that one can consider the electron motion in z-direction and in lateral direction as being independent. Instead, the problem separates in parabolic coordinates! However, since the “exceptional” symmetry of hydrogen-like ions is broken in many-electron atoms, the over-barrier formula given (and to be derived) in Problem 3.6 below [Eq. (3.241)] is useful and quite accurate for many practical applications.

3.4.1 Tunneling ionization

Going one step beyond a classical over-barrier analysis amounts to take tunneling into account. This can be done in a semi-classical way. Let us consider the tunneling of the electron in atomic hydrogen through the barrier of the “downhill potential” in Fig. 3.6. We assume the electron is initially in the 1s ground state. The Schrödinger equation (3.200) reads for m = 0, Z2 = 1/2, = −1/2 − Substituting χ (η) = yields the Schrödinger equation ∂ 2χ 1 1 1 1 + 2 + Eη χ = 0. + − + 4 2η 4η 4 ∂ η2 1 ∂ 2χ 2 ∂ η2 (3.217) η f2 (η) (3.216) 1 2 d2 dη

2

+

1 d η dη

−

1 4η

−

E

1 η f2 (η) = − f2 (η). 8 8

(3.215)

Comparison with − + V (η)χ = εχ (3.218)

3.4. ATOMS IN STRONG, STATIC ELECTRIC FIELDS

57

1/ E η0

sufﬁciently low ﬁelds E is in good approximation given by η1 located inside the barrier where 1 η0 1/E holds.

Figure 3.7: Plot of the potential V (η) [Eq. (3.219)] for E = 0.0075. The tunnel “exit” η1 for

1/E. The matching point η0 is

shows that we effectively deal with one-dimensional motion of an electron in the potential 1 1 1 1 + 2 + Eη (3.219) V (η) = − 2 2η 4η 4 with total energy 1 ε=− . 8 The potential V (η) is of the form depicted in Fig. 3.7. We now match at a position η0 inside the barrier, 1 the “left” quasi-classical wave function χleft (η) = − iC | p|

η

(3.220)

η0

1/E

(3.221)

exp

η0

p(η ) dη

(3.222)

**with the “right” quasi-classical outgoing wave function χright (η) = C p
**

η

exp i

η0

p(η ) dη − iπ/4

(3.223)

58 where p(η) =

CHAPTER 3. ATOMS IN EXTERNAL FIELDS

2[ε − V (η)] =

1 1 1 1 − + + 2 + Eη. 4 2η 4η 4

(3.224)

The semi-classical approximation breaks down at the classical turning point η1 1/E since p(η1 ) = 0. In general, semi-classical wave functions are accurate as long as the de Broglie wave length 2πħ h λdB = (3.225) p is small compared to the length scale characterizing changes in the potential (i.e., the potential should be sufﬁciently “ﬂat”). For vanishing momentum p the de Broglie wave length is inﬁnite so that the semi-classical approximation necessarily breaks down. However, for the calculation of the probability ﬂux out of the potential the disagreement between the semi-classical wave function and the exact wave function in a narrow region around the classical turning point η1 plays no role. For the determination of the normalization constant C we set the left wave function at position η0 equal to the unperturbed wave function so that η0 1 π e−(ξ +η0 )/2 = − iC | p0 | (3.226)

with p0 = p(η0 ). The “uphill” coordinate ξ appears as a parameter here which will be integrated out later on; in other words: the wave function is assumed to retain its ground state shape with respect to ξ (i.e., the Stark effect is neglected). We obtain for the right wave function χright (η, ξ ) = i so that |χright (η, ξ )|2 = η 0 | p0 | π p(η) η 0 | p0 | π p(η)

η

e−(ξ +η0 )/2 exp i

η0

p(η ) dη − iπ/4

(3.227)

exp −ξ − η0 + 2ℜ i

η η0

p(η ) dη (3.228)

where ℜ denotes the real part. Because of (3.221) we can expand p(η) in = 1/η, 1 1 + ··· outside barrier, η > η1 Eη − 1 + 2 η Eη − 1 . (3.229) p(η) = 1 1 i 1 − Eη + + ··· inside barrier, η < η1 2 iη 1 − Eη Since Eη0 1 it is sufﬁcient to take | p0 | = 1/2. In order to keep the leading terms dependent on E in the prefactor as well as in the exponent, we set in the denominator

3.4. ATOMS IN STRONG, STATIC ELECTRIC FIELDS

59

of the prefactor in (3.228) p(η) = ( Eη − 1)/2. In the exponent we integrate inside the barrier and have to keep both terms in the expansion (3.229). We thus obtain η1 η0 1 Eη − 1 − dη . |χright (η, ξ )|2 = e−(ξ +η0 ) exp − π Eη − 1 η Eη − 1 η0 (3.230) The integral can be solved. Using η1 1/E and η0 E 1 we obtain for the probability density outside the barrier |χright (η, ξ )| =

2

4 e−ξ πE Eη − 1

e−2/(3E) .

(3.231)

**The total probability current through a plane perpendicular to the z-axis is
**

∞

w=

0

| f1 (ξ ) f2 (η)|2 v z 2πρ dρ

(3.232)

where f1 (ξ ), f2 (η) are the wave functions introduced in (3.195), v z is the velocity in z-direction and ρ is the radial cylindrical coordinate. The ξ -dependent part | f1 |2 is included in our |χright (η, ξ )|2 so that

∞

w=

0

|χright (η, ξ )|2 η

v z 2πρ dρ.

(3.233)

With z = (ξ − η)/2 1 2 so that

**−η/2 for small ξ and large η, we estimate for v z 1 1 2 v z − Eη 2 2
**

∞

2 vz + E z

⇒

vz

Eη − 1

(3.234)

w=

0

|χright (η, ξ )|2 η

Eη − 1 2πρ dρ.

(3.235)

Finally, with ρ= ξη ⇒ dρ = d ξ η = 1 2 η ξη dξ + 1 ξ 2 ξη dη 1 2 η ξ dξ (3.236)

**(where the last step again follows from η
**

∞

ξ ) we arrive at ξη 1 2 4 E η ξ

∞

w=

0

|χright (η, ξ )|2 η

Eη − 1 2π

dξ =

0

4 E

e−2/(3E) e−ξ dξ

(3.237)

⇒

w=

e−2/(3E) .

(3.238)

60

**CHAPTER 3. ATOMS IN EXTERNAL FIELDS
**

1/16 0.147

**Figure 3.8: The LANDAU-rate (3.238) vs ﬁeld strength E. The vertical lines indicate the (here
**

wrong) over-barrier ﬁeld strength (3.192) (1/16, dashed) and the correct (3.214) 0.147 (solid), respectively.

This is the L ANDAU-rate for tunneling ionization of atomic hydrogen from the ground state. Its derivation is given as an exercise in the Quantum Mechanics volume of L ANDAU & L IFSHITZ ! It has been checked numerically that (3.238) is exact in the limit of low ﬁeld strengths E while it overestimates ionization as the over-barrier ﬁeld strength is approached. Figure 3.8 shows w vs the ﬁeld strength E. It is, of course, desirable to extend the above calculation to laser ﬁelds, to more complex atoms, and to higher ﬁeld strengths. All directions have been pursued, and there exists a vast amount of literature on tunneling ionization (see “Further reading” below). Here we have restricted ourselves to the “generic” case of atomic hydrogen where the typical tunneling exponent ∼ E −1 already arises, as derived above. The most commonly used tunneling formula is the so-called ADK-formula (named after AMMOSOV, DELONE, AND KRAINOV although it was, even more generally, derived much earlier by POPOV):

2 w = Cn ∗ f ( , m)

Z2 2n ∗2

3E n ∗3 πZ 3

2Z 3 E n ∗3

2n ∗ −|m|−1

exp −

2Z 3 3n ∗3 E

(3.239)

with Cn ∗ = 2e n∗

n∗

(2πn ∗ )−1/2 ,

∗

f ( , m) =

(2 + 1)( + |m|)! 2|m| |m|! ( − |m|)!

,

n∗ =

Z 2

ip

,

(3.240) and e = 2.71828. n , , and m are the (effective) quantum numbers of the initial state with ionization potential ip . The behavior of w as a function of E is again dominated

3.5. ATOMS IN STRONG LASER FIELDS

61

by the exponent ∼ E −1 . The varying laser ﬁeld is taken into account by cycle-averaging E(t ). Hence, by E in (3.239) the laser electric ﬁeld amplitude is meant. The expression for circular polarization is obtained by multiplying (3.239) with (πZ 3 /3E n ∗3 )1/2 . The expression is supposed to be increasingly accurate as E Z 3 /16n 4 , n ∗ 1, and n∗. Experimentalists are used to compare their measured results for ion yields with the corresponding ADK-prediction. Often, the agreement is satisfactory if one allows for an adjustment of the laser intensity (multiplication of the latter by factors between, say, 0.5 and 2).

Problem 3.5 Estimate the laser intensity needed to fully strip Uranium. Problem 3.6 Show (using an over-barrier estimate) that the (classically) expected appearance intensity Iapp,Z for a charge state Z of an atom with ionization potential ip,Z is given by Iapp,Z =

4 ip,Z

16Z 2

.

(3.241)

Further reading: The hydrogen atom in parabolic coordinates is treated in many Atomic Physics and Quantum Mechanics textbooks (i.e., L ANDAU & LIF SHITZ ’ S Quantum Mechanics volume). The correct over-barrier ﬁeld strength of hydrogen-like ions is calculated in D. BAUER, Ejection energy of photoelectrons in strong ﬁeld ionization, Phys. Rev. A 55, 2180 (1997). A review of tunneling ionization is given by V.S. POPOV in Tunnel and multiphoton ionization of atoms and ions in a strong laser ﬁeld (Keldysh theory), Physics Uspekhi 47, 855 (2004).

**3.5 Atoms in strong laser ﬁelds
**

There are at least three different energy scales (and the related time scales) in the interaction physics of atoms in strong laser ﬁelds: (i) the ionization potential ip = | |, (ii) the photon energy ω, and (iii) the ponderomotive energy Up [see Eq. (2.14)]. The pulse duration may introduce an additional laser-related time-scale while the energy spectrum of the atom, through typical transitions, could introduce an additional species-related time-scale. If one ignores the two latter parameters, the atomic species enter through | | only. In case ω > | | Up or | | > ω Up perturbation theory in lowest nonvanishing order (LOPT) can be applied. In contrast, when with the increasing laser intensity the regime | | > Up > ω is reached, non-perturbative effects such as above-threshold

62

CHAPTER 3. ATOMS IN EXTERNAL FIELDS

ionization (ATI) or channel-closing take place. This regime is commonly referred to as (nonperturbative) multiphoton ionization (MPI). Finally, increasing the intensity further (or decreasing the photon energy) one arrives at Up > | | > ω. Translated into the timedomain this implies that both the inner-atomic time-scale and the ionization dynamics are “fast” with respect to a laser period. If this is the case, a quasi static ﬁeld ionization picture may be applied where, at the instant of ionization t , the electron “feels” an effective potential which is the sum of the Coulomb (or effective core) potential and the instantaneous potential of the laser, as depicted in Fig. 3.4. If the ﬁeld reaches the critical ﬁeld estimated above, the electron may escape classically over the barrier [over-barrier or barrier suppression ionization (OBI) and (BSI), respectively]. Below the critical ﬁeld strength the electron can escape via tunneling through the barrier (tunneling ionization). MPI and tunneling are deﬁned by Up Up < 1 (MPI), > 1 (tunneling). (3.242) | | | | KELDYSH introduced a parameter γ as the ratio of “tunneling time” and laser period, or, expressed in frequencies, γ = ω/ω t with the tunneling frequency ω t estimated by ω t = E/ 2| | where E is the electric ﬁeld |E |. Hence, one has the Keldysh parameter γ= ω ωt = | | 2Up , (3.243) 2 which does not (3.244)

and conditions (3.242) can be also stated as (neglecting a prefactor matter here) γ > 1 (MPI), γ < 1 (tunneling).

Numerous strong laser-atom experiments operate around γ 1 or at γ > 1 and are thus not in the tunneling domain. Taking, for instance, the case of atomic hydrogen in an 800 nm and 1014 W/cm2 laser pulse one ﬁnds γ 1.1. This is a typical value for ATI measurements. What are the differences between the ionization dynamics in the MPI and in the tunneling domain? Since in the tunneling regime the process is fast compared to a laser period, signiﬁcant ionization occurs during a single half laser cycle, predominantly around the electric ﬁeld maximum because the barrier is lowest then. Furthermore, in tunneling ionization the quiver amplitude E/ω 2 of the freed electron in the laser ﬁeld is large compared to the atomic dimension while in MPI this is not the case. This has consequences for the rescattering dynamics which is responsible for various effects, such as the ATI plateau, high-harmonic generation, and nonsequential ionization, as will be discussed below.

