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Mercury—the Rosetta stone of physics?

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2002 J. Opt. B: Quantum Semiclass. Opt. 4 S376

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INSTITUTE OF PHYSICS PUBLISHING JOURNAL OF OPTICS B: QUANTUM AND SEMICLASSICAL OPTICS
J. Opt. B: Quantum Semiclass. Opt. 4 (2002) S376–S383 PII: S1464-4266(02)37875-3

Mercury—the Rosetta stone of physics?

Thomas Walther1 and Edward S Fry
Department of Physics, Texas A&M University, College Station, TX 77843-4242, USA

E-mail: thw@tamu.edu

Received 19 December 2001

Published 29 July 2002
Online at stacks.iop.org/JOptB/4/S376
Abstract
A surprisingly long list of historical experiments have used mercury atoms.
Thus, these atoms have contributed a tremendous number of the pieces to
the jigsaw puzzle of physics as we know it today. This legacy continues up
to the present. We illustrate the latest phases of this legacy via two ongoing
experiments based on mercury: an implementation of Bohm’s version of an
Einstein–Podolsky–Rosen experiment and UV-lasing without inversion.
Keywords: Entanglement, Einstein–Podolsky–Rosen, Bell inequality,
lasing without inversion
(Some figures in this article are in colour only in the electronic version)

1. Historical overview 2. The Einstein–Podolsky–Rosen experiment

Starting with the first observation of superconductivity in 1911 2.1. Introduction

by Kamerlingh Onnes (1911), a surprisingly long list of historic
In spite of the emerging applications of quantum entanglement
experiments were performed based on mercury. Among others
and quantum information (Steane 1998, Rodgers 1998), their
we find such important discoveries as resonance fluorescence
nature continues to puzzle us. The long-lasting discussion
(Wood 1912), the experiment of Franck and Hertz (1913a,
has an origin dating back in 1935 when EPR published their
1914a, 1916) and the first observation of atomic coherence in
gedanken experiment (Einstein et al 1935). EPR argued that
the Hanle effect (Hanle 1923). More recently we find the first
quantum mechanics is not a ‘complete’ theory. The two
experiments in optical pumping by Kastler (1950), the first
basic problems they saw with quantum mechanics are (1) non-
laser-based Einstein–Podolsky–Rosen (EPR) experiment by
locality or action-at-a-distance and (2) incompleteness in the
Fry and Thompson (1976) and a measurement of an upper limit
description. Both of these could presumably be avoided by
of the permanent electric dipole moment in 199 Hg (Romalis
postulating the presence of some hidden variables (HVs) that
et al 2001).
would permit deterministic predictions for microscopic events.
This historic chain of important experiments leads us to
The relation of quantum mechanics to HV could be considered
reflect on the importance of Hg as an element that has provided
analogous to the relation of thermodynamics to statistical
tremendous help in understanding the atom, just as the Rosetta
mechanics. For example, the thermodynamic quantities in a
stone has helped unravel the mysteries of the hieroglyphs.
gas, temperature and pressure, can be understood in terms of
Clearly, other atomic species deserve distinction as well, which
microscopic (hidden) values of the speeds and directions of the
is why we append a question mark to our title.
individual atoms.
Three reasons for the early success of mercury in atomic
In 1964, John Bell made a giant step forward (Bell
physics lie in the availability of a resonant light source even
1964). Bell revisited the EPR experiment and considered a
before the advent of the laser, the ease of vaporization, and the
version based on the entanglement of spin- 12 particles that
relative stability against oxidation or chemical reactions. But
was introduced by Bohm (1951). The latter has conceptual
even today the importance of mercury as an atom of choice
advantages in comparison to the original EPR experiment
in fundamental experiments continues. As evidence, we will
that involves entanglement in position and momentum. The
discuss the experimental status of two experiments that are
wavefunction of such a system can be written as
underway in our laboratory.
1 1
Present address: Institute for Applied Physics, TU Darmstadt, |

= √ (| ↑
1 | ↓
2 − | ↓
1 | ↑
2 ). (1)
Schlossgartenstr. 7, D-64289 Darmstadt, Germany. 2

