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F. W. Helbing, G. Steinmeyer and U. Keller- Carrier–Envelope Control of Femtosecond Lasers with Attosecond Timing Jitter

F. W. Helbing, G. Steinmeyer and U. Keller- Carrier–Envelope Control of Femtosecond Lasers with Attosecond Timing Jitter

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05/13/2014

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 644
  Laser Physics, Vol. 13, No. 4, 2003, pp. 644–651.
 Original Text Copyright © 2003 by Astro, Ltd.Copyright © 2003 by
 MAIK “Nauka/Interperiodica”
 (Russia).
 1. INTRODUCTIONRecent advances in ultrashort pulse generation havepushed pulse durations down to a few femtoseconds[1]. Some of the shortest pulses generated to date havea width equivalent to about two optical cycles [2–6].When pulse durations approach this regime, the com-monly used approach of the slowly varying envelopeapproximation (SVEA) starts to fail. Nonlinear opticaleffects, such as second-harmonic generation, are thenexpected to depend not only on the envelope structureof the pulses but also on the structure of the electricfield itself, including its relative phase to the envelope,which has been referred to as the absolute phase.Recently, some first experimental evidence for the fail-ure of the SVEA was reported [7]. In that study, theenergy distribution of electrons generated by multipho-ton ionization (MPI) was investigated. An anticorrela-tion of the electron energies was detected between MPIelectrons ejected in opposite directions. This effect wasonly observed for the very shortest 6-fs pulses availablein that study, but not for longer pulses. However, adirect correlation with measurements of the relativephase between the carrier and envelope has not beenexperimentally confirmed yet.Given the electric-field structure of an optical pulse
  E 
 (
 
 ), the conversion efficiency
η
 
(
 
n
 
)
 for a nonlinear pro-cess of order
n
 can be estimated from(1)
 
1
 Author to whom correspondence should be addressed:Present address: Max-Born-Institut für Nichtlineare Optik undKurzzeitspektroskopie, D-12489 Berlin, Germany.
η
n
()
 E
()
2
n
.
∫ 
 For a simple estimation of the severity of phaseeffects of few-cycle pulses, we separate the carrier andenvelope, assuming that(2)The envelope function
 A
 (
 
 ) has to be carefully cho-sen to ensure energy conservation, i.e.,
η
 
(1)
 
 const, anda vanishing DC part (
 0) when varying theabsolute phase [8] of the pulse. For the computations inFig. 1, we have chosen(3)where
 A
 
0
 and
 A
 
1
 have been chosen to fulfill the above-mentioned criteria. To evaluate the carrier–envelope-phase sensitivity of 
η
 
(
 
n
 
)
 , we calculate the quantity(4)Figure 1 depicts the behavior of 
 
(
 
n
 
)
 for pulses of one to eight cycles in duration and nonlinear opticaleffects up to order
n
 = 50. For pulse durations of morethan three cycles and
n
 
 6, it appears virtually impos-sible to measure any deviation of the quantity fromzero. With current technology and pulses of two ormore cycles in duration, one has to employ highly non-linear processes for a measurable effect. In this regime,the strongest effects are expected for high-harmonicgeneration processes, where
n
 can be on the order of 100 or greater. For low-order processes, such as sec-ond-harmonic generation or two-photon absorption, anoticeable phase-dependence is only expected forpulses approximately one cycle or less in duration.These considerations make it clear that, with currentultrafast technology, direct observation of the break-
 E
()
 A
()ω
ϕ
0
+
()
.cos=
 E
()
∫ 
 A
()
 A
0
 A
1
 / 
0
()
,sech+=
n
()
η
n
()
ϕ
0
= 0
()η
n
()
ϕ
0
=
π
 /2
()
-----------------------------------1.=
 LASER TECHNOLOGIESAND OPTICAL ENGINEERING
 Carrier–Envelope Control of Femtosecond Laserswith Attosecond Timing Jitter
 F. W. Helbing, G. Steinmeyer
 