3.5.1

Floquet formalism

When we discussed atoms in strong, static electric ﬁelds in Sec. 3.4 we made use of the fact that in the tunneling regime the laser ﬁeld may be considered “quasi-static” since

3.5. ATOMS IN STRONG LASER FIELDS

63

the inner-atomic dynamics is much faster than a laser period. What else could we take advantage of in the treatment of atoms in laser ﬁelds in order to render it tractable? If the laser pulse duration is long, i.e., if the pulse contains many laser cycles, we may in good approximation consider it inﬁnitely long. As a consequence the Hamiltonian will then be periodic, ˆ ˆ ˆ H (t ) = H0 + W (t ), ˆ ˆ W (t + T ) = W (t ), T= 2π ω , (3.245)

and the TDSE will be a partial differential equations with periodic coefﬁcients. This type of problem has been studied by FLOQUET more than 120 years ago (see “Further reading” below). The Floquet theorem tells us that the TDSE ˆ(t )|Ψ(t )〉 = 0, has solutions of the form |Ψ(t )〉 = e−iεt |Φ(t )〉, |Φ(t + T )〉 = |Φ(t )〉, (3.247) ˆ(t ) = H (t ) − i∂ ˆ

t

(3.246)

i.e., the wave function |Φ(t )〉 is periodic (while |Ψ(t )〉 itself is not!). Note that the Bloch theorem used in solid state physics to treat particle motion in periodic potentials is the Floquet theorem applied to spatially periodic systems. Inserting (3.247) into (3.246) leads to the eigenvalue equation ˆ(t )|Φ(t )〉 = ε|Φ(t )〉. ε is called quasi-energy. Note that if ε and |Φ(t )〉 solve (3.248), then also ε = ε + mω, |Φ(t )〉 = eimωt |Φ(t )〉, m∈ (3.249) (3.248)

**do so. Let |α〉 be the solution of the unperturbed problem ˆ H0 |α〉 =
**

0 |α〉. α

(3.250)

**Because of the periodicity of |Φ(t )〉 we can expand
**

∞

|Ψ(t )〉 = e

−iεt

|Φ(t )〉 = e

−iεt n=−∞ α

Φ(n) |α〉e−inωt α

(3.251)

where the expansion coefﬁcients Φ(n) are time-independent. Inserting (3.251) into α (3.246) gives ˆ [H (t ) − ε − nω]Φ(n) |α〉e−inωt = 0. (3.252) α

nα

Multiplying from the left with 〈β|, eimωt , and integrating T −1

T 0

dt yields (3.253)

nα

ˆ [〈β|H (m−n) |α〉 − (ε + mω)δn m δαβ ]Φ(n) = 0 α

64

CHAPTER 3. ATOMS IN EXTERNAL FIELDS

with the time-independent Hamiltonian ˆ H (m−n) = Introducing the Floquet state |αn〉 = |α〉 ⊗ |n〉, we can recast (3.253) into

nα

1 T

0

T

ˆ H (t ) ei(m−n)ωt dt .

(3.254)

〈t |n〉 = einωt

(3.255)

ˆ [〈βm|HF |αn〉 − ε〈βm|αn〉]Φ(n) = 0 α

(3.256)

ˆ where HF is the Floquet Hamiltonian whose matrix elements read ˆ ˆ 〈βm|HF |αn〉 = 〈β|H (m−n) |α〉 − mωδ mn δαβ . Hence, we obtain the eigenvalue equation ˆ [〈βm|HF |αn〉Φ(n) = εΦβ α

(m)

(3.257)

(3.258)

nα

**or, in matrix notation,
**

HF Φ = εΦ.

(3.259)

Here, HF and Φ are an inﬁnite matrix and an inﬁnite vector, respectively. In practice, the size of the system has to be truncated, of course. In order to illustrate the Floquet approach let us return to the two-state problem of Sec. 3.3.2 where the Hamiltonian reads ˆ ˆ H (t ) = ωa |a〉〈a| + ω b |b 〉〈b | − q E z cos ωt ,

ˆ H0 ˆ −W (t )

ωa > ω b .

(3.260)

**We thus have ˆ H (n) = 1 T
**

0 T

ˆ dt H (t ) einωt ˆ qE z 2T ˆ qE z 2

0 T

ˆ = H0 δn0 − ˆ = H0 δn0 −

dt einωt eiωt + e−iωt (δn,−1 + δn1 ), (3.261)

i.e., a tridiagonal Hamiltonian in the “photon subspace”. For (3.257) we obtain 1 ˆ ˆ ˆ 〈βm|HF |αn〉 = 〈β|H0 |α〉 − mωδαβ δnm − q E〈β|z|α〉(δ m,n−1 + δ m,n+1 ) (3.262) 2

**3.5. ATOMS IN STRONG LASER FIELDS
**

ˆ so that (using 〈β|H0 |α〉 = ωα δαβ ) (3.258) reads

∞ |b 〉

65

n=−∞ |α〉=|a〉

**1 (m) ˆ (ωα − mω)δαβ δ mn − q E〈β|z|α〉(δ m,n−1 + δ m,n+1 ) Φ(n) = εΦβ . α 2 (3.263) 1 1 ˆ A = − q E〈a|z|b 〉 = − ΩRe−iϕ , 2 2
**

(m) α

Deﬁning = ωα − mω, (3.264)

**the corresponding matrix equation has the following structure (e.g., around m = 0): (−1) a A∗ A
**

(−1) b

A∗

(0) a (0) b

A

A∗

(1) a

A A∗

A (1)

b

Φ(−1) a (−1) Φb Φ(0) a (0) Φb Φ(1) a (1) Φb

= ε

Φ(−1) a (−1) Φb Φ(0) a (0) Φb Φ(1) a (1) Φb

.

(3.265)

In Sec. 3.3.2 we applied the rotating wave approximation (RWA). In the Floquet framework this corresponds to allow only for transitions between Floquet states |αn〉 and (m) (n) |βm〉 of equal energies α = β . Hence,

(n) a

= ωa − nω = ω b − mω =

(m) b

!

(m) b

(3.266) (3.267)

⇒

(n) a

−

= ∆ = ωa − ω b − (n − m) ω

ωab =1

!

where ∆ is the detuning (3.168), and we are only interested in one-photon transitions between |a〉 and |b 〉 (so that n − m = 1). It would have been smarter to choose the opposite sign for n in the Fourier expansion (3.251) since then the energy would be, more intuitively, the atomic energy plus the number of photons (as if we quantized the electromagnetic ﬁeld). However, in most of the literature on Floquet theory the sign convention is like in (3.251). Equation (3.265) now reduces to the 2 × 2 equation

(n−1) b

A∗

(n) a

A

Φb Φ(n) a

(n−1)

=ε

Φb Φ(n) a

(n−1)

.

(3.268)

The eigenvalues are 1 1 1 (n) ε1,2 = (ωa + ω b ) + ω −n ± 2 2 2 Ω2 + ∆ 2 . R (3.269)

66

**CHAPTER 3. ATOMS IN EXTERNAL FIELDS
**

Ω n= −1 ωa (ωa + ωb )/2 ωb n= 2 Ω n= 0 n= 1 Ω Ω

**Figure 3.9: Illustration of Eq. (3.269) for ∆ = 0. The coupling of the two unperturbed levels b
**

and a to the laser ﬁeld gives rise to an inﬁnite manifold of pairs of ﬁeld-dressed levels (labelled by n). Because of (3.249) all the different ns are equivalent. The ﬁeld dressed levels are separated by the energy (3.174) (which equals ΩR for the vanishing detuning considered here).

The ﬁrst term is the energy half way between |b 〉 and |a〉, the second term is the energy of the “photon ﬁeld”, and the third term gives rise to two levels, separated by the frequency (3.174). Figure 3.9 illustrates the situation for vanishing detuning ∆ = 0. The energy levels (3.269) are called ﬁeld dressed energy levels. Let us ﬁnally calculate the ﬁeld dressed states for our two-state problem in RWA and vanishing detuning. Because of (3.249) we are free to choose, say, n = 1. We also can, without loss of generality, set ω b = 0. Vanishing detuning ∆ = 0 then implies ωa = ω. Moreover we assume A to be real. Then 1 ε1,2 = ± ΩR (3.270) 2 and the eigenvalue problem reduces to 0 A A 0 The matrix

M=

(0) (0)

Φb Φ(1) a 1 2

= ε1,2

Φb Φ(1) a

.

(3.271)

−1 1 1 1 Ψ− Ψ+

= M−1

(3.272)

**diagonalizes (3.271) and yields 1 2 where Ψ− = ΩR 0 0 −ΩR 1 (Φ(1) − Φ b ), a
**

(0)

= ε1,2 1 2

Ψ− Ψ+ (Φ(1) + Φ b ) a

(0)

(3.273)

2 are the ﬁeld-dressed states or Floquet states.

Ψ+ =

(3.274)

3.5. ATOMS IN STRONG LASER FIELDS

67

**3.5.2 Non-Hermitian Floquet theory
**

As long as we are dealing only with discrete states the quasi energy ε is real. If, on the other hand, we allow for transitions into the continuum, e.g., via (multiphoton) ionization, the quasi-energies become complex, Γ ε = ε0 + ∆ε − i . 2 (3.275)

Here, ε0 is the unperturbed energy, ∆ε is the AC Stark shift, and Γ is the ionization rate [cf. Eq. (3.162)]. One may wonder why a Hermitian Floquet Hamiltonian should yield complex eigenvalues. The reason for complex quasi-energies lies in the boundary conditions. Decaying dressed bound states or dressed resonances must fulﬁll the so-called Siegert boundary conditions. Instead of explicitly taking these boundary conditions into account one may apply the complex dilation (also called complex scaling) method. Let us write (3.251) in position space representation as

∞

Ψ(r , t ) = e−iεt Φ(r , t ) = e−iεt

n=−∞ (κ)

e−inωt

(n) 1 (κ) ΦN LM SN L (r )YLM (Ω) r N LM

(3.276)

where SN L are Sturmian functions, YLM (Ω) are spherical harmonics, N LM are principal, angular momentum, and magnetic quantum number, respectively, and κ is a scaling parameter which may be complex. Sturmian functions proved useful in calculations involving Coulomb potentials because they have the following properties (independent of κ):

∞ 0

1 SN L SN L dr = 0 r

∞

for

N =N

(3.277) (3.278)

SN L SN L dr = 1,

0

and their overlap matrix is tridiagonal. Note that none of the Sturmian functions under the integrals in (3.277), (3.278) have to be taken complex conjugated. Sturmian functions can be expressed in terms of Laguerre polynomials (note that the deﬁnition of the Sturmians is not unique in the literature), SN L (r ) =

(|κ|)

|κ|(N − 1)! (N + L)(N + 2L)!

(2|κ|r )L+1 e−|κ|r L2L+1 (2|κ|r ) N −1

(3.279)

where we specialized on a real and positive κ = |κ| for the moment. Complex scaling amounts to the transformation of the position space coordinate r → r eiθ (3.280)

68

CHAPTER 3. ATOMS IN EXTERNAL FIELDS

where θ is a real angle. Imagine we express the matrix elements of the non-Hermitian Floquet Hamiltonian in (3.258) in position space representation. The complex scaled Floquet Hamiltonian is obtained as

HF (θ) (r ) = HF (eiθ r ).

(3.281)

Transforming the Floquet Hamiltonian in this manner turns out to be equivalent to ˆ calculate the matrix elements of HF using the complex Sturmians SN L (r ) =

(κ)

−iκ(N − 1)! (N + L)(N + 2L)!

(−2iκr )L+1 eiκr L2L+1 (−2iκr ) N −1

(3.282)

if the rotation angle θ and the complex scaling parameter κ are related through θ= π 2 − arg κ. (3.283)

The Siegert boundary condition will be automatically fulﬁlled if κ lies within the ﬁrst quadrant of the complex κ-plane and is chosen “properly” (see example in Fig. 3.11). So what does complex scaling do to the energy spectrum? Note that κ is, dimensionally, a momentum. From (3.283) can be inferred that the angle of κ with the imaginary axis of the complex κ-plane is θ. Because energy is ∼ κ2 we see from (3.283) that energy eigenstates (previously all on the real energy-axis, of course) will be rotated by 2θ into the lower half of the complex energy plane. In the absence of the perturbation and if κ is chosen properly, only the continuum states are rotated (about the continuum threshold) while the bound states remain on the real axis. However, if the perturbation (the laser ﬁeld) is present, also the formerly discrete, real levels acquire an imaginary contribution to their quasi-energy ε, namely the −iΓ/2 in Eq. (3.275). This is illustrated in Fig. 3.10. We mentioned above that κ has to be chosen “properly”. What do we mean by that? The modulus |κ| should be chosen such that the states of interest are well represented with as few as possible Sturmian functions in the numerical basis set. Since (|κ|) SN L (r ) ∼ e−|κ|r , |κ| is obviously related to the width of the states in position space (if we are interested in the shift of the H(1s) state, for instance, |κ| close to one would be a reasonable choice). arg κ is directly related to θ [cf. Eq. (3.283)]. It turns out that the quasi-energies become quasi-stationary up to high accuracy (i.e., up to 6 or more decimal places) within a certain θ-interval. An illustrative example is shown in Fig. 3.11. Figure 3.12 shows how resonances (where the photon energy ﬁts exactly with a transition energy) are related to avoided crossings of the dressed energies. Let us consider an experiment where we drive atomic hydrogen with a laser frequency around the 1s ↔ 2p-resonance at ω = −1/8 − (−1/2) = 0.375. Let us ﬁrst keep the driving ﬁeld strength very low so that the Rabi-frequency is small. From Fig. 3.9 we then expect at resonance the two dressed states being very close to one of the unperturbed states. In fact,

3.5. ATOMS IN STRONG LASER FIELDS

69

Im ε

(a)

Im ε

(b)

discrete states ...

x

x x x xx

continuum threshold

2θ

Re ε

continuum

x

x

x x x x

new continuum threshold

Re ε

Figure 3.10: Illustration of the effect of complex scaling on the eigenenergies. Without perturbation (a) the discrete states remain on the real energy-axis while the continuum is rotated by 2θ about the continuum threshold into the lower half of the complex energy plane. With perturbation (b) the discrete states acquire a negative imaginary contribution −iΓ/2 where Γ is the ionization rate. They may also be shifted horizontally (∆ε, AC Stark effect).