1464-4266/02/040376+08$30.00 © 2002 IOP Publishing Ltd Printed in the UK S376


For a given two-particle system, if particle 1 is found to
have spin-up (↑) in some spatial direction, particle 2 must
necessarily have spin-down (↓) in that direction and vice
versa. Specifically, quantum mechanics predicts that the
total spin of this two-particle system is zero, and that for
measurement of both components in one specific direction
the results will be opposite with unit probability. However,
quantum mechanically it is not possible to predict the absolute
orientation of either spin, or to even predict absolute values for
two of the components of the spin of a single particle.
John Bell considered Bohm’s version of the EPR
experiment. Then, by assuming positive probabilities, he
showed that any HV theory satisfying a physically reasonable
condition of locality (LHV theory, e.g. a classical theory) will
yield statistical predictions which must satisfy restrictions for
certain correlated phenomena involving entangled states (see
equation (1)). In other words, classical theories put upper
bounds on measurements of the statistical correlations between
the spin components of the two particles. These restrictions
can be cast into the form of inequalities, which are now
generally referred to as Bell inequalities. Thus, at least in
principle, Bell’s work made it possible for the first time to
experimentally distinguish between the LHV and quantum
mechanical pictures. It should be emphasized that no specifics
of an LHV theory are involved in Bell’s argument. Thus, a
test of a Bell inequality is general and leads to discrimination
between any LHV and quantum mechanics.
Several researchers have since formulated other versions
of the Bell inequalities (Clauser and Shimony 1978) that are
more experimentally amenable. A well known example is
the Bell–Clauser–Horne (BCH) inequality (Clauser and Horne
1974). The BCH inequality is
S(θ1 , θ2 , θ1 , θ2 ) = {R↑↑ (θ1 , θ2 ) − R↑↑ (θ1 , θ2 ) + R↑↑ (θ1 , θ2 )
+ R↑↑ (θ1 , θ2 )}{R1↑ (θ1 ) + R2↑ (θ2 )}−1
1, (2)
where a typical R↑↑ (θ1 , θ2 ) denotes the experimental
coincidence count rates when both particles are detected with
spin up in the directions θ1 and θ2 , respectively; R1↑ (θ1 )
and R2↑ (θ2 ) are singles count rates at detectors 1 and 2,
respectively. The BCH inequality is especially important
because it provides a direct constraint on the experimentally
accessible (observed) detection count rates; it does not require
any additional assumptions for experimental implementation.
However, it depends on the ratio of coincidence rates to singles
rates and is therefore proportional to the detector efficiency.
Consequently, for low detection efficiency, the inequality
(equation (2)) is always satisfied by the quantum mechanical
predictions; this is easily recognized by noting that for low
detection efficiencies the singles rates in the denominator are
large compared with the coincidence rates in the numerator.
Therefore, equation (2) can only be used for a definitive test if
the detectors have very high efficiencies so that the quantum
mechanical predictions violate the inequality. Note also, that
it is not necessary to simultaneously measure both projections
in the case of the BCH inequality.
The principal problem for experimental tests of the BCH
inequality lies in the fact that experimental imperfections
generally preclude a definitive test, i.e. they tend to change the
quantum mechanical predictions so that they no longer violate
the Bell inequalities.
Mercury—the Rosetta stone of physics?
In an actual experiment, the goal will be to choose
the experimental conditions such that the resulting quantum
mechanical prediction, SQM , provides a maximum violation of
the BCH inequality. For θ1 , θ2 , θ1 , θ2 equal to 135◦ , 0◦ , 225◦ ,
and 90◦ , respectively, we find