1
 , and U. Keller
Ultrafast Laser Physics Laboratory, Institute of Quantum Electronics, Swiss Federal Institute of Technology, ETH  Hönggerberg-HPT, CH-8093 Zürich, Switzerland 
 e-mail: steinmey@mbi-berlin.deReceived September 9, 2002
 Abstract
 —In the generation and applications of few-cycle laser pulses, the relative phase between the carrierand envelope plays an important role. In laser oscillators, fluctuations of the carrier–envelope phase are foundto be highly irregular. Several mechanisms contributing to the carrier–envelope-phase noise are identified. Weanalyze thermal contributions, amplitude-to-phase conversion mechanisms, and beam-pointing induced effects.Based on our analysis, we can avoid or reduce certain mechanisms. This is demonstrated with a highly stabi-lized oscillator which displays a residual carrier-envelope-phase noise of a few mrad over integration times of a minute. The residual noise of the stabilized laser corresponds to a timing jitter between the carrier and enve-lope of 10 attoseconds. Control of the carrier–envelope phase to this degree is an important prerequisite for theexploration of phase-dependent nonlinear optical effects and may also be useful in frequency metrology.
 
 LASER PHYSICS
 
Vol. 13
 
No. 4
 
2003
 CARRIERENVELOPE CONTROL645
 down of the SVEA is more likely to be detected withamplified short pulses than at the oscillator level, wheresub-two-cycle pulses are required for a measurableeffect. In this paper, we will first describe methods tomonitor changes of the absolute phase. We will thendiscuss jitter measurements of the phase between thepulse carrier and envelope in a femtosecond laser. Wewill trace back the origin of this noise. Based on theunderstanding of the underlying noise mechanisms, wedescribe the setup of a femtosecond oscillator with arigorously controlled drift of the absolute phase.2. BASIC DEFINITIONSThe relative phase between the carrier and envelopeof an ultrashort pulse (the carrier-envelope-offset phaseor CEO phase [9]) changes on propagation through adispersive medium. The envelope travels at groupvelocity
 
g
 =
c
  / 
 n
 
g
 =
c
  /(
 n
 +
ω
 dn
  / 
 
 ω
 ), whereas the under-lying electric field structure, i.e., the carrier, propagatesat phase velocity
 
ϕ
 =
c
  / 
 n
 . This means that a pulse willundergo a permanent change of the CEO phase in a dis-persive medium. When propagating through a dispersivematerial with an index of refraction
n
 (
  z
 ) along an axis
 z
 ,the pulse will accumulate a CEO phase change of (5)where
 L
 is the length of the dispersive material. Notethat it is the first-order dispersion term
dn
 (
  z
 )/ 
 
 ω
 whichgives rise to differing group and phase velocities in amedium. A case of particular importance is propagationthrough a laser cavity, as used in the generation of ultrashort pulses. In such a cavity, the pulse accumu-lates the CEO phase change of Eq. (5) every round tripand
 L
 takes the role of twice the cavity length. For a typ-ical Ti : sapphire laser cavity, such as that described in[6], the roundtrip phase shift between the carrier andenvelope from the 2.3-mm Ti : sapphire crystal, a 3-mair path, and the prism compressor can be estimated asabout 250 optical cycles. However, only the fractionalpart of this phase shift is included in the
∆ϕ
 
CEO
 . As longas the cavity dispersion does not vary, the CEO phasewill evolve strictly linearly with a constant phasechange
∆ϕ
 