**Figure 3.11: Quasivariational determination of an optimal value of θ in the DC Stark case
**

ˆ (E = F = 0.1, ω = 0) in the complex energy-plane. In the case of N = 10 basis functions (per atomic symmetry) a stationary point near θ = 0.4 is found. [From A. MAQUET, SHIH-I CHU, and WILLIAM P. REINHARDT, Stark ionization in dc and ac ﬁelds: An L2 complex-coordinate approach, Phys. Rev. A 27, 2946 (1983).]

70

CHAPTER 3. ATOMS IN EXTERNAL FIELDS

Figure 3.12: Real part of the quasi-energy ε for laser-driven atomic hydrogen as a function of

ˆ the laser frequency ω and for three different driver amplitudes E = F , as given in the plot. Avoided crossings occur at the 1s ↔ 2p-resonance frequency ω = 0.375. The separations of the quasi-energies at resonance (indicated by the colored arrows) equal the corresponding Rabifrequencies. [From A. MAQUET, SHIH-I CHU, and WILLIAM P. REINHARDT, Stark ionization in dc and ac ﬁelds: An L2 complex-coordinate approach, Phys. Rev. A 27, 2946 (1983), colored arrows added by the author of these Lecture Notes.]

Fig. 3.12 explains how this comes about. For a small driving ﬁeld far off any resonance the dressed energies are close to the unperturbed ones. As the resonance at 0.375 is approached the dressed energy (which once was the 2p-energy −1/8) “collides” with the 1s-energy. However, the energies do not cross. Instead, as ω becomes > 0.375 the former 2p state assumes the role of the 1s state while the former 1s state continues like the 2p state for ω < 0.375. The separation of the two quasi-energy levels at resonance is given by Ω. As expected, the separation at resonance increases with increasing driver ˆ strength since Ω ∼ |E| = F . However, the resonance frequency will also shift due to the AC Stark effect [i.e., the ∆ε in (3.275)]. Figure 3.13 shows the ionization rate of H(1s) for λ = 1064 nm laser light as a function of the laser intensity, calculated using the non-Hermitian Floquet method. At this wavelength at least 12 photons must be absorbed by the electron in order to escape. The lowest order perturbation theory (LOPT) results for S excess photon-ionization (i.e., (12 + S)-photon ionization) are included in Fig. 3.13. They by far overestimate the ionization rate. The exact Floquet-result displays an interesting structure which can be explained in terms of so-called Freeman resonances. As the AC Stark up-shift of the continuum (which is given by the ponderomotive potential Up ) increases, the min-

3.5. ATOMS IN STRONG LASER FIELDS

71

**Figure 3.13: Ionization rate vs laser intensity for H(1s) irradiated by linearly polarized light
**

of wavelength λ = 1064 nm. Dashed curves are partial rates for (12 + S)-photon ionization obtained within LOPT. The arrows indicate the intensities at which the real part of the 1s Floquet eigenvalue crosses the 13- and 14-photon ionization thresholds. [From R.M. POTVLIEGE and ROBIN SHAKESHAFT, Multiphoton processes in an intense laser ﬁeld: Harmonic generation and total ionization rates for atomic hydrogen, Phys. Rev. A 40, 3061 (1989).]

imum number of photons required for ionization increases from 12 to 13 (ﬁrst arrow) and to 14 (second arrow). After, with increasing intensity, these thresholds are passed, structures appear, indicating a strong enhancement of the ionization rate at certain laser intensities. It turns out that this is due to Rydberg states that are brought into (12 + S)photon resonance with the ground state via the AC Stark effect (Freeman resonances).

**3.5.3 High-frequency Floquet theory and stabilization
**

ˆ The coupling W (t ) to the laser ﬁeld in (3.245) reads in dipole approximation and velocity gauge 1 ˆ ˆ (3.284) W (t ) = p · A(t ) + A2 (t ) 2 with A(t ) the vector potential. The transformation of the wave function |Ψ(t )〉 = e− 2

i t A2 (t −∞

) dt

ˆ e−iα(t )· p |ΨKH (t )〉

(3.285)

**removes the A2 -term and transforms to the system of an electron oscillating with an excursion
**

t

α(t ) =

−∞

A(t ) dt

(3.286)

72

CHAPTER 3. ATOMS IN EXTERNAL FIELDS

in the laser ﬁeld (Kramers-Henneberger transformation). In this system the nuclear potential appears to oscillate. The TDSE then reads i∂ t |ΨKH (t )〉 = ˆ p2 2 + V [r + α(t )] |ΨKH (t )〉. (3.287)

The Kramers-Henneberger Hamiltonian ˆ HKH (t ) = ˆ p2 2 + V [r + α(t )] (3.288)

is, for an inﬁnitely long laser pulse, periodic as well so that we may apply the Floquet theorem. Introducing the time-averaged Kramers-Henneberger potential VKH (ˆ, r ) = α 1 T

0 T

V [r + α(t )] dt ,

α = max |α(t )|, ˆ

(3.289)

**which is the zero-frequency contribution in a Fourier-expansion of the potential, Eq. (3.253) can be written as −(ε + mω)Φβ +
**

(m)

〈β|

α

ˆ p2 2

+ VKH (ˆ, r )|α〉Φ(m) + α α

αn n=m

〈β|V (m−n) |α〉Φ(n) = 0. (3.290) α

If the laser frequency is large compared to the relevant inner-atomic transitions, we may neglect the third term so that we are left with an equation diagonal in the photon index, which corresponds to the solution of the time-independent Schrödinger equation ε|ΨKH 〉 = ˆ p2 2 + VKH (ˆ, r ) |ΨKH 〉. α (3.291)

If it is possible to transfer the entire electron population to the bound states of VKH (ˆ, r ) α there will be no ionization whatsoever. For intense ﬁelds where α 1 Bohr radius the ˆ potential VKH (ˆ, r ) looks very different from the unperturbed nuclear potential since α it has a double-well structure with the minima close to the classical turning points ±ˆ. α If electronic probability density is trapped in this potential the ionization rate decreases despite increasing laser ﬁeld strength. This has indeed been observed in numerical simulations and is called adiabatic stabilization. The stabilization effect survives also for a “real” laser pulse with an up- and a down-ramp (dynamical stabilization). Figure 3.14 illustrates stabilization of a one-dimensional model atom employing a soft-core binding potential V (x) = −(x 2 + )−1/2 with = 1.9 (leading to a binding energy of −0.5). The full TDSE was solved. The laser pulse of frequency ω = 2.5 was ˆ ramped over 10 cycles up to E = 62.5 and thereafter held constant. The excursion of a free electron in this ﬁeld is α(t ) = 10 sin ωt . The cycle-averaged Kramers-Henneberger

3.5. ATOMS IN STRONG LASER FIELDS

73

(a) Energy (a.u.)

(b) Time (cycles)

x (a.u.)

**Figure 3.14: Adiabatic stabilization in a one-dimensional model atom. The cycle-averaged
**

ionic potential in a reference frame where a freely oscillating electron is at rest is depicted in (a) (solid line). The three lowest energy levels in this “dressed” potential and the corresponding probability densities are also plotted. In (b) a shadowgraph of the probability density, obtained from the full solution of the time-dependent Schrödinger equation, is shown. The probability density remains trapped in the effective potential. Low-frequency Rabi-ﬂoppings are responsible for the oscillatory pattern. Note that the time scale of these oscillations is small compared to the laser period.

74

CHAPTER 3. ATOMS IN EXTERNAL FIELDS

Figure 3.15: Lifetime of the H atom in the ground state according to the high-frequency Floquet theory, vs intensity, at various laser frequencies ω; circular polarization. Numbers adjacent ˆ to points on the curves are the corresponding values of α. The descending branches of the curves correspond to LOPT, the ascending ones to adiabatic stabilization (the latter can be “trusted” as the laser frequency increases beyond the ionization potential 0.5). [From M. PONT AND M. GAVRILA, Stabilization of atomic hydrogen in superintense, high-frequency laser ﬁelds of circular polarization, Phys. Rev. Lett. 65, 2362 (1990).]

potential, its three lowest levels and the corresponding probability densities are indicated in Fig. 3.14a. The potential has the above mentioned double-well shape with the minima close to the classical turning points ±ˆ. In Fig. 3.14b a shadowgraph of the α probability density obtained from the TDSE solution is shown. The probability density remains conﬁned within the two turning points. Only during the up-ramping of the pulse some density escapes. Obviously, not only a single dressed state is occupied since the probability density distribution oscillates in time. It can be shown that this oscillation is due to Rabi ﬂoppings between several of the dressed states. Note that the time-scale of this dynamics is slow compared to the laser period. Figure 3.15 shows the lifetime (i.e., the inverse ionization rate) of atomic H in circularly laser pulses of various frequencies and intensities as predicted by the highfrequency Floquet theory. With increasing laser intensity the lifetime ﬁrst decreases (i.e., ionization increases). This is the expected behavior from LOPT. Then, however, the lifetime passes through a minimum (the “death valley”) before it increases again (i.e., ionization is reduced). So far, adiabatic stabilization with the electron starting from the ground state was observed in numerical simulations only. This is because there are no sufﬁciently strong

3.5. ATOMS IN STRONG LASER FIELDS

75

lasers available yet at short wavelengths. The photon energy ω has to exceed the ionization potential, and the laser intensity must be strong enough in order to lead to the two minima in the time-averaged potential so that the probability density is kept far away from the nucleus (where absorption of laser energy is efﬁcient) most of the time. Since the elongation α is inversely proportional to ω 2 , the laser intensity necessary for adiabatic stabilization increases with ω. However, with the free electron lasers (FELs) under development, for example at DESY in Hamburg, the regime of adiabatic stabilization should become accessible experimentally. Stabilization of Rydberg atoms by the same mechanism was already demonstrated. There are (at least) three effects which counteract to adiabatic stabilization. Firstly, there is the so-called “death-valley” effect: an atom experiences during the rising edge of a strong laser pulse ﬁeld intensities in which violent ionization may occur and hence no more electrons are left to be stabilized once the optimal stabilization condition is reached. Secondly, inner electrons might be excited or removed by few photon processes induced by the incident high frequency radiation. Then the question arises whether an outer electron can stabilize although there are electron holes in the lower lying shells. Thirdly, at high frequencies and high intensities the dipole approximation breaks down, and the magnetic v × B-force pushes the electron into the propagation direction, thus enhancing ionization. These three effects will probably make the experimental veriﬁcation of stabilization of atoms initially in the ground state a formidable task. However, in case this kind of stabilization will be achieved, a new and interesting kind of matter is formed: pseudo atoms with charge clouds extending over tens or more atomic units.

Problem 3.7 How does Fig. 3.9 look for non-vanishing detuning? Further reading: A recent review of Floquet methods is given in SHIH-I CHU and DIMITRY A. TELNOV, Beyond the Floquet theorem: generalized Floquet formalisms and quasienergy methods for atomic and molecular multiphoton processes in intense laser ﬁelds, Phys. Rep. 390, 1 (2004). A Floquet-code can be downloaded from the Computer Physics Communications-archive: R.M. POTVLIEGE, STRFLO: a program for time-dependent calculations of multiphoton processes in one-electron atomic systems I. Quasienergy spectra and angular distributions, Comput. Phys. Comm. 114, 42 (1998). The original paper on what later became the Floquet theorem is G. FLOQUET, Sur les equations differentielles lineares à coefﬁcients periodique, Ann. Ecol. Norm. Sup. 12, 47 (1883). The fact that Floquet states can be interpreted as the quantum ﬁeld states of the electromagnetic ﬁeld was pointed out in J.H. SHIRLEY, Solution of the Schrödinger Equation with a Hamiltonian Periodic in Time, Phys. Rev. 138, B979 (1965).