2 
◦ ◦ ◦ ◦1 √ ε−
SQM (135 , 0 , 225 , 90 ) = ηgε+ 1 + 2F (3)
2 ε+
where η is the detection efficiency for both detectors, g is
the conditional probability of particle 2 entering detector 2,
if particle 1 has entered detector 1, ε± are measures of the
quality of the spin analysis, and F is a measure of the purity
of the entangled state. In order to obtain the largest possible
violation of the BCH inequality, equation (2), by the quantum
mechanical prediction, equation (3), the parameters η, g, ε± ,
F should be as close to unity as possible.
Finally, any test of the Bell inequalities is statistical in
nature; specifically, count rates have statistical errors and the
measured quantities are ratios of coincidence count rates to
singles count rates. These statistical errors must be sufficiently
small so that the resulting error in the measured value of S is
much less than the magnitude of the violation (the amount
by which SQM exceeds one). Specifically, it is not the
magnitude of the violation, but rather its comparison to the
error limits of an experimentally determined value of S that
is a measure of the significance of the violation. As an aside
it should be noted that some experimental parameters must
be measured (and therefore have errors associated with them)
in order to evaluate SQM ; therefore, the quantum mechanical
prediction SQM will have errors associated with it.
2.2. Loopholes
Despite a substantial number of experimental tests of the
Bell inequalities, no experiment to date has been entirely
loophole free (Pearle 1970, Clauser and Horne 1974, Clauser
and Shimony 1978, Zeilinger 1986, Santos 1996, Gisin and
Gisin 1999). Specifically, one or more of the following
loopholes were present: (1) the spatial correlation loophole, (2)
the detection efficiency loophole, and (3) the enforcement
of locality (communication loophole). For a more detailed
discussion on the loopholes in previous experiments, we refer
to the literature (Zeilinger 1986, Santos 1996, Fry and Walther
1999, 2001).
The first loophole. The spatial correlation loophole relates to
the requirement that correlations between the two particles can
only be measured as long as each partner of the entangled pair
enters its respective detector. In the ideal case the two-particle
entangled state is generated by a two-body decay that involves
only the two particles that are entangled.
The second loophole. The detection efficiency loophole
originates from experimental imperfections. Low detection
efficiencies reduce the observable correlation, since the lower
the detection efficiency, the lower the probability that both
partners of an entangled pair will be detected. However, high
detection efficiencies must also be accompanied by a high
probability of actually detecting both particles of an entangled
S377
T Walther and E S Fry
Figure 1. A two-photon dissociation scheme for the generation of
entangled states between the dissociation products requires potential
energy curves with distinct differences between the electronic states
involved.
pair in their respective detectors, i.e. a high conditional
probability g of finding particle 2 in detector 2 provided that
particle 1 entered detector 1 (Santos 1996). This also relates
to the first loophole, spatial correlation.
The third loophole. Enforcement of the locality condition is
also known as the communication loophole. It requires that
the choice of correlation measurement for the two particles
be completely independent at each analyser. Specifically, one
must guarantee no communication between the two analysers
during a measurement, i.e. the time interval from choice of
analyser ‘orientation’ to detection from one particle must be
outside the space–time light cone of the other particle and vice
versa.
This means that the times required for the two detection
events must be short compared with the time required for a
light signal to propagate from one analyser/detector to the
other. This involves not only a large separation between
the two analyser/detectors, but also the requirement for fast
detection schemes and electronics. The time for fast detection
as defined in this context is the time it takes to choose and