CEO
 per round trip time
 
R
 = 1/ 
  f 
 
rep
 . For thefollowing, it is useful to define the CEO frequency [9]:(6)In the case of constant intracavity dispersion, thisCEO frequency is constant. Note that even the tiniestchanges of intracavity dispersion will give rise to ameasurable change of the CEO frequency. In the case
∆ϕ
CEO
2
πλ
------
n
g
 z
()
nz
()
 z
0
 L
∫ 
mod2
π
==
ω
2
c
------
nz
()
ω
-------------
 z
0
 L
∫ 
mod2
π
,
 f 
CEO
∆ϕ
CEO
2
π
---------------
 f 
rep
.=of the above-mentioned Ti : sapphire laser, e.g., a 10
–6
change of cavity dispersion will already cause a 25-kHzshift of the CEO frequency. This consideration immedi-ately demonstrates the necessity to shield the laser cav-ity from environmental influences when excessive fluc-tuations of the CEO frequency need to be avoided.3. MEASUREMENT OF THE CEO PHASEThe electric field structure of an optical pulse cannotbe directly accessed by any measurement. In the fol-lowing, we will describe how the CEO phase can beaccessed by an indirect measurement employing het-erodyning of two different harmonics of the laser field.We will also show how the CEO and absolute phase arerelated to each other.The field of a short laser pulse can be written as(7)where
ω
c
is the (angular) carrier frequency,
 A
(
) is theenvelope function, and
ϕ
0
is the absolute phase of thepulse. In the spectral domain, we can rewrite Eq. (7) as(8)The field of the second-harmonic of (
ω
) is thenwritten as
 E
()
 A
()
i
ω
c
ti
ϕ
0
+
()
,exp=
 E 
˜
ω()
 A
˜
ω()
i
ϕ
0
()
.exp=
 E 
˜
10.10.011 E–31 E–41 E–51 E–61 E–71 E–81 E–91 E–1012345678468101214161820
4HGTHGSHG
n
= 50
n
= 6
n
= 8
n
= 10
n
= 15
n
= 20
n
= 30
n
= 40
Pulse width, cycles
   M  o   d  u   l  a   t   i  o  n  c  o  e   f   f .
      ∆
   (
     n
   )
Pulse duration, fs
Fig. 1.
Sensitivity to carrier–envelope effects
(
n
)
as a func-tion of pulse duration for nonlinear processes of differentorder
n
. Orders
n
= 2, 3, and 4 are designated by SHG, THG,and 4HG, respectively. The bottom axis refers to theFWHM duration of the intensity envelope of the pulse inoptical cycles, i.e., in units
λ
 / 
c
. The top axis designatespulse duration in femtoseconds for a center wavelength of the pulse of 800 nm (Ti : sapphire wavelength range). Thetime axes of the electric field representations in the bottompart of the graph are centered at the respective pulse widthon the pulse width axis of the plot.
 