76

**CHAPTER 3. ATOMS IN EXTERNAL FIELDS
**

A relatively recent review on stabilization (by one of the eminent persons in the ﬁeld) is MIHAI GAVRILA, Atomic stabilization in superintense laser ﬁelds, J. Phys. B: At. Mol. Opt. Phys. 35, R147 (2002). Dynamic stabilization of a two-electron model system has been studied in D. BAUER and F. CECCHERINI, Electron correlation vs stabilization: A two-electron model atom in an intense laser pulse, Phys. Rev. A 60, 2301 (1999). Two-color stabilization in circularly polarized laser ﬁelds was investigated in D. BAUER and F. CECCHERINI, Two-color stabilization of atomic hydrogen in circularly polarized laser pulses, Phys. Rev. A 66, 053411 (2002). Very recently, two-electron stabilization beyond the dipole approximation has been studied in ANDREAS STAUDT and CHRISTOPH H. KEITEL, Two-electron ionization and stabilization beyond the dipole approximation, Phys. Rev. A 73, 043412 (2006).

3.6

Strong ﬁeld approximation

The strong ﬁeld approximation (SFA) and its extensions are the theoretical workhorse in strong ﬁeld laser-atom and laser-molecule interaction. It is sometimes referred to as Keldysh-Faisal-Reiss (KFR) theory because of the papers of these authors (see “Further reading” below). As the laser ﬁeld is far from being a small perturbation, “conventional” perturbation theory is not applicable. The SFA does neither consider the laser ﬁeld being small compared to the binding forces nor does it assume the contrary at all times during the interaction. Instead, the SFA’s assumptions consist basically of considering the binding potential dominant until ionization whereas the laser ﬁeld takes over after ionization. The SFA has been applied to ionization, harmonic generation, and non-sequential ionization. The beauty of the SFA lies, besides in its predictive power, in the possibility to interpret its equations in intuitively accessible terms, as will be seen below. However, there are “problems” and limits as well, to be discussed in the last part of this Section. Let us start with an electronic eigenstate of the ﬁeld-free Hamiltonian. The electron may at time ti be in the ground state |Ψ0 (ti )〉 with energy 0 < 0, for instance, and the laser ﬁeld is not yet switched on. Now let us consider the matrix element ˆ M p (tf , ti ) = 〈Ψ p (tf )|U (tf , ti )|Ψ0 (ti )〉, (3.292)

which governs the probability wi→f = |M p (tf , ti )|2 to ﬁnd the electron at time tf in the scattering state |Ψ p (tf )〉 where p is the asymptotic momentum far away from the atom (where the measurement is performed). We assume that at time tf the laser ﬁeld is off ˆ ˆ again. U (t , t ) = U † (t , t ) is the time-evolution operator associated with the TDSE i ∂ ∂t ˆ |Ψ(t )〉 = H (t )|Ψ(t )〉, ˆ H (t ) = 1 2 ˆ [ ˆ + A(t )]2 + V (r ) p (3.293)

3.6. STRONG FIELD APPROXIMATION

77

where A(t ) is the vector potential describing the laser ﬁeld (in dipole approximation). ˆ The minimum coupling Hamiltonian H (t ) can be splitted in various ways: i with ˆ H0 = ∂ ∂t ˆ ˆ ˆ ˆ |Ψ(t )〉 = [H0 + W (t )]|Ψ(t )〉 = [H (V) (t ) + V (r )]|Ψ(t )〉, ˆ p2 2 ˆ p2 2 (3.294)

ˆ + V (r ),

ˆ H (V) (t ) =

ˆ + W (t ),

(3.295)

ˆ and W (t ) the interaction with the laser ﬁeld, 1 ˆ ˆ W (t ) = p · A(t ) + A2 (t ) 2 (velocity gauge). (3.296)

The gauge transformation of the potentials (both scalar potential φ and vector potential A) and the wave function |Ψ(t )〉 A = A + ∇χ (r , t ), φ =φ− ∂ χ (r , t ) ∂t , |Ψ (t )〉 = e−iχ (r ,t ) |Ψ(t )〉 (3.297)

where χ (r , t ) is an arbitrary differential scalar function, leaves the electric and the magnetic ﬁeld unchanged: E = −∂ t A − ∇φ = E , B = ∇×A= B . (3.298)

This gauge invariance offers the possibility to choose a gauge that suits us best, e.g., as far as computational simplicity is concerned. However, this statement only holds true as long as all approximations we make do not destroy the gauge invariance. Unfortunately, the standard SFA does break the gauge invariance. Transformation to the so-called length gauge is achieved by choosing χ (r , t ) = −A(t ) · r . (3.299)

Because of ∇χ = −A the vector potential is “transformed away” while φ = −∂ t χ = −E · r . The Hamiltonian in length gauge reads ˆ H (t ) = ˆ2 p 2 ˆ + V (r ) − φ (r , t ) = ˆ2 p 2 ˆ + V (r ) + E (t ) · ˆ r (3.300)

ˆ (one could also absorb V (r ) in φ and φ ). Note that the transformation of the wave function r |Ψ (t )〉 = eiˆ·A(t ) |Ψ(t )〉 (3.301) can be interpreted as a translation in momentum space. In fact, while in velocity gauge the quiver momentum is effectively subtracted from the kinetic momentum, leading to

78

CHAPTER 3. ATOMS IN EXTERNAL FIELDS

a canonical momentum different from the kinetic momentum, in length gauge kinetic and canonical momentum are equal. From (3.300) we can infer ˆ W (t ) = E (t ) · ˆ r (length gauge) (3.302)

with E (t ) = −∂ t A(t ). ˆ H0 describes the unperturbed atom and seemingly does not depend on the gauge ˆ ˆ ˆ ˆ chosen, i.e., H0 = H0 . However, one should bear in mind that the momentum p in H0 ˆ is not the kinetic momentum (which, in atomic units, equals the velocity) while in H0 (length gauge) it is. ˆ The Volkov-Hamiltonian H (V) (t ) governs the free motion of the electron in the laser ﬁeld. It fulﬁlls in velocity gauge i 1 ˆ ˆ |Ψ(V) (t )〉 = H (V) (t )|Ψ(V) (t )〉 = [ p + A(t )]2 |Ψ(V) (t )〉. ∂t 2 ∂ (3.303)

Thanks to the dipole approximation the Volkov-Hamiltonian is diagonal in momentum space. The solution of (3.303) is thus readily written down: |Ψ (t )〉 = e

(V) −iS p (t ,ti )

|p〉,

S p (t , ti ) =

1 2

t

dt [p + A(t )]2

ti

(3.304)

where |p〉 are momentum eigenstates, 〈r |p〉 = eip·r /(2π)3/2 . Note that the lower integration limit ti affects the overall phase of the Volkov solution only. As mentioned above, the transition to the length gauge corresponds to a translation in momentum space. It is thus easy to check that in length gauge one has |Ψ(V) (t )〉 = e−iS p (t ,ti ) |p + A(t )〉 (length gauge) (3.305)

with the same action S p (t , ti ) as in (3.304). Let us now continue to derive the SFA transition matrix element. The time evoluˆ tion operator U (t , t ) satisﬁes the TDSE (3.294), ˆ ˆ ˆ ˆ i∂ t U (t , t ) = [H0 + W (t )]U (t , t ). Its formal solution is given by the integral equations [cf. (3.87) and (3.88)] ˆ ˆ U (t , t ) = U0 (t , t ) − i

t t

(3.306)

ˆ ˆ ˆ dt U (t , t )W (t )U0 (t , t ), ˆ ˆ ˆ dt U0 (t , t )W (t )U (t , t ),

(3.307)

ˆ = U0 (t , t ) − i

t

t

3.6. STRONG FIELD APPROXIMATION

79

ˆ ˆ where U0 (t , t ) is the evolution operator corresponding to the TDSE with H0 only. Inserting (3.307) in the matrix element (3.292) leads to

tf

M p (tf , ti ) = −i

ti

ˆ ˆ dt 〈Ψ p (tf )|U (tf , t )W (t )|Ψ0 (t )〉

(3.308)

ˆ where use of 〈Ψ p (tf )|U0 (tf , ti )|Ψ0 (ti )〉 = 〈Ψ p (tf )|Ψ0 (tf )〉 = 0 was made because |Ψ p (tf )〉 ˆ is a scattering state perpendicular to |Ψ0 (tf )〉, and U0 (t , ti )|Ψ0 (ti )〉 = |Ψ0 (t )〉. Since the ˆ propagator U (t , t ) also satisﬁes the integral equations ˆ ˆ U (t , t ) = U (V) (t , t ) − i

t t

ˆ ˆ ˆ dt U (V) (t , t )V U (t , t ), ˆ ˆ ˆ dt U (t , t )V U (V) (t , t ),

(3.309)

ˆ = U (V) (t , t ) − i

t

t

ˆ where U (V) (t , t ) is the evolution operator corresponding to the TDSE (3.303), one obtains, upon inserting (3.309) in (3.308),

tf

M p (tf , ti ) = −i

ti

ˆ ˆ dt 〈Ψ p (tf )|U (V) (tf , t )W (t )|Ψ0 (t )〉

tf tf

(3.310)

−i

ti

dt

t tf ti tf tf ti

ˆ ˆ ˆ ˆ dt 〈Ψ p (tf )|U (V) (tf , t )V U (t , t )W (t )|Ψ0 (t )〉 .

tf ti

Using t f dt t f dt = i be recast in the form

t

t

dt

dt Θ(t − t ) =

dt

t ti

dt expression (3.310) may

M p (tf , ti ) = −i

ti

ˆ ˆ dt 〈Ψ p (tf )|U (V) (tf , t ) W (t )|Ψ0 (t )〉

t

(3.311)

−i

ti

ˆ ˆ ˆ dt V U (t , t )W (t )|Ψ0 (t )〉 .

Eq. (3.311) is still exact and gauge invariant. Whatever is missed in the ﬁrst term of (3.311) is included in the second term where the full but unknown time evolution operˆ ator U (t , t ) appears. Neglecting the second term and replacing the ﬁnal state |Ψ p (tf )〉 with a plane wave |p〉 yields the SFA or so-called Keldysh-amplitude

(SFA) M p (tf , ti ) = −i tf ti

ˆ dt 〈Ψ(V) (t )|W (t )|Ψ0 (t )〉 p

(3.312)

ˆ where in velocity gauge the Volkov wave |Ψ(V) (t )〉 = U (V) (t , ti )|p〉 is given by (3.304) and in length gauge by (3.305). The SFA transition amplitude integrates over all ionization

80

**CHAPTER 3. ATOMS IN EXTERNAL FIELDS
**

(V)

times t where the transition from the bound state |Ψ0 (t )〉 to the Volkov state |Ψ p (t )〉, ˆ mediated by the interaction with the laser ﬁeld W (t ), may take place. It is thus a bit surprising, at least at ﬁrst sight, that the Keldysh amplitude can be recast in a form ˆ ˆ where W (t ) is replaced by V (r ):

(SFA) M p (tf , ti ) tf

= −i

ti tf

ˆ ˆ ˆ dt 〈Ψ(V) (t )| H (V) (t ) − H0 + V |Ψ0 (t )〉 p

ˆ W (t )

= −i

ti tf

ˆ dt 〈Ψ(V) (t )| − i ∂ t +V − i ∂ t |Ψ0 (t )〉 p

←

→

= −

ti

ˆ dt ∂ t 〈Ψ(V) (t )|Ψ0 (t )〉 + i〈Ψ(V) (t )|V |Ψ0 (t )〉 p p

tf ti tf ti

= − 〈Ψ(V) (t )|Ψ0 (t )〉 − i p

ˆ dt 〈Ψ(V) (t )|V |Ψ0 (t )〉. p

(3.313)

Since the laser is off at the times ti and tf , the ﬁrst term is just the difference of the Fourier-transformed initial state at the two times ti and tf . The latter can be always chosen such that the term vanishes. The fact that the boundary term shows up at all is due to the non-orthogonality of plane waves (introduced within the SFA) and the initial bound state. However, the contribution of the ﬁrst term vanishes at latest when the asymptotic rate is calculated. Hence, the SFA-amplitude (3.312) may be also written as

(SFA) M p (tf , ti ) = −i tf ti

ˆ dt 〈Ψ(V) (t )|V (r )|Ψ0 (t )〉. p

(3.314)

Following the above interpretation it now seems that ionization is mediated by the ˆ binding potential V (r ), which appears to be absurd. However, upon time-reversal ionization turns into (re)combination, for which indeed the nuclear potential is responsiˆ ˆ ble. Moreover, in the above derivation of (3.312) W and V are treated on an equal, symmetrical footing since the essential steps consisted of using the integral equations (3.307) and (3.309). ˆ ˆ In velocity gauge where W (t ) = p · A(t ) + A2 (t )/2 one can write (3.312) as

(SFA) M p (tf , ti ) = −Ψ0 (p) eiS p, 0 (t ,ti ) + iΨ0 (p) ti tf

p2 2

tf

−

0 ti

dt eiS p, 0 (t ,ti ) (3.315)

**with the classical action
**

t

S p, 0 (t , ti ) =

ti

dt

p2 2

−

0

ˆ + W (t ) ,

(3.316)

**3.6. STRONG FIELD APPROXIMATION
**

Ψ0 (p, t ) = 〈p|Ψ0 (t )〉, and Ψ0 (p, t ) = exp(−i transformed initial state wave function Ψ0 (p) = and

0 0 t )Ψ0 (p),

81 that is, Ψ0 (p) is the Fourier-

1 (2π)

3/2

d3 r e−ip·r Ψ0 (r )

(3.317)

**is the initial energy. The ﬁrst term in (3.315) vanishes when the asymptotic rate Mp T
**

2

Γ p = lim is calculated:

T →∞

,

M p = tlim M p (tf , ti ) →−∞

i tf →∞

(3.318)

(SFA) Mp = iΨ0 (p)

p2 2

∞

−

0 −∞

dt eiS p, 0 (t ,−∞) .