set the analyser settings in a random fashion, analyse the spin
state, and complete and record the outcome of the experiment.
Very recently, two experiments were reported which close
the first loophole and either the second (Weihs et al 1998) or
the third loophole (Rowe et al 2001).
2.3. A Bell inequality test based on diatomic molecules
The use of a two-particle system in an entangled state for a test
of Bell inequalities suggests that a diatomic molecule might be
an ideal starting ground. In fact, assuming a nuclear spin- 12 for
each atom, one of the nuclear wavefunctions (the singlet state)
of the molecule in the separated atom basis can be written as
in equation (1). This state is identical to that of the two spin-
1 ionization and detection of the photo-ions and photo-
2
particles in Bohm’s classic version of the EPR gedanken
experiment (Bohm 1951, Clauser and Shimony 1978).
Is it possible to prepare a diatomic molecule in such a
state? Yes, but in selecting a suitable atomic species for such
an experiment several requirements must be fulfilled:
(i) The dissociation process must be state specific, since
only nuclear spin singlet states with a total spin I = 0
should result from the dissociation. This suggests a photo-
dissociation process with Fourier-transform-limited laser
S378
two-photon
dissociation
199 199
Hg Hg
199
two-photon Hg S=0 two-photon
2
ionization ionization
for spin-analysis for spin-analysis
Figure 2. Schematic of the mercury-based experiment for the test of
the Bell inequalities. After the generation of the entangled state by a
two-photon dissociation process the correlation of the spin between
the two 199 Hg atoms is measured using a two-photon ionization
process.
pulses and a spectroscopic selection of the dissociation
states.
(ii) Furthermore, the dissociation products must have
lifetimes much longer than the anticipated duration of the
detection process plus the time required to actually arrive
at their respective detectors. It is therefore advantageous
if the dissociation process produces two fragments in their
ground states. Thus, an obvious approach is dissociation
of the molecule via a resonant two-photon Raman
transition to an auto-dissociating level of the molecular
ground state. But this results in a severe limitation on the
atomic species suitable for our experiment: specifically,
in order to reach an auto-dissociating level, the two-
photon process must use photons of different energies and
the Franck–Condon factors must be favourable for both
transitions. This is only possible if the electronic ground
state and the first excited state have potential minima that
are shifted with respect to each other, see figure 1. If
they have minima at the same nuclear distance, only one
transition could be pumped efficiently. It should be noted
that, for example, this requirement precluded the use of
silver atoms for our test; Ag2 dimers have very similar
potential energy curves for the ground and excited states.
(iii) A test of the Bell inequalities requires the measurement of
the correlation between the components of the nuclear spin
in a spin singlet state. This spin analysis should also be
as straightforward as possible. Due to the complications
that result from fine or hyperfine interactions it is
advantageous to perform the experiment with a diatomic
molecule consisting of two spin- 12 atoms with total angular
momentum zero and total electron spin zero. Clearly,
the analysis of the nuclear spin components must be
fast, and highly efficient in order to be able to close
the present loopholes. These requirements suggest that
photo-ionization might be an ideal way of simultaneously
performing the spin-analysis and detection. This can be
achieved by a state-selective excitation followed by photo-
electrons.
All of the aforementioned features are combined ideally in
our favourite atom, 199 Hg, and the resulting 199 Hg2 dimer. For
these proceedings, we will only briefly repeat some of the key
elements of our experiment. For a more detailed discussion,
the reader is referred to the following set of references (Fry
et al 1995, Walther and Fry 1997a, 1997b, Fry and Walther
1996a, 1996b, 1999, Fry et al 1998). The experiment is based

