J. Camparo and P. Lambropoulos Vol. 19, No. 5 / May 2002 / J. Opt. Soc. Am.

B 1169

Multiphoton transitions in a colored vacuum:

coupling of the ac Stark shift with
spontaneous decay and the Lamb shift

James Camparo
Electronics and Photonics Laboratory, The Aerospace Corporation, Mail Stop M2-253, P.O. Box 92957,
Los Angeles, California 90009

Peter Lambropoulos
Institute of Electronic Structure and Laser, FORTH, P.O. Box 1527, Heraklion 71110, Crete, Greece,
and Department of Physics, University of Crete, Crete, Greece

Received April 9, 2001; revised manuscript received October 9, 2001

In free space, where the vacuum mode density varies relatively slowly in the spectral region of an atomic tran-
sition, an atoms real-field and vacuum interactions are effectively decoupled. Consequently, spontaneous de-
cay and the Lamb shift are, for all practical purposes, independent of any real-field atomic perturbation.
However, in a colored vacuum (i.e., a low-Q cavity) the vacuum mode density can change significantly in the
vicinity of an atomic transition, so that a Stark shift will alter an atoms vacuum environment and thereby
couple real-field and vacuum effects. Since the ac Stark shift is an inherent aspect of multiphoton processes,
this coupling is unavoidable for highly nonlinear fieldatom interactions that occur in cavities. Here we con-
sider this effect for 3 2 resonance-enhanced multiphoton ionization of xenon. 2002 Optical Society of
America
OCIS codes: 270.0270, 270.6620, 020.3690, 020.1670, 190.4180.

There is a fundamental equivalence between the Lamb
and the ac Stark shifts, since both alter the energy level
structure of a quantum system through virtual transi-
tions. The difference, of course, is that the ac Stark shift
induces these transitions with real photons, while the
Lamb shift employs the virtual photons of the vacuum.1
In the early days of optical pumping, when electronic
transitions were excited by rf-discharge lamps, Kastler
sought to reinforce this fundamental equality in a play on
words by referring to the ac Stark shift as a Lamp shift.2
Recently, Brune et al.3 and Marrocco et al.4 highlighted
the relationship between the Lamb and the Stark effects
by studying the vacuum shift of Rydberg atoms with few
and then with zero real photons in a microwave cavity.
Notwithstanding their basic equivalence, the ac Stark
and Lamb shifts are typically viewed as distinct, indepen-
dent processes, primarily because in free space the vacu-
ums mode density is essentially constant over the spec-
tral ranges associated with Stark shifts. However, in a
colored vacuum (i.e., a low-Q cavity), when an atomic
transition is shifted by the Stark effect, the vacuum mode
density in the vicinity of the atomic transition can change
significantly, thereby coupling the Lamb and Stark shifts.
Moreover, as spontaneous decay also depends on the
vacuum mode density, one expects a similar coupling be-
tween spontaneous decay and the Stark shift. Since ac
Stark shifts are an inherent aspect of multiphoton pro-
cesses, this coupling between the vacuum and a real field
is unavoidable for nonlinear fieldatom interactions that
take place in a cavity.
In the present paper, we consider the coupling between
vacuum effects and the ac Stark shift in the highly non-
linear situation of resonance-enhanced multiphoton ion-
ization (REMPI); specifically, 3 2 REMPI of xenon in a
low-Q confocal cavity. The experimental situation we en-
vision is similar to that of Heinzen and Feld,5 who exam-
ined the spontaneous decay and vacuum shift of Ba for a
one-photon transition in an optical cavity. We recognize,
of course, that multiphoton ionization is typically not
studied in cavities, primarily because the physical pro-
cesses of interest in multiphoton ionization generally de-
rive from the strong-fieldatom interaction and not
vacuum effects. Consequently, our investigation of
REMPI in the present context is meant only to illustrate
the fundamental coupling that takes place in a cavity be-
tween the real-fieldinduced ac Stark effect and virtual-
field vacuum effects. As we show, this coupling can have
a significant influence on a transition lineshapes reso-
nant frequency and amplitude.
For computational expediency and consistency, we de-
scribe the real and the virtual radiative interactions by
using a semiclassical density matrix methodology.6,7
Further, since the only dynamically relevant Xe states are
the 5p 6 1 S 0 ground state and the 6s 3/2 1 excited state,
we approximate Xe as a two-level atom as illustrated in
Fig. 1.8 Thus, defining 1 as the Xe ground state, our
previous one-photon transition treatment7 may be
straightforwardly generalized to the case of a multipho-
ton transition.9 This yields the following set of integro-
differential density matrix equations for an ensemble of
atoms placed at the center of a low-Q cavity, in our case a
UV cavity resonant at 147 nm:

0740-3224/2002/051169-05$15.00 2002 Optical Society of America

1170 J. Opt. Soc. Am. B / Vol. 19, No. 5 / May 2002 J. Camparo and P. Lambropoulos

Notice that the ac Stark shift does not appear explicitly in

the expressions for L , 1 , or 2 . Its only influence on
these terms is through the atomic density matrix ele-
ments.
In Eqs. (2) the function F(t) corresponds to the vacuum
field, approximated as a classical zero point field11 with
vacuum mode spacing s :

F t
s
s s exp i s cav t . (3)

Here s is a term related to the cavitys optical character-

istics; s is a vacuum modal frequency; s is the frequency
offset between the cavitys resonant frequency, cav , and
the vacuum modal frequency (i.e., s s cav); and
cav cav 21
0
. As is illustrated in Fig. 1, for those
vacuum modes within a solid angle defined by c , the cav-
ity gives rise to either constructive or destructive interfer-
ence. For the case of present interest, where an atomic
sample is located at the center of a FabryPerot etalon
with mirror reflectivity R and mirror spacing d, it is
straightforward to show that
Fig. 1. Cavity geometry and the relevant Xe energy levels.

11 1 ; t Im 12 , (1a)
s
2
3
2s
3 2s 1
4
cos c
cos3 c
3
, (4)

with
22 1 ; t Im 12 ion 22 , (1b) 1
1 R 1 4R
sin2
sd 1/2
. (5)

s 1 R 2
c
ion i
12 i 0 acI 12 22 11 For vacuum modes outside the critical solid angle, the
2 2
cavity has essentially no effect, so that s 2/3.
12 ; t i L ; t . (1c) Briefly, the numerical computations proceed by averag-
ing F(t) over a zero-point-field simulation time step, T,
(Though cavity QED experiments typically deal with vis- and cutting off the modal expansion of the function at the
ible transitions, we note that UV cavities of reasonable di- first zero of sinc 1/2( s cav) T . More specifically, for
mensions are realizable.10) Here, 0 is the unperturbed the present computations we consider a Gaussian laser
fieldatom detuning (3 f 21 0
), with 21
0
the free-space pulse of full width (which reaches its peak intensity at
resonant frequency of the 5p 6 1 S 0 to 6s 3/2 1 transi- t 1.5 ) and integrate the density matrix equations from
tion; ion is the two-photon ionization rate from 0 to 3 by using a variable-step-size RungeKutta
6s 3/2 1 ; is the three-photon Rabi frequency; acI is Fehlberg method.12,13 The parameters used in the calcu-
the ac Stark shift (for laser intensity I) of the 5p 6 1 S 0 to lations are collected in Table 1; for the Xe ensemble
6s 3/2 1 transition; and the longitudinal and transverse
relaxation terms ( 1 and 2 , respectively) and the Lamb Table 1. Parameters Used in the Density Matrix
shift, L , are functionals of the density matrix given by Calculationsa

Parameter Value
2 21
2
s t
1 ; t 21 2
22 t Re F t t dt , 21 146.96 nm
c 3 0
(2a) Cavity length 5.0 cm
Mirror diameter 2.5 cm

21
2
s t Mirror reflectivity at 147 nm 0.7
2 ; t 21 2 12 t Free-space spontaneous decay rate 44.6 MHz
c 3
0 21 1.68 1018 esu cm
ac 22.7 cm2/(W s)
Re F t t exp i 0 t t dt ,
I peak 3 108 W/cm2
(2b) 10 ns
5 107 I 3/2 s1
21 s

2 t ion 7 1013 I 2 s1
L ; t 21 2 12 t s /2 2 MHz
c 3 0
Simulation time step, T 2.0 ps
Im F t t exp i 0 t t dt .
a
Coefficients for and ion were obtained from MQDT calculations,
(2c) where I is in W/cm2.
J. Camparo and P. Lambropoulos Vol. 19, No. 5 / May 2002 / J. Opt. Soc. Am. B 1171

s ; we found that photoionization probabilities were

Fig. 2. 3 2 REMPI line shapes. The peak of the photoion-
ization probability is P 0 , and the laser detuning corresponding to