(3.319)

**3.6.1 Circular polarization and long pulses
**

In this case one may write the vector potential in dipole approximation as 1 ˆ A(t ) = A[ exp(iωt ) + 2

∗

exp(−iωt )]

(3.320)

where the polarization vectors , ∗ fulﬁll 2 = ∗2 = 0 and · ∗ = 1, e.g., = (e x + ˆ iey )/ 2. The factor 1/2 is introduced in order to obtain Up = A2 /4, as in the linearly polarized case. With 1 ˆ ˆ [p + A(t )]2 = p 2 + A2 + 2A|p · | cos(ωt − ϕ), 2 where p · = |p · | exp(−iϕ), the action (3.316) reads S p, 0 (t , −∞) = p2 2 − + Up t + ˆ A ω |p · | sin(ωt − ϕ) (3.322) (3.321)

0

where we neglected contributions from ti = −∞ since they just affect the irrelevant, overall phase of the transition matrix element. The SFA transition matrix element then is M p, circ. = 2πiΨ0 (p)

(SFA) ∞

(nω − Up ) exp(inϕ) Jn

n=−∞

ˆ −A|p · | ω

δ( p 2 /2 −

0

+ Up − nω), (3.323)

82

CHAPTER 3. ATOMS IN EXTERNAL FIELDS

**where use of the Bessel functions Jn (ζ ), obeying
**

∞

**exp[−iζ sin(ωt − ϕ)] =
**

n=−∞

Jn (ζ ) exp[−in(ωt − ϕ)],

(3.324)

was made. The time integration in (3.319) leads to the energy-conserving δ-function. Employing (3.318) one obtains the ionization rate

(SFA) Γ p, circ. (SFA) ∞

= 2π|Ψ0 (p)|

2 n=−∞

2 (nω − Up )2 Jn

ˆ −A|p · | ω

δ( p 2 /2 −

0 + Up − nω).

(3.325)

Γ p, circ. has the dimension of a density in momentum space per time. To evaluate the square of the δ-function we used the “working formula” δ(Ω) = 1

T /2

2π T →∞

lim

**exp(iΩt ) dt = lim
**

−T /2

T 2π

T →∞

for Ω = 0

(3.326)

(and zero otherwise). For obtaining the total rate Γ the partial rate Γ p has to be integrated over all ﬁnal momenta p, Γ= d3 p Γ p = d p dΩ p 2 Γ p = dΩ dΓ dΩ (3.327)

where dΩ = sin ϑ dϑ dϕ is the solid angle element. The ﬁnal rate for ionization with the electron ejected into the solid angle dΩ is given by dΓcirc. dΩ with pn = 2(nω − Up +

0 ). (SFA) ∞

= 2π

8ω 5

n=nmin

(n − Up /ω)2

pn 2ω

2 |Ψ0 ( pn )|2 Jn

ˆ −Apn sin ϑ 2ω

,

(3.328)

(3.329)

The sum in (3.328) runs over all n which yield real pn , starting with the minimum number of absorbed photons nmin .

3.6.2

Channel closing in above-threshold ionization

The increase of nmin with increasing Up is the channel-closing phenomenon. This is illustrated in Fig. 3.16. We expect peaks in the photoelectron spectra at the positions

n =

1 2

2 pn = nω − (Up + | 0 |),

n ≥ nmin

(3.330)

where | 0 | is the ionization potential and Up + | 0 | is the “effective” ionization potential due to the AC Stark shift of the continuum threshold with respect to the ground state

small so that the Up -shift of the continuum threshold is less than a photon energy. In (b) the channels n = 5 and n = 6 are closed due to the pronounced AC Stark shift of the continuum. The photoelectron spectra look different in the short (blue) and long pulse regime (red) since the released electron gains Up in the latter case upon leaving the laser focus.

**Figure 3.16: Channel closing in the short and long pulse regime. In (a) the laser intensity is
**

¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡

3.6. STRONG FIELD APPROXIMATION

(a)

short pulse

long pulse

(b)

short pulse

Up

long pulse

ε0

¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡ ¡

83

84

CHAPTER 3. ATOMS IN EXTERNAL FIELDS

level. Due to the fact that peaks n > nmin are present—even with higher probability than n = nmin —the name above-threshold ionization has been coined for this strong ﬁeld ionization phenomenon. In actual measurements the positions of the peaks depend on the laser pulse duration. In short-pulse experiments the released electron has no time to leave the focus before the laser pulse is over. In long pulses, instead, the electron has time to leave the focus and, by doing so, gains the energy Up . As a consequence the Up -term in (3.330) is cancelled and the peak positions in the long-pulse regime are determined by

(long pulse) n

=

1 2

2 pn = nω − | 0 |,

n ≥ nmin

(3.331)

with nmin , however, still to be calculated with Up (since before leaving the laser focus, ionization has to occur in the ﬁrst place). In Fig. 3.16a the Up -shift of the continuum threshold is small, and the channel n = 5 is responsible for the ﬁrst peak in the photoelectron spectra. At higher laser intensity, in Fig. 3.16b, the channels n = 5 and n = 6 are closed since 6 photons are not sufﬁcient to overcome the effective ionization potential | 0 | + Up . In the long pulse regime peaks corresponding to a certain channel are always at the same positions in the energy spectra whereas in the short pulse regime the peaks move with Up . As a consequence, focal averaging reduces the contrast in the short pulse regime whereas it has less of an effect in the long pulse regime. In Fig. 3.17 we show the example of an experimental long-pulse spectrum where lower order peaks are indeed suppressed due to channel closing.

3.6.3

**Linear polarization and long pulses
**

ˆ A(t ) = A cos(ωt ),

2

We assume a laser ﬁeld of the form = 1. (3.332)

The action (3.316) reads in this case S p, 0 (t , −∞) = p2 2 − + Up t − ˆ A ω p · sin(ωt ) + ˆ A2 8ω sin(2ωt ). (3.333)

0

**Proceeding as in the circular ﬁeld-case one arrives at M p,lin. = 2πiΨ0 (p)
**

(SFA) ∞ n=−∞ ∞ n=−∞

˜ (nω−Up )Jn

ˆ −Ap · ω

,−

Up 2ω ,−

δ( p 2 /2− Up 2ω

0 +Up −nω),

(3.334)

Γ p,lin. = 2π|Ψ0 (p)|2

(SFA)

˜2 (nω − Up )2 Jn

ˆ −Ap · ω

δ( p 2 /2 −

0

+ Up − nω), (3.335)

3.6. STRONG FIELD APPROXIMATION

85

Up

Figure 3.17: Channel closing in the long-pulse regime. The experimental spectrum was taken

from R.R. FREEMAN & P.H. BUCKSBAUM, Investigation of above-threshold ionization using subpicosecond laser pulses, J. Phys. B: At. Mol. Opt. Phys. 24, 325 (1991).

86 dΓlin. dΩ

(SFA) ∞

**CHAPTER 3. ATOMS IN EXTERNAL FIELDS
**

= 2π 8ω 5

n=−∞

(n − Up /ω)2

pn 2mω

˜2 |Ψ0 ( pn )|2 Jn

ˆ −Ap · ω

,−

Up 2ω

. (3.336)

**˜ Jn is the generalized Bessel function of integer order deﬁned by ˜ Jn (u, v) = 1 2π
**

π

**dθ exp[i(u sin θ + v sin(2θ) − nθ)].
**

−π

(3.337)

**The relation to the ordinary Bessel functions is ˜ Jn (u, v) =
**

∞

Jn−2k (u)Jk (v).

k=−∞

(3.338)

**The equation used in the derivation of (3.334) is
**

∞ n=−∞

˜ exp(inθ)Jn (u, v) = exp[iu sin θ + iv sin(2θ)].

(3.339)

Further properties of the generalized Bessel functions may be found in the Appendix B of the original SFA paper by REISS. In the same article it is also demonstrated how the typical exponential behavior ∼ exp[−2(2| 0 |)3/2 /(3|E|)] arises in the case of tunneling ˜ ionization through the asymptotic behavior of the generalized Bessel functions Jn .

Problem 3.8 Which channels n are closed in Fig. 3.17? Further reading: The KFR papers are: L.V. KELDYSH, Zh. Eksp. Teor. Fiz. 47, 1945 (1964); [Sov. Phys. JETP 20, 1307 (1965)]; F.H.M. FAISAL, J. Phys. B: Atom. Molec. Phys. 6, L89 (1973); H.R. REISS, Phys. Rev. A 22, 1786 (1980).

**3.6.4 Few-cycle above-threshold ionization
**

ˆ In few-cycle pulses the pulse envelope A(t ) varies on a time scale not much slower than the period T = 2π/ω corresponding to the carrier frequency ω. Moreover, the carrier envelope phase φ, governing the shift of the carrier wave with respect to the envelope, affects basically all observables. Hence, instead of (3.332) we write ˆ A(t ) = A(t ) sin(ωt + φ) ˆ with A(t ) a sin2 or a Gaussian envelope, for instance. (3.340)

3.6. STRONG FIELD APPROXIMATION

87

In the case of few-cycle pulses it would be very cumbersome to deal with Bessel ˆ functions, as we did above for constant (or slowly varying) A. Instead, we start off with the still exact matrix element (3.311) and replace once again the ﬁnal state by a plane ˆ ˆ wave and the full propagator U (t , t ) by U (V) (t , t ). In that way we obtain the extended SFA transition matrix element

(SFA) (SFA,dir) (SFA,resc) M p (tf , ti ) = M p (tf , ti ) + M p (tf , ti ),

(3.341)

(SFA,dir) Mp (tf , ti ) (SFA,resc) Mp (tf , ti )

=

(SFA) M p (tf , ti ) = tf t

tf

−i

ti

ˆ dt 〈Ψ(V) (t )|W (t )|Ψ0 (t )〉, p

(3.342)

= −

ti

dt

ti

ˆ ˆ ˆ dt 〈Ψ(V) (t )|V U (V) (t , t )W (t )|Ψ0 (t )〉. (3.343) p

In what follows we set ti = 0, and we assume that A(0) = A(Tp ) = 0 (3.344)

where Tp is the laser pulse duration. Relabelling the integration variables and making use of the fact that ionization can only happen while the laser is on, (3.342) and (3.343) can be recast in the form

(SFA,dir) Mp = −i (SFA,resc) Mp = − Tp 0 Tp 0

**ˆ dtion 〈Ψ(V) (tion )|W (tion )|Ψ0 (tion )〉, p
**

∞ tion

(3.345)

dtion

ˆ ˆ ˆ dtresc 〈Ψ(V) (tresc )|V U (V) (tresc , tion )W (tion )|Ψ0 (tion )〉. (3.346) p

The interpretation of the second term is straightforward: ionization due to interaction ˆ with the laser (W ) occurs at time tion and is restricted to times where the laser is on. ˆ After ionization, the electron moves freely in the laser ﬁeld (governed by U (V) ) before ˆ ). Note that t may be > T . After the it rescatters at time tresc with the ionic core (V resc p rescattering event, the electron ends up in the Volkov state |Ψ p 〉, meaning that it will ﬁnally arrive with a (ﬁeld free and thus kinetic) momentum p at the detector. In length gauge the matrix elements read

(SFA,dir) Mp (SFA,resc) Mp Tp (V)

= −i

0 Tp

**dtion 〈p + A(tion )|r · E (tion )|Ψ0 〉 eiS p, 0 (tion ) ,
**

∞

(3.347)

= −

0

dtion ×e

dtresc

tion

ˆ d3 k eiS p (tresc ) 〈p + A(tresc )|V |k + A(tresc )〉 (3.348)

−iSk (tresc )

〈k + A(tion )|r · E (tion )|Ψ0 〉eiSk, 0 (tion )

88 where

t

CHAPTER 3. ATOMS IN EXTERNAL FIELDS

S p, 0 (t ) =

0

dt

1 2

[p + A(t )]2 −

0

,

S p (t ) =

1 2

0

t

dt [p + A(t )]2 .