on 199 Hg, which has nuclear spin I = 12 ; it is the first attempt
to actually test the BCH inequalities (equation (2)).
In our experiment 199 Hg2 dimers are generated in a
supersonic jet expansion and are photo-dissociated using two
laser beams in a stimulated Raman transition (see figures 1
and 2). The two wavelengths are at approximately 266 and
355 nm. The energy difference between a photon from each
laser beam is distributed equally to the kinetic energies of the
two atoms. Due to momentum conservation the atoms will
fly apart in exactly opposite directions (180◦ ) in the centre-of-
mass frame. However, as a consequence of the initial velocity
of the dimers in the supersonic jet, the dissociated atoms will
separate at an angle of approximately 130◦ in the laboratory
frame.
The preparation of the entangled state given by
equation (1) requires selecting a molecular state with a total
nuclear spin I = 0. This is possible due to the specific
symmetry rules for the total wavefunction of a homonuclear
diatomic molecule consisting of two fermions. Thorough
analysis of these symmetries (Walther and Fry 1997b) shows
that only the entangled nuclear spin singlet state is dissociated
if the excitation transition at 266 nm starts from states whose
rotational quantum number N is even.
Determination of the correlation in the spin components
of the two entangled atoms as well as detection of the
atoms is achieved via a state-selective two-photon excitation–
ionization scheme (see figure 3). Based on the selection
rules for electronic transitions, one can photo-ionize only
those atoms which are in the state m F = +1/2, i.e. spin up
along the quantization axis by using left-circularly polarized
resonant radiation at 253.7 nm. Since the quantization axis is
determined by the propagation direction of the left-circular
polarized laser beam, the spin component in any direction
is measured by orienting the laser beam to propagate in that
direction. The ionized atoms are detected in two independent
ways, i.e. by observing the photo-ions as well as the photo-
electrons.
In our experiment the enforcement of Einstein locality,
also known as the communication loophole, can be
implemented by employing electro-optic modulators (EOM).
Specifically, the EOM together with a beamsplitting polarizer
can, in a couple of nanoseconds, change the propagation
direction of the excitation laser beam and hence the component
of nuclear spin angular momentum being observed. A 12 m
separation between the detectors will be necessary in order to
rigorously close the locality loophole. This estimate includes
allowances for the selection of a random number, switching
the EOM, firing the nanosecond-detection lasers, the passage-
time of the electrons through the detection system including
the channeltron, and the time to digitize the detector output.
2.4. Relationship to other experiments
Recently, Zeilinger and co-workers were the first to close the
detection efficiency loophole (Weihs et al 1998). They utilized
a down-conversion source and coupled the entangled photon
pairs into two fibres that led to two detector arrangements that
were separated by 400 m. At each detector, fast EOM rotated
the plane of polarization between two randomly selected
values, 0◦ and 45◦ . This is equivalent to randomly rotating
Mercury—the Rosetta stone of physics?
the subsequent analysing polarizer. Zeilinger et al used
a light emitting diode and a beamsplitter as their random
generator. This experiment represents a very important step
in the clarification of the EPR argument.
The flight time of the particles from the source to their
respective detectors does not influence the arguments in
the discussion of the locality condition. It is solely the
communication between the two analyser/detectors that is
important. However, the time of flight for the particles is
important to a discussion of the lifetime of the entangled
state. It is conceivable that the strong correlations predicted
by quantum mechanics only exist for a limited time. This is
the reason why the experiment by Gisin and co-workers (Tittel
et al 1998) represents a major step forward. They performed
a Bell inequality test of the Franson type (Franson 1989) with
position–time entanglement, where the two detectors were
separated by more than 10 km. They measured correlations
consistent with quantum mechanics after taking into account
the losses in the fibre due to imperfect transmission. The
large separation requires a minimum entangled state lifetime
of around 30 µs; this is very long compared with the 40 ns
in Zeilinger’s experiment. Herein lies one of the benefits of
using atoms. Atom speeds are generally much less than the
velocity of light and even with relatively small separations
of the detectors a very long lifetime (milliseconds) of the
entanglement is tested via the Bell inequalities.
The first entanglement of atoms was generated by
Haroche and co-workers (Hagley et al 1997). The specific
implementation of this extremely challenging experiment,
however, did not allow a test of the Bell inequality in the context
described here.
Wineland and co-workers (Rowe et al 2001) are the
first group to close the detection efficiency loophole. They
prepared two Be+ -ions in an ion trap in an entangled state
between two hyperfine Zeeman substates. The two substates
can be identified with spin-up and spin-down and are therefore
equivalent to an entangled state as depicted by equation (1).
The determination of the spin components is, however,
considerably more subtle than in the usual case of spin- 12
particles. The detection efficiency loophole is closed by
resonantly scattering photons in a cycling transition. Due to
the large number of photons observed, the detection efficiency
can be very large. A drawback, however, is that this detection
scheme takes time. And due to the proximity of the two ions
in the trap, it is impossible in these experiments to enforce
the locality condition. In fact, Vaidman has argued that the
situation is even worse in these experiments (Vaidman 2001).
Specifically, due to the detection of the state by the scattering
of many photons, both detection events and the choice of
both analyser orientations overlap throughout a relatively long
period of time (orders of magnitude longer than the time
required for light to travel between the two ions). Another
drawback is that the parameters in the experiment such as
fidelity of the purity of the entangled state, the detection
efficiency and the analyser efficiency cannot be determined
independently. Thus, an independent comparison with the
quantum mechanical expectation value cannot be performed.
S379
T Walther and E S Fry