646
LASER PHYSICS
 
Vol. 13
 
No. 4
 
2003
HELBING
et al
.
(9)where the proportionality factor
γ 
includes the second-order susceptibility and a constant phase shift. Notethat the second-harmonic field is centered at 2
ω
c
while the fundamental field reaches its maximum at
ω
c
. The main consequence of Eq. (9) is that absolutephases add up in sum-frequency generation processes.In the same way, absolute phases will subtract in differ-ence-frequency generation processes. This is wellknown for optical rectification in the generation of THzwaves [10] and can also be employed to generate mid-IR waveforms with a static absolute phase. Parametricamplification may also be used to generate pulses withstatic
ϕ
0
[11].Let us consider a delayed superposition of bothfields and at a frequency
ω
in the area of spec-tral overlap of the fundamental and second harmonic:(10)In the following, we will only consider the cosineterm, which gives rise to a spectral interference signalif the delay
is chosen a nonzero value. Detection of this interference signal allows the determination of theabsolute phase
ϕ
0
in principle. Dispersive effects, how-ever, will typically prevent a direct determination of theabsolute phase using spectral interferometry. Still, thismethod allows the monitoring of shot-to-shot changesof 
ϕ
0
, as has been described in [12–14]. This methodrequires acquisition of a complete spectrum per indi-vidual laser shot. Therefore, spectral interferometrycannot be directly used with MHz repetition rates of oscillators. In the latter case, let us reconsider Eq. (10)with
= 0 and a varying absolute phase
ϕ
0
(
). In thecase of a linear phase evolution
ϕ
0
(
) = 2
π
 f 
0
, the inter-ference term in (10) gives rise to a beat signal with con-stant frequency
 f 
0
. This beat signal is exactly synchro-nous with relative phase changes between the carrierand envelope of the pulse propagating through the lasercavity. One can therefore identify the frequency of thebeat note as
 f 
0
=
 f 
CEO
. The connection to the previouslydefined CEO phase is then given by(11)
 E 
˜
SH
()
ω()γ 
 E 
˜
ω
'
()
 E 
˜
ωω
'
()ω
'
0
∫ 
==
γ 
2
i
ϕ
0
()
 A
˜
ω
'
()
 A
˜
ωω
'
()ω
',
0
∫ 
exp
 E 
˜
SH
()
 E 
˜
 E 
˜
SH
()
 E 
˜
 I 
˜
ω()
 E 
˜
SH
()
ω()
 E 
˜
ω()
+
2
=
i
ϕ
0
()
 A
˜
ω()
exp
γ 
i
ω∆
2
i
ϕ
0
+
()
 A
˜
SH
()
ω()
exp+
2
=
 A
˜
ω()
2
γ 
2
 A
˜
SH
()
ω()
2
2
γ 
 A
˜
ω()
 A
˜
SH
()
ω()
++
×ω∆
ϕ
0
π
 /2++
()
.cos
∆ϕ
CEO
1
 f 
rep
--------
ϕ
0
()
dt 
----------------,=which also holds in the more general case of varyingintracavity dispersion. Note that neither the spectralinterferometry method for single shot CEO phase mea-surement [12] nor the narrowband heterodyningschemes [9] used with mode-locked oscillators allowsdetermination of the absolute phase. In fact, all meth-ods monitor changes in the absolute phase with time,which is effectively proportional to the CEO phaseaccording to Eq. (11).4. MEASURING AND STABILIZINGTHE CEO FREQUENCYOF A FEMTOSECOND LASERFor experimental realization of the heterodynedetection scheme, we additionally broaden the laseroutput spectrum through white-light continuum gener-ation in a microstructure fiber [15], regardless of thelaser used. To some extent this may be disputable,because pulse fluctuations may also give rise tochanges in the CEO phase via an amplitude-to-phasecoupling mechanism inside the fiber [16]. This mayappear particularly cumbersome because of the muchhigher nonlinearity of the microstructure fiber. How-ever, as the fiber is placed outside the laser cavity, non-linear or thermally induced phase changes will not addup as they do for intracavity, as will be shown in moredetail below. This means that a change of first-orderdispersion in the laser gain crystal affects the CEO fre-quency, whereas a change of dispersion in the fiberaffects only the CEO phase in a single pass. For mea-suring the CEO frequency, we heterodyne the funda-mental and the second harmonic of the microstructurefiber continuum [17]. For frequency-doubling of thelong-wavelength components at 1060 nm, an LBOcrystal is used to generate the second harmonic withnoncritical phase matching. Given the 1-cm crystallength, one calculates a phase-matching bandwidth of about 4 nm. Note that all modes within the phase-matching bandwidth contribute to the beat signal. Fun-damental and SHG components at 530 nm are hetero-dyned in a Michelson interferometer. Careful optimiza-tion of the arm lengths in this interferometer is requiredfor detection of the beat signal. Experimental parame-ters of the laser were set to ensure maximum intensityand stability of the continuum components at 1060 andat 530 nm.Figure 2 shows the setup employed and a typical rf spectrum measured by this setup. The CEO beat noteand its mirror frequency are clearly visible at 35 and65 MHz. The measured signal level is 45 dBc in a300 kHz bandwidth. In our experiments, we found asignal level of at least 30 dBc necessary for reliablelocking of the carrier-envelope-offset frequency. In theunstabilized laser with prism dispersion compensation,the frequency of this beat note may change very rapidlyby up to several MHz in one second. This behavior ismost likely due to air turbulence and is already stronglyreduced by enclosing the laser in a box. Excursions of 

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