(3.349)

Introducing the new variables t = tresc , τ = tresc − tion (3.350)

**the rescattering SFA matrix element (3.348) can be written as
**

∞ (SFA,resc) Mp = − t ˆ V p−k =〈p|V |k〉

dt

0 ∞ 0

dτ

ˆ d3 k eiS p (t ) 〈p + A(t )|V |k + A(t )〉

t

(3.351)

×e−iSk (t ) 〈k + A(t − τ)|r · E (t − τ)|Ψ0 〉 = −

0

dt eiS p, 0 (t )

0

dτ

d3 k V p−k e−iSk, 0 (t ,t −τ) ×〈k + A(t − τ)|r · E (t − τ)|Ψ0 〉

(3.352)

where Sk, 0 (t , t − τ) =

t

dt

t −τ

1 2

k + A(t )

2

−

0

.

(3.353)

The time τ is the time the electron spends in the continuum between ionization and rescattering. The inﬁnite upper limit in the integration over the rescattering time in (3.348) can be restricted to Tp since rescattering after the laser is off will not lead to energy absorption. As a consequence, the ﬁnal energy will be within a region strongly dominated by the more probable direct ionization process. The integration over the intermediate momentum k can be performed using the saddle-point approximation (stationary phase method) where we seek the stationary momentum ks (t , τ) contributing most to the k-integration: ∇k Sk, 0 (t , t − τ) = 0

!

⇒

ks (t , τ) = −

α(t ) − α(t − τ) τ

(3.354)

with α(t ) the excursion as in (3.286). Hence,

(SFA,resc) Mp = −

Tp 0

iτ ×〈ks (t , τ) + A(t − τ)|r · E (t − τ)|Ψ0 〉

0

dt eiS p, 0 (t )

t

dτ

2π

3/2

V p−ks (t ,τ) e−iSs, 0 (t ,t −τ)

(3.355)

**3.6. STRONG FIELD APPROXIMATION
**

where the stationary action Ss, 0 (t , t − τ) is given by Ss, 0 (t , t − τ) = Sks (t ,τ), 0 (t , t − τ)

89

(3.356)

and the factor [2π/(iτ)]3/2 comes from the saddle-point integration. In actual numerical evaluations the denominator iτ can be either regularized by adding a real, positive ε, or the lower integration limit 0 for τ can be replaced by ε. As long as ε is sufﬁciently small, the results are independent of ε. In the case of a hydrogen-like atom the matrix element needed in (3.355) reads 〈k|r · E (t )|Ψ0 〉 = −i27/2 (2| 0 |)5/4 For rescattering at potentials of the form V (r ) = − b + the matrix element V p−k is given by V p−k = − 2b λ + aC 2π C

2 2

k · E (t ) π(k 2 + 2| 0 |)3

.

(3.357)

a r

e−λr

(3.358)

,

C = (p − k)2 + λ2 .

(3.359)

In few-cycle laser pulses the concept of an ionization rate is not useful since the latter would be time-dependent and sensitive to all details of the pulse (duration, shape, carrier-envelope phase, peak ﬁeld strength). In experiments one measures the differential ionization probability w p , which is the probability to ﬁnd an electron of ﬁnal energy p = p 2 /2 emitted in a certain direction, given by the solid angle element dΩ p that is covered by the measuring device. The probability w p is related to the transition matrix element M p through wp d so that w p = p |M p |2 . (3.361)

p

dΩ p = |M p |2 d3 p = |M p |2 p 2 d p dΩ p

(3.360)

p dp

**3.6.5 “Simple man’s theory”
**

The remaining time integral(s) in (3.347) and (3.355) can be either solved numerically or approximately by using modiﬁcations of the saddle-point method with respect to time. We do not want to go into the details but only emphasize here that the SFA transition matrix element can be approximated by a sum over the stationary contributions,

(SFA) Mp =

a s ,p eiSs,p .

s

(3.362)

90

CHAPTER 3. ATOMS IN EXTERNAL FIELDS

As it turns out the saddle-point equations deﬁne quantum orbits that are close to the classical orbits of the so-called simple man’s theory. In the following we will use simple man’s theory to derive the cut-off laws for the photoelectron spectra. If an electron is set free at time tion and from thereon does not interact with the ionic potential anymore, its momentum and position at times t > tion are given by

t

p(t ) = −

tion t

dt E (t ) = A(t ) − A(tion ), dt A(t ) − A(tion )(t − tion )

(3.363)

r (t ) =

tion

= α(t ) − α(tion ) − A(tion )(t − tion ).

(3.364)

If the vector potential fulﬁlls (3.344) the momentum at the end of the pulse is determined by the value of the vector potential at the time of ionization, p(Tp ) = −A(tion ), so that the ﬁnal energy is

dir,p (tion ) =

1 2

A2 (tion ) ≤ 2Up

(3.365)

ˆ because the ponderomotive potential is Up = A2 /4. The fact that the direct electrons are classically restricted to energies up to 2Up is one of the celebrated cut-off laws in strong ﬁeld physics. Let us now allow for one rescattering event, i.e., at the time tresc the electron returns to the origin (where the ion is located), ε > |r (tresc )| = |α(tresc ) − α(tion ) − A(tion )τ|

!

(3.366)

where ε is a distance small compared to the Bohr radius. Let us assume the extreme case of 180◦ back-reﬂection where the electron changes the sign of its momentum so that immediately after the scattering event p(tresc + ) = −[A(tresc ) − A(tion )]. At later times we have

t

(3.367)

p(t > tresc ) = −

tresc

dt E (t ) − [A(tresc ) − A(tion )] (3.368)

**= A(t ) − 2A(tresc ) + A(tion ) so that presc (Tp ) = −2A(tresc ) + A(tion ) and
**

resc,p (tresc , tion ) =

1 2

[A(tion ) − 2A(tresc )]2 ≤ 10Up .

(3.369)

3.6. STRONG FIELD APPROXIMATION

91

final energy contours / Up

"direct" electrons rescattered electrons

Figure 3.18: Final photoelectron energy

vs ionization time tion and rescattering time tresc > tion (black: high value of resc,p , white: small value of resc,p , contours 2, 10 and 16Up labelled explicitly). The red branch labelled “rescattered electrons” indicate times tion and tresc where (3.366) is fulﬁlled. The highest energy those rescattered electrons can have is 10Up (see red branch touching the 10Up -contour). The inlet shows the ﬁnal energy (3.365) of the “direct” electrons vs the ionization time. The highest energy there is 2Up .

resc,p

Because of the condition (3.366) the 10Up cut-off law for the rescattered electrons is not so obvious. However, it can be readily checked numerically by plotting resc,p (tresc , tion ) vs all possible tresc , tion (where tresc > tion ) and then indicating those pairs of tion , tresc that fulﬁll (3.366). This is shown in Fig. 3.18. How good is the strong ﬁeld approximation? In order to answer this question we compare the results of an ab initio TDSE solution with the corresponding SFA predictions. Apart from the dipole approximation (which is well applicable for the peak intensities used) the TDSE result is exact. Comparisons with TDSE results serve as a much more demanding testing ground for approximate theories such as the SFA than comparison with experiments, mainly because of focal averaging effects present in experiments, the uncertainties in laser intensity, pulse dura-

92

2 Up

**CHAPTER 3. ATOMS IN EXTERNAL FIELDS
**

2 Up

(a) φ=0 θ=π (b) φ=0 θ=0

Yield (arb.u.)

10 Up

10 Up

Photoelectron energy (a.u.)

ˆ pulse (ω = 0.056, φ = 0, E = 0.0834). The TDSE and SFA results are drawn solid and dashed, respectively. Panel (a) shows the “left-going” electrons (i.e., opposite to the laser polarization e z ), panel (b) the “right-going” electrons (in e z )-direction. The spectra were adjusted vertically by multiplication with a single factor in such a way that agreement is best in the cut-off region for the right-going electrons. The spectra were not shifted in energy.

Figure 3.19: Photoelectron spectra of the H(1s) electron after irradiation with a 4-cycle laser

tion, and shape, the limited resolution in energy, and the limited dynamic range in the yields. In Fig. 3.19 the results for a n = 4-cycle pulse of the form E (t ) = ˆ sin2 [ωt /(2n)] cos(ωt + φ) for 0 < t < n2π/ω, ω = 0.056, E = 0.0834, φ = 0 ˆ Ee z are shown. The agreement between TDSE and SFA results improve with increasing photoelectron energy. A possible explanation for that might be that slow electrons spend more time in the vicinity of the atomic potential where Coulomb corrections are expected to be important. As can be seen in Fig. 3.19, the transition regime between the cut-off for the direct electrons at = 2Up = 1.1 up to energies where rescattered electrons start to take over at ≈ 2.5 is quite smooth in the TDSE spectra whereas pronounced patterns are visible in the SFA results. Moreover, at very low energies the positions of the local maxima disagree. It has been shown (see “Further reading” below) that the agreement at lower energies improves if the binding potential is made shortrange by cutting it at certain distances. This is expected since the crucial assumption in SFA is that the electron is not affected by the ionic potential anymore once ionization has occurred. This assumption is well justiﬁed for short-range potentials but less so for long range Coulombic ones as in the H(1s) case. However, the pronounced pat-

**3.6. STRONG FIELD APPROXIMATION
**

same final energy

93

(a) rescattered electrons

"direct" electrons

(b)

Figure 3.20: (a) Final energy of direct electrons (black line) vs the ionization time tion . If

rescattered is allowed, higher energies may occur. The color coding for the rescattered electrons indicates the time spent in the continuum between ionization and rescattering, i.e., tresc − tion (the lighter the color the longer the time). The cut-off energies for the direct and the rescattered electrons are 2 and 10Up , respectively. Panel (b) shows the course of the laser ﬁeld. Ionization is improbable for small |E(t )|.

tern showing a spiky, downward-pointing structure in the rescattering plateaux between energies ≈ 3 and 6 a.u. is remarkably well reproduced using the SFA. Interference effects The spiky structure in Fig. 3.19 is due to quantum interference. For a ﬁxed ﬁnal momentum p the sum (3.362) is a sum over all quantum orbits that end up with the same momentum at the detector. It turns out that, most of the time, there are two dominating contributions. Depending on their phase-difference those may interfere constructively (local maxima in Fig. 3.19) or destructively (downward-pointing spikes in Fig. 3.19). The corresponding two trajectories of simple man’s theory can be readily calculated. As an example we show the ﬁnal energy vs the ionization time for a “ﬂat-top” pulse in Fig. 3.20. In the lower panel of Fig. 3.20 the course of the electric ﬁeld is indicated. Let us focus on the time t = 0.5 cycles where the electric ﬁeld has a maximum and ionization is therefore most likely. The upper panel shows that a “direct” electron emitted at that time will have vanishing ﬁnal energy. In order for a direct, classical electron to have the maximum energy 2Up it has to be emitted at times where the electric ﬁeld is zero (which is unlikely in the tunneling and over-barrier regime). However, if an electron is

94

CHAPTER 3. ATOMS IN EXTERNAL FIELDS

emitted around the maximum of the electric ﬁeld and rescatters once, its ﬁnal energy may be close to 10Up . It is clearly seen that two emission times very close to each other lead to the same ﬁnal energy (as indicated in the upper panel). These are the two trajectories that interfere. Exactly at the cut-off 10Up those two solutions merge to a single one. The “travel times” tresc − tion between rescattering and ionization are color-coded from black (tresc − tion = 0) to yellow (tresc − tion = 2 cycles). In very short pulses the situation is more complex than in the regular, ﬂat-top pulse case. Since the ionization probability is strongly weighted with the modulus of the electric ﬁeld, only a few “time-windows” may remain “open”, thus affecting the number of interfering quantum orbits for a given p. The interference pattern is then very sensitive to the details of the few-cycle pulse, e.g., to the carrier-envelope phase. Because of the “time-windows” that are opened and closed depending on the parameters of the fewcycle pulse, one may view the setup as a “double slit experiment in time” (see “Further reading” below).

Problem 3.9 Write down the SFA amplitude for the direct electrons emitted during a few-cycle pulse using velocity gauge. What is the difference with respect to (3.347)? Further reading: A review of few-cycle above-threshold ionization including many of ´ the relevant references is D.B. MILOŠEVI C, G.G. PAULUS, D. BAUER, and W. BECKER, Above-threshold ionization by few-cycle laser pulses, J. Phys. B: At. Mol. Opt. Phys. 39 (in press). The gauge problem in SFA has quite some history. Recent work on the subject, showing that in the case of atoms the velocity gauge may ´ lead to (even qualitatively) wrong results, is D. BAUER, D.B. MILOŠEVI C, and W. BECKER, Strong-ﬁeld approximation for intense laser-atom processes: the choice of gauge, Phys. Rev. A 72, 023415 (2005). A comparison of SFA with TDSE results focussing on the effect of the range of the binding potential has been undertaken ´ in D. BAUER, D.B. MILOŠEVI C, and W. BECKER, On the validity of the strong ﬁeld approximation and simple man’s theory, J. Mod. Opt. 53, 135 (2006). The emergence of the simple man’s theory-orbits in ab initio TDSE results has been demonstrated in D. BAUER, Emergence of Classical Orbits in Few-Cycle AboveThreshold Ionization of Atomic Hydrogen, Phys. Rev. Lett. 94, 113001 (2005). The above-mentioned “double slit in time”-experiment has been published in F. LINDNER , M.G. S CHÄTZEL , H. WALTHER , A. BALTUŠKA , E. G OULIELMAKIS , F. ´ KRAUSZ, D.B. MILOŠEVI C, D. BAUER, W. BECKER, and G.G. PAULUS, Attosecond Double-Slit Experiment, Phys. Rev. Lett. 95, 040401 (2005).