2 3
Level 3 F=1/2 (6p ) P0

Ionization limit
Ionization (197.3 nm)

F=3/2 3
(6s6p) 6 P°1
Level 2 F=1/2

22 GHz
−
σ−
Analysis (253.7 nm)

2 1
Level 1 F=1/2 (6s ) 6 S 0

m F= −3/2 − 1/2 + 1/2 +3/2

Figure 3. Photo-ionization scheme used for spin analysis of the Hg atoms. The quantization axis is determined by the propagation direction
of the left-hand circular (σ − ) polarized 253.7 nm laser beam. The atom has been analysed as ‘spin-up’ (m F = +1/2) if it is ionized in the
two-photon process, 253.7 + 197.3 nm (via the 6 3 Po1 (F = 1/2) state). Excitation/ionization transitions from m F = −1/2 correspond to a
‘spin-down’ analysis; by the selection rule for σ − , m F = −1, this transition must go via the 6 3 P1o (F = 3/2) state and is highly
suppressed due to its 22 GHz detuning from the F = 1/2 state.

3. Lasing without inversion To further illustrate some of these features, we describe

One of the most exciting potential applications of atomic
coherence effects is the extension of conventional lasers
into the far-ultraviolet. Ordinarily, lasers require population
inversion, since otherwise absorption on the lasing transition
would be too large and gain could never occur. The generation
of atomic coherence by the use of a strong-drive laser can
effectively cancel absorption so that a small number of
atoms in the excited state are sufficient to produce gain
(Kocharovskaya and Khanin 1988, Harris 1989, Scully et al
1989, Kocharovskaya 1992, Scully 1992, Mandel 1994).
However, such three-level schemes that involve two transitions
(a strong-drive transition and the lasing transition) present
two fundamental physics problems for development of cw
ultraviolet lasers based on lasing without inversion (LWI).
First, if the lasing and drive frequencies differ significantly,
then only atoms within a very narrow slice of the velocity
distribution contribute to the gain. Second, the requirement of
fast decay on the drive transition leads to discouragingly high
drive absorption when the drive wavelength is significantly
greater than the lasing wavelength (Lukin et al 1996).
It has been shown that four-level schemes that involve
three transitions (a strong drive, a weak drive, and a lasing
transition) can circumvent these problems (Lukin et al 1999).
If the propagation direction of the lasers involved can be
arranged such that the Doppler shifts of the levels just cancel,
all atoms can be made to contribute to the gain. Huge gain
spikes result that have an additional important feature. Since
the cancellation of the Doppler shifts is only perfect in one
particular direction in space, the lasing will also only occur
in one direction. This is very important for situations where
one wants to generate radiation at frequencies for which mirror
coatings are not available.
a mercury-based experiment which is currently in progress at
Texas A&M University. We consider lasing on the 253.7 nm
resonance transition of mercury as depicted in figure 4. This
is a very practical transition experimentally for the following
reasons:
(1) there is no hyperfine structure,
(2) vapour cells are easy to fabricate and access optically, and
(3) it is currently possible to build a cw probe laser at
this frequency using fibre amplifiers and non-linear up-
conversion in crystals.
Although this is not a VUV transition, and it is already possible
to build robust lasers at this wavelength, this would still be the
first example of large-frequency up-conversion using atomic
coherence techniques. Furthermore, the existence of a probe
laser at the lasing wavelength would be critical as a ‘first step’
to a thorough analysis of the system and to optimize incoherent
pumping schemes.
Figure 4(a) shows a four-level scheme as it exists in
mercury. Level |b
= |6 1 S0
is the ground state, level |d

is the long-lived, metastable state 63 P2 . Level |a
= |6 3 P1

decays to level |b
with decay rate γ B ; level |c
= |7 3 S1

decays to level |a
with rate γC and to level |d
with rate γ D .
Two lasers produce the atomic coherence: one is a strong drive
(Rabi frequency C) tuned to transition c ↔ a, the second is a
weak perturbing drive (Rabi frequency D) tuned to transition
c ↔ d. By strong and weak we mean that typically C > γC
and D > γ D . The lasing transition is denoted by B. Level
|e
= |6 3 P0
is an additional metastable level which does not
contribute to the principal physics of the problem. However, in
a practical implementation we use a repump 404.7 nm laser on
the transition |e
↔ |c
in order to prevent population trapping
in this level.

S380
 Mercury—the Rosetta stone of physics?

λ C=435.8 nm
γ C=7.19 MHz
c +
λ D=546.1 nm
γ D=9.14 MHz D λ E =404.7 nm kB
C 0
d γ E = 3.32 MHz
a kD
e −
o
B +70.7
λ B =253.7 nm
γ B = 1.3 MHz − 74.7 o
b b kC
(a) (b) (c)

Figure 4. (a) Relevant energy levels of mercury to produce lasing at 253.7 nm. (b) Dressed states for a generic four-level scheme, i.e. levels
a–d from part (a). (c) Wavevector orientations that cancel the Doppler effect for the three-photon transition |d
↔ |b
; the x-axis is
perpendicular to the figure, and ki is the wavevector for the transition with wavelength λi .

The dressed-state picture generated by the driving fields
C and D and bare states |b
, |c
, and |d
is discussed elsewhere
(Lukin et al 1999). The results are summarized in figure 4(b).
For the case of all three fields on resonance, the three dressed
states are given to first order in D by


1 D
|+
= √ |a
+ |c
+ |d
(4)
2 C


1 D
|−
= √ |a
− |c
− |d
(5)
2 C
D of the susceptibility over a 3D Maxwell velocity distribution
|0
= |d
− |a
. (6)
C of Hg atoms at a temperature of 300 K. The required
In the limit D → 0 the two dressed states |+
and |−

correspond to the usual Autler–Townes components split by
2C and the dressed state |0
corresponds to the bare state |d
. In
the presence of the perturbing drive D, the state |0
contains an
admixture of |a
and thus has a non-zero dipole matrix element
with ground state |b
. As a result of this coupling, there are
transitions between |0
and |b
, corresponding to three-photon
resonances from |d
to |b
that exhibit interference effects.
It is straightforward to solve the equations of motion of
the density matrix (Scully and Zubairy 1997) for the system
of figure 4. The most relevant result for the present discussion
is that the gain spike is very sensitive to the energy separation
between states |d
and |b
; if it varies, the detuning at which
the gain spike appears varies correspondingly. These facts
are understandable physically by noting that, in the bare state
basis, the gain arises from three-photon Raman-like transitions
from |d
to |b
. For example, consider bare atomic energy
levels ordered as in figure 4(a). The energy separation of |d

and |b
is then E = hν B + hνC − hν D , where ν B , νC , and ν D
are the resonance frequencies of the corresponding transitions.
Clearly, if E changes and the drive frequencies νC and ν D are
fixed then the frequency ν B of the gain spike must change.
For a moving atom, the three photons will have different
Doppler shifts; thus, the effective energy separation of |d

and |b
will generally vary with atomic velocity and the gain
spike will be washed out by velocity averaging. This is just
the four-level version of previous three-level LWI studies.
However, for the atomic energy levels in figure 4(a), the
energy separation E is independent of velocity, if the Doppler
shifts satisfy ν B + νC − ν D = 0. Since Doppler shifts
are proportional to the wavevector k,  this is equivalent to
kB + kC − kD = 0. Thus, if kB + kC − kD = 0 then E will be
constant regardless of the atomic velocity. This relation can
always be satisfied, if the three k-vectors satisfy the triangle
condition. Consequently, it is possible to observe the sharp
gain spike even in a Doppler-broadened medium, provided we
properly orient the three laser beams. This is an important
result. Furthermore, such a cancellation of the Doppler effect
can never be achieved in a three-level LWI system with only
two transitions.
Figure 5 shows the result of averaging the imaginary part
wavevector orientations (laser propagation directions) are
given in figure 4(c). Figure 5(a) shows the usual Doppler
broadened absorption profile for the |b
↔ |a
resonance
transition when both C and D are off. Turning on C has
a negligible effect on this Doppler broadened profile. The
usual Autler–Townes doublet is washed out by the different
Doppler shifts. To see effects at zero detuning, figures 5(b)–
(d) have an expanded abscissa (×10). Although the y-axis
units are arbitrary, they are the same for all four subfigures.
Figure 5(c) shows the characteristic, although relatively small,
sharp absorption spike at resonance when the perturbing drive
D is turned on. Finally, figure 5(d) shows a strong gain spike
when an incoherent pump rab excites some atoms to the state
|a
. As discussed above, a second incoherent pump rec excites
atoms from |e
to |c
to avoid optical pumping into state |e
. It
is noteworthy that the peak gain actually exceeds the depth of
the Doppler-broadened absorption line. Because of the angles
chosen for the three lasers such that kB + kC − kD = 0, all
velocity groups participate in the gain process. Every atom in
the broad Doppler profile contributes to this narrow gain spike!
For the conditions shown, this peak is 800 kHz, FWHM.
It is also interesting to investigate the behaviour of this
gain spike as a function of the deviation in the direction of B
from the ideal direction, specified as the +y-axis in figure 4(b).
Since the cancellation of the Doppler effect is no longer perfect
for such deviations, a rapid reduction of the gain should be
observed with increasing deviation. Indeed, the calculated
FWHM of the gain is only 0.13◦ = 2.3 mrad. This results
in a very narrow gain spike as a function of angle. Thus,
regardless of the diameter or length of the lasing medium, the