3.6. STRONG FIELD APPROXIMATION

95

**3.6.6 High harmonic generation
**

When an intense laser pulse of frequency ω1 impinges on any kind of sample usually harmonics of ω1 are emitted. A typical signature of the emission spectrum in the case of strongly driven atoms, molecules or clusters is that the harmonic yield does not simply roll-off exponentially with increasing harmonic order. Instead, a plateau is observed. This is a prerequisite for high order harmonic generation (HOHG) being of practical relevance as an efﬁcient short wavelength source. As targets for HOHG one may think of single atoms, dilute gases of atoms, molecules, clusters, crystals, or the surface of a solid (which is rapidly transformed into a plasma by the laser). In fact, for all those targets HOHG has been observed experimentally. Even a strongly driven two-level system displays nonperturbative HOHG. The mechanism generating the harmonics and its efﬁciency, of course, vary with the target-type. In the case of atoms the socalled three step model explains the basic mechanism in the spirit of simple man’s theory: an electron is freed by the laser at a certain time t , subsequently it oscillates in the laser ﬁeld, and eventually recombines with its parent ion upon emitting a photon of frequency ω = n ω1 , n ≥ 1. (3.370) This process is illustrated in Fig. 3.21. If the energy of the returning electron is , the energy of the emitted photon is ω = + | f | where f is the energy of the level which is ﬁnally occupied by the electron, for example, the groundstate.

Energy

**Figure 3.21: Illustration of the three step model for high harmonic generation. An electron
**

is (i) released, (ii) accelerated in the laser ﬁeld, and (iii) driven back to the ion. There it may recombine upon emitting a single photon which corresponds to a multiple of the photon energy of the incident laser light.

From this simple considerations we conclude that the maximum photon energy one can expect is ωmax = max + | f |. Using (3.363) we obtain at the recombination time trec

¡ ¡ ¡ ¡ ¡ ¡ ¡

Space

**96 for the return energy
**

ret ret =

CHAPTER 3. ATOMS IN EXTERNAL FIELDS

1

1 p 2 (trec ) = [A(trec ) − A(tion )]2 2 2

(3.371)

**where we have to impose [see (3.366)] |r (trec )| = |α(trec ) − α(tion ) − A(tion )(trec − tion )| < ε.
**

!

(3.372)

Figure 3.22 shows the possible return energies fulﬁlling (3.371) and (3.372). We infer that the maximum return energy is around 3.2. Closer inspection shows that the number is 3.17 so that the cut-off law reads ωmax = 3.17Up + | f | . (3.373)

LEWENSTEIN showed (see “Further reading” below) that, more precisely, it reads ωmax = 3.17Up + 1.32| f |.

**Figure 3.22: Return energy as a function of the ionization time. The color coding indicates
**

the time between recombination and ionization (the longer this time the lighter the color). The maximum return energy is 3.17Up . The course of the laser ﬁeld is shown in panel (b).

From simple man’s theory one expects that harmonic generation should be much less efﬁcient in elliptically polarized laser ﬁelds since, classically, the freed electron never comes back to its parent ion so that recombination can be considered unlikely. This indeed was conﬁrmed experimentally.

3.6. STRONG FIELD APPROXIMATION

97

Besides the academic interest, harmonic generation in atoms, molecules and clusters has huge practical relevance as an efﬁcient source of intense XUV radiation. This is because (i) the ponderomotive scaling of the cut-off allows to achieve high values of max and thus high harmonic orders n, and (ii), fortunately, the strength of the harmonics does not decay exponentially with the order n but displays, after a decrease over the ﬁrst few harmonics, an overall plateau (at least on the logarithmic scale) up to the cut-off energy 3.17 Up +| f |, allowing relatively high intensities at short wavelengths. In fact, high order harmonics below λ = 4.4 nm, the so-called water-window (between the K-edges of carbon and oxygen) have been observed experimentally. The intensity of the emitted radiation in the plateau region is about 10−6 of the incident laser intensity which is typically 1015 –1018 Wcm−2 in rare gas experiments. Therefore, the intensity of the high order harmonics is sufﬁcient for various kinds of applications, such as interferometry, for dense plasma diagnostics, holography, high-contrast microscopy of biological materials, and attosecond spectroscopy or metrology. Attosecond pulses are generated via harmonic generation. If the incoming pulse is already short (i.e., consists only of a few cycles) the harmonic emission is restricted to a narrow time window similar to the “double slit in time”-experiment mentioned above. As a consequence, the harmonic pulse has a duration that is short compared to the laser period of the incoming pulse (usually a few hundred attoseconds). If the incoming laser pulse is longer, one can construct attosecond pulse trains by selecting a few phase-locked harmonics. Attosecond pulses that are generated via harmonic generation have been used to probe the ionizing laser ﬁeld itself as well as fast atomic processes such as Auger decay. Figure 3.23 shows an example for experimental high-order harmonic spectra. For calculating the rate of harmonic emission one may follow the same route as in the SFA treatment of ionization. Harmonic generation and above threshold ionization (ATI) are complementary to each other: while in harmonic generation the electron comes back to the ion and eventually recombines, upon emitting radiation, in ATI it rescatters upon which it may gain additional energy. In harmonic generation one observes a plateau reaching up to photon energies 3.17 Up + | f |. In ATI a plateau is observed as well—this time with respect to the kinetic energy of the photo electrons— extending up to 10 Up (for one rescattering event). In classical electrodynamics, the total radiated power by a dipole of charge q is given by Larmor’s formula 2q 2 P = 3 |¨|2 . r (3.374) 3c Thus, in a semiclassical approach, it appears reasonable to replace the acceleration by its quantum mechanical expectation value and making use of Ehrenfest’s theorem. One obtains 2 ˆ 2 2q 2 1 ∂H 2q 2 d2 . (3.375) 〈ˆ〉 = 3 r − P= 3 ∂ˆ r 3c dt 2 3c m The last expression on the right-hand side is particularly suited for the numerical evalu-

98

CHAPTER 3. ATOMS IN EXTERNAL FIELDS

**Figure 3.23: Harmonic production efﬁciency in Ar and Ne at 2 × 1015 and 5 × 1014 Wcm−2 ,
**

respectively, using a 7-fs Ti:sapphire laser pulse. [From M. SCHNÜRER et al., Absorption-Limited Generation of Coherent Ultrashort Soft-X-Ray Pulses, Phys. Rev. Lett. 83, 722 (1999).]

ation of the harmonic spectra. In order to simplify even further we write the dipole as a Fourier-transform, ∞ q dω exp(iωt )d(ω). (3.376) d(t ) = q 〈ˆ〉 = r 2π −∞ The total emitted energy then is

∞ rad

=

dt P =

−∞

2 3c

3

∞

dω ω 4 |d(ω)|2 ,

−∞

(3.377)

and we infer that the yield radiated into a spectral interval [ω, ω + dω] is εrad, ω dω ∼ ω 4 |d(ω)|2 dω. (3.378)

A full quantum mechanical treatment reveals that calculating the harmonic spectrum emitted by a single atom from the square of the dipole expectation value is actually incorrect. Since the expectation value of the number of photons in a mode ω, k (with ˆ ˆ creation and annihilation operators a † , a , respectively) at time t is

t

**〈ˆ† (t )ˆ(t )〉 = 〈ˆ† (ti )ˆ(ti )〉 + 2C ℜ dt 〈ˆ(t )ˆ(ti )〉 exp(−iωt ) a a a a r a
**

ti

**3.6. STRONG FIELD APPROXIMATION
**

t t

99 (3.379)

+C 2

ti

dt

ti

dt 〈ˆ(t )ˆ(t )〉 exp[iω(t − t )], r r

where C is a coupling constant, one sees that if the mode under consideration is not excited at the initial time t = ti , as it is the case here, only the third term survives. This term accounts for spontaneous emission and scattering. Hence, the harmonic spectrum of a single atom should be calculated from the two-time dipole-dipole correlation function 〈ˆ(t )ˆ(t )〉 instead of the Fourier-transformed one-time dipole. However, if one r r considers a sample of N atoms

N N t t

〈ˆ† (t )ˆ(t )〉 = C 2 a a

k=1 j =1 ti

dt

ti

dt 〈ˆk (t )ˆj (t )〉 exp[iω(t − t )] r r

(3.380)

results and, by assuming that all these atoms are uncorrelated, that is 〈ˆk (t )ˆj (t )〉 r r 〈ˆk (t )〉〈ˆj (t )〉, one arrives at r r

N t 2

〈ˆ (t )ˆ(t )〉 ≈ C a a

†

2 k=1 ti

dt 〈ˆk (t )〉 exp(iωt ) r

(3.381)

if N 1 is assumed so that the self-interaction terms ∼ 〈ˆk (t )〉〈ˆk (t )〉 contribute neglir r gibly. Moreover, if all atoms “see” the same ﬁeld one obtains simply the absolute square of N times the single dipole expectation value. Therefore, calculating the harmonic spectra from the Fourier-transformed dipole, although not correct in the single atom response case, is a reasonable method when comparison with high-order harmonic generation experiments in dilute gas targets is made. Hence, for the study of macroscopic propagation effects the dipole expectation value may be inserted as a source in Maxwell’s equations. SFA for harmonic generation: the Lewenstein-model The dipole expectation value of a single atom with one active electron (q = −1) is d(t ) = −〈Ψ(t )|ˆ|Ψ(t )〉 r ˆ = −〈Ψ0 (ti )|U (ti , t ) ˆ U (t , ti )|Ψ0 (ti )〉, r ˆ (3.382)

where we assumed that at an initial time ti the electron starts in the state |Ψ0 (ti )〉 =: |Ψ0 〉. Using (3.307) we obtain d(t ) = −〈Ψ0 (t )|ˆ|Ψ0 (t )〉 r

t

(3.383)

−i +i

ti t

ˆ ˆ dt 〈Ψ0 (t )|W (t )U (t , t )ˆ|Ψ0 (t )〉 r ˆ dt 〈Ψ0 (t )|ˆU (t , t )W (t )|Ψ0 (t )〉 r ˆ

t ti

ti t

−

ti

dt

ˆ ˆ ˆ dt 〈Ψ0 (t )|W (t )U (t , t )ˆU (t , t )W (t )|Ψ0 (t )〉. r ˆ

100

CHAPTER 3. ATOMS IN EXTERNAL FIELDS

The ﬁrst term vanishes for a spherically symmetric binding potential. The second and ˆ third term are complex conjugates of each other and describe ionization (W ), propagaˆ ), and recombination (ˆ) (i.e., the emission of harmonic radiation) in different tion (U r time-ordering. The last term involves one additional interaction with the laser ﬁeld. We will neglect it here without, however, omitting to point out that it has been discussed in the literature (see “Further reading” below). Replacing—as in the SFA for ionization— ˆ ˆ the full time evolution operator U by U (V) ,

t

d (t ) = −i

ti

(L)

ˆ ˆ dt 〈Ψ0 (t )|W (t )U (V) (t , t )ˆ|Ψ0 (t )〉 + c.c., r

(3.384)

**ˆ we shall recover the Lewenstein-result. In length gauge [W (t ) = E (t ) · ˆ] we obtain r (suppressing the +c.c.)
**

t

d (L) (t ) = −i dt

ti

d3 p 〈Ψ0 (t )|E (t ) · ˆ|p + A(t )〉〈p + A(t )|ˆ|Ψ0 (t )〉e−iS p (t ,t ) (3.385) r r

**ˆ where we used (3.305) and U (V) (t , t )|p + A(t )〉 = e−iS p (t ,t ) |p + A(t )〉. With
**

t

**S p, 0 (t , t ) = we can write (3.385) as
**

t

dt

t

1 2

[p + A(t )]2 −

0

(3.386)

d (L) (t ) = −i dt

ti

d3 p 〈Ψ0 |E (t ) · ˆ|p + A(t )〉〈p + A(t )|ˆ|Ψ0 〉e−iS p, 0 (t ,t ) . r r

(3.387)

**Introducing the dipole matrix element µ(p) = 〈p|ˆ|Ψ0 〉 = r we have
**

t

1 (2π)

3/2

d3 r e−ip·r r Ψ0 (r )

(3.388)

d (L) (t ) = −i dt

ti t

d3 p e−iS p, 0 (t ,t ) µ[p + A(t )]E (t ) · µ∗ [p + A(t )] + c.c. (3.389) d3 p e−iS p, 0 (t ,t ) µ∗ [p + A(t )]E ∗ (t ) · µ[p + A(t )] + c.c. (3.390)

= i dt

ti

**The integration over momentum can be performed using the saddle-point approximation again: ∇ p S p, 0 (t , t ) = 0.
**

!