S381
T Walther and E S Fry
-100 -50 0 50 100
0.00
-0.01
-0.02
(a)
-0.03
-0.025
C C
(b)
-0.026
-10 -5 0 5 10
Figure 5. Doppler-averaged results for an ensemble of Hg atoms with a Maxwell velocity distribution at a temperature of 300 K. The
imaginary part of the susceptibility χ (in arbitrary units) is shown versus the detuning of the |b
↔ |a
transition (in units of γ D ). Subfigures
(a)–(d) represent the results for cases when the different radiation fields are applied as depicted in the insets (double-headed arrows). The
parameters used are (a) C = 0.0 or C = 6.0, D = 0.0 (expanded abscissa), (b) C = 6.0, D = 0.0, (c) C = 6.0, D = 0.45 and (d) C = 6.0,
D = 0.45, rab = 0.05 (dashed arrow). Furthermore, an auxiliary incoherent pump on the |e
↔ |c
transition with rate rec = 0.3γ D is
included in the calculation.
gain is unidirectional and is positive only at very small angles
to the axis. This means that the laser output will always be
well collimated; it is lasing without mirrors! This is especially
interesting for lasing in the vacuum ultraviolet where it is
difficult to make mirrors.
Numerical calculations with the energy level scheme of
figure 4(a), including all magnetic sublevels and appropriate
angular coupling coefficients, show that coherent population
trapping occurs on the |d
↔ |c
transition and that gain is
reduced because population is optically pumped into these
trapped states. To destroy the trapping, an incoherent pump
rcd must be added on the |d
↔ |c
transition. But, to avoid
destroying the four-level coherence, the polarizations must be
carefully chosen.
The experiment analysed here for lasing at 253.7 nm
is readily generalizable to the VUV. For example, the same
scheme can be modified to lase at 185 nm using the 6 1 P1 ↔
6 1 S0 transition of Hg. Practical cw lasers at other wavelengths
in the deep and/or vacuum ultraviolet are also possible.
Furthermore, the technique described for producing Doppler-
free gain by angular compensation of the Doppler shift is
readily applicable to any multi-step process involving more
than two photons.
4. Trapping
In still another application of Hg to fundamental experiments,
it is noted that mercury is well suited for magneto-optical
trapping experiments. Specifically,
(i) the trapping occurs on a forbidden transition resulting in
small Doppler-limited temperatures;
(ii) mercury has bosonic and fermionic isotopes, which all can
be trapped;
S382
-0.025
D
C
-0.0255
-0.026
(c)
-0.0265
0.05
D
rab
0.025
(d)
-0.025
-10 -5 0 5 10
(iii) the vapour pressure can be easily adjusted over a wide
range;
(iv) mercury possesses long-lived metastable states (3 P0 -
and 3 P2 -state), one of which (3 P2 -state) can be trapped
magnetically and/or optically;
(v) due to the absence of hyperfine or fine structure in the
ground state no repumping lasers are required in order to
prevent optical pumping into states not accessible to the
trapping laser.
5. Summary
Mercury continues to be the choice for many exciting
experiments in atomic physics. The quest for a final answer in
the test of Bell inequalities and thus the answer to the question
whether or not quantum mechanics is a complete theory
creates new ideas for more and more refined experiments.
Simultaneously closing the existing loopholes has proven
difficult. However, the atom-based experiments that have
emerged in the last few years are especially promising.
Acknowledgments
The research described in this paper was supported by
the Robert A Welch Foundation grant no A-1218, by the
National Science Foundation grant PHY-9732459, and by the
Office of Naval Research. The authors thank John Clauser,
Marlan Scully, George Welch, Chris J Bednar, Suzanne Yelin,
and Michael Fleischhauer for many helpful discussions on
the theory and encouragement as well as Robert Kenefick,
Seiichirou Yokoo, Ling Wang and Joe Musser for their
experimental contributions and active participation.

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