(3.391)

**3.6. STRONG FIELD APPROXIMATION
**

For a linearly polarized laser pulse with a slowly varying envelope we have ˆ E (t ) = Ee z cos ωt , so that α(t ) − α(t ) =

t t

101

A(t ) = − ˆ E ω2

ˆ E ω

e z sin ωt ,

(3.392)

dt A(t ) =

e z (cos ωt − cos ωt )

(3.393)

and

∂ S p, 0 (t , t ) ∂ pz ⇒ p z,s (t , τ) = −

= p z (t − t ) +

ˆ E ω

2

(cos ωt − cos ωt ) = 0

!

(3.394)

, τ=t −t . (3.395) ω2 τ The transverse stationary momentum vanishes, p x,s = py,s = 0. Plugging ps into (3.386) and integrating yield the stationary action Ss (t , τ) = (Up − with C (τ) = sin ωτ −

0 )τ − 2Up

ˆ E[cos ωt − cos ω(t − τ)]

1 − cos ωτ ω2τ

− Up 4

C (τ) ω

cos[(2t − τ)ω]

(3.396)

. (3.397) ωτ 2 In the original Lewenstein-paper it is shown that the cut-off law 3.17Up + | 0 | can be derived from the function C (τ). Setting ti = 0, the ﬁnal result for the SFA dipole after saddle-point integration reads

t 3/2

sin2

ωτ

d (L) (t ) = i

0

dτ

2π iτ

µ∗ [ p z,s (t , τ) + A(t )] z

(3.398)

ˆ ×µ z [ p z,s (t , τ) + A(t − τ)]E cos ω(t − τ)e−iSs (t ,τ) + c.c. from which, via Fourier-transformation, the harmonic spectra εrad, ω [Eq. (3.378)] can be calculated. Figure 3.24 shows an example for a harmonic spectrum calculated using the Lewenstein model. Harmonic generation selection rules As the name “harmonics” suggests, the emission of laser-driven targets mainly occurs at multiples of the fundamental, incoming laser frequency ω1 , ω = nω1 (3.399)

102

CHAPTER 3. ATOMS IN EXTERNAL FIELDS

**Figure 3.24: Harmonic spectrum obtained using the SFA for H(1s), 2×1014 Wcm−2 , and photon
**

energy 1.17 eV. The time integral in (3.398) was calculated either directly (labelled “exact”) or applying the saddle-point approximation. The expected cut-off at harmonic order n = 72.3 is ´ conﬁrmed. [From D.B. MILOŠEVI C and W. BECKER, Role of long quantum orbits in high-order harmonic generation, Phys. Rev. A 66, 063417 (2002).]

3.6. STRONG FIELD APPROXIMATION

103

with n the harmonic order. In the case of atoms in a linearly polarized laser ﬁeld, for instance, only odd harmonics are emitted, i.e., n = 1, 3, 5, . . .. One could think that this “quantized” emission is a quantum effect. However, this is not the case. Pure classical simulations also show harmonic generation and not just continuous spectra. The selection rules governing which harmonic orders n are allowed and which are forbidden are determined by the symmetry of the combined system target + laser ﬁeld, i.e., the symmetry of the ﬁeld dressed target, also called dynamical symmetry. We shall now employ the Floquet theory introduced in Sec. 3.5.1 to derive the selection rules for harmonic emission for a few exemplary systems. ˆ Let H (t ) be the Hamiltonian of an electron in a linearly polarized monochromatic ˆ ˆ ˆ r laser ﬁeld E cos(ω1 t )e z of amplitude E and an ionic potential V (ˆ), ˆ H (t ) = ˆ2 p 2 ˆ r ˆˆ + V (ˆ) + E z cos ω1 t . (3.400)

ˆ The Schrödinger equation reads i∂ t |Ψ(t )〉 = H (t )|Ψ(t )〉, and since the Hamiltonian is periodic in time, ˆ ˆ H (t + 2π/ω1 ) = H (t ), (3.401) from the Floquet theorem (cf. Section 3.5.1) |Ψ(t )〉 = e−iεt |Φ(t )〉, |Φ(t + 2π/ω1 )〉 = |Φ(t )〉 (3.402)

**follows where ε is the quasi-energy, and |Φ(t )〉 fulﬁlls the Schrödinger equation ˆ(t )|Φ(t )〉 = ε|Φ(t )〉, ˆ(t ) = H (t ) − i∂ ˆ
**

t

(3.403)

which looks like a stationary Schrödinger equation in an extended Hilbert space with the time as an additional dimension and with the scalar product ω1 2π

0 2π/ω1

〈〈Φ|Φ 〉〉 :=

dt 〈Φ(t )|Φ (t )〉.

(3.404)

Hereafter, we refer to ˆ and |Φ(t )〉 already as Floquet-Hamiltonian and Floquet state, respectively (although usually this is done not before expanding them in Fourier series [see Section 3.5.1]). Floquet states are ﬁeld-dressed states. For the derivation of the harmonic generation selection rules we assume an inﬁnitely long laser pulse. It is then reasonable to assume that the system is well described by a single, nondegenerate Floquet state. The only nonvanishing dipole expectation value is in ﬁeld-direction and then reads d (t ) = −〈Ψ(t )|ˆ|Ψ(t )〉 = −〈Φ(t )|ˆ|Φ(t )〉. z z (3.405)

104

CHAPTER 3. ATOMS IN EXTERNAL FIELDS

**We deﬁne the dipole strength of the harmonic n as
**

2π/ω1 2 2

|d (n)|2 =

0

ˆ dt exp(−inω1 t ) d (t ) = 〈〈Φ| exp(−inω1 t ) z |Φ〉〉

(3.406)

which is proportional to the absolute square of the Fourier-transformed dipole. The squared extended Hilbert space matrix element on the right-hand side of (3.406) may be also interpreted as the probability for a transition from a Floquet state to itself, genˆ erated by the operator exp(−inω1 t ) z , accompanied by the emission of radiation of frequency nω1 . The Floquet-Hamiltonian ˆ(t ) is invariant under space inversion plus a translation in time by π/ω1 , ˆ Pinv = (r → −r , t → t + π/ω1 ) (3.407) ˆ ˆ −1 ˆ so that Pinv |Φ〉 = σ|Φ〉 and σ is a phase, i.e, |σ|2 = 1. Inserting the unity Pinv Pinv in the matrix element in (3.406) twice yields ˆ −1 ˆ ˆ ˆ ˆ −1 ˆ 〈〈Φ| exp(−inω1 t ) z |Φ〉〉 = 〈〈Φ|Pinv Pinv exp(−inω1 t ) z Pinv Pinv |Φ〉〉

〈〈Φ|σ ∗ σ|Φ〉〉

(3.408)

ˆ ˆ ˆ −1 ˆ = 〈〈Φ|Pinv exp(−inω1 t ) z Pinv |Φ〉〉 = − exp(−inπ) 〈〈Φ| exp(−inω1 t ) z |Φ〉〉. It follows that n must be odd in order to fulﬁll − exp(−inπ) = 1.

(3.409)

(3.410)

Hence, only odd harmonics are emitted in the case of linearly polarized laser pulses impinging on spherically symmetric systems such as atoms. In the case of monochromatic circularly polarized laser light (with the electric ﬁeld vector lying in the xy-plane) the Floquet-Hamiltonian may be written (using the cylindrical coordinates ρ and ϕ) as ˆ(t ) = H ˆ ˆ r kin + V (ˆ) + ˆ E 2 ρ cos(ϕ − ω1 t ) − i∂ t . (3.411)

This expression is invariant under the continuous symmetry operation ˆ Prot = (ϕ → ϕ + θ, t → t − θ/ω1 ) with θ an arbitrary real number. Instead of (3.408) and (3.410) one has 〈〈Φ| exp(−inω1 t ) ρ exp( iϕ)|Φ〉〉 = exp(inθ iθ) 〈〈Φ| exp(−inω1 t ) ρ exp( iϕ)|Φ〉〉 (3.413) (3.412)

3.6. STRONG FIELD APPROXIMATION

105

where ρ exp( iϕ) is the dipole operator for circularly polarized light (with the same helicity (−) and the opposite helicity (+) as the incident pulse, respectively). Equation (3.413) requires for all θ exp[iθ(n 1)] = 1 (3.414) to hold, which cannot be fulﬁlled for any n > 1 so that no harmonics are emitted. However, circularly polarized harmonics may be emitted if bichromatic incident laser light is used. With the two lasers polarized in opposite directions and frequencies ω1 and mω1 , respectively, the interaction Hamiltonian reads ˆ W (t ) = ˆ E1 2 ρ cos(ϕ − ω1 t ) + ˆ E2 2 ρ cos(ϕ + mω1 t ). (3.415)

ˆ ˆ E1 and E2 are the electric ﬁeld amplitudes of the ﬁrst and second laser, respectively. The symmetry operation under which the Floquet-Hamiltonian is invariant now reads ˆ (m+1) Prot = ϕ → ϕ + 2π m +1 , t→t− 2π ω1 (m + 1) . (3.416)

In the same manner as in the two previous examples one arrives at the condition 1 = exp i2π Hence, harmonics of order n = k(m + 1) ± 1, k = 1, 2, 3, . . . (3.418) n 1 . (3.417)

m +1

are expected. The harmonics with n = k(m + 1) + 1 have the same polarization as the incident laser, whereas those with n = k(m + 1) − 1 are oppositely polarized. With increasing m more and more low order harmonics are suppressed. This might be a promising way to transfer laser energy efﬁciently to shorter wavelengths. The same selection rule (3.418) is obtained for a target having a M -fold discrete rotational symmetry axis parallel to the laser propagation direction. An example for such a target is the benzene molecule with M = 6. The Floquet-Hamiltonian in this case may be written as ˆ(t ) = H ˆ ˆ kin + V (ρ, ϕ, z) + ˆ E 2 ρ cos(ϕ − ω1 t ) − i∂ t . (3.419)

ˆ Owing to the discrete rotational symmetry CM of V (ρ, ϕ, z) the symmetry operation of interest now is 2π 2π ˆ (M Prot ) = ϕ → ϕ + , t→t− , (3.420) M ω1 M

106 from which the selection rule

CHAPTER 3. ATOMS IN EXTERNAL FIELDS

n = kM ± 1,

k = 1, 2, 3, . . .

(3.421)

follows which is indeed of the same form as in the bichromatic, atomic case (3.418). Note, that (3.419) is only a single active electron-Hamiltonian but sufﬁcient for the purposes here because the electron-electron interaction term is invariant under the operation (3.420) anyway. For deducing these selection rules one assumes that the incident laser pulse is inﬁnitely long. This is required for (3.401) to be true. In ﬁnite laser pulses the simple selection rules above may be violated and one has to consider not only a single Floquet states but superpositions of them (see “Further reading”).

Further reading: The “classic” paper on the Lewenstein model is M. LEWENSTEIN, PH. BALCOU, M. YU. IVANOV, ANNE L’HUILLIER, and P.B. CORKUM, Theory of high-harmonic generation by low frequency laser ﬁelds, Phys. Rev. A 49, 2117 (1994). Perhaps the clearest account of HOHG [including a discussion of the fourth term in (3.383)] is presented in W. BECKER, A. LOHR, M. KLEBER, and M. LEWENSTEIN, A uniﬁed theory of high-harmonic generation: Application to polarization properties of the harmonics, Phys. Rev. A. 56, 645 (1997). A review is given P. SALIÈRES, A. L’HUILLIER, P. ANTOINE, and M. LEWENSTEIN, Adv. At. Mol. Opt. Phys. 4, 83 (1999). Concerning the proper quantum mechanical calculation of the harmonic emission of an isolated atom see, for instance, B. SUNDARAM and P.W. MILONNI, Phys. Rev. Lett. 41, 6571 (1990); J.H. EBERLY and M.V. FEDOROV , Phys. Rev. A 45, 4706 (1992); P.L. K NIGHT and P.W. M ILONNI , Phys. Rep. 66, 21 (1980). Work where attosecond pulses (produced from harmonics) were used to follow atomic dynamics in real time or for measuring the incoming laser pulse itself is presented in M. DRESCHER et al., Time-resolved atomic inner-shell spectroscopy, Nature 419, 803 (2002) and R. KIENBERGER et al., Steering attosecond electron wave packets with light, Science 297, 1144 (2002). For the realtion of dynamical symmetries and harmonic generation selection rules see, e.g., V. AVERBUKH, O.E. ALON, and N. MOISEYEV, Phys. Rev. A 60, 2585 (1999); F. CECCHERINI and D. BAUER, Phys. Rev. A 64, 033423 (2001); F. CECCHERINI, D. BAUER, and F. CORNOLTI, J. Phys. B: At. Mol. Opt. Phys. 34, 5017 (2001).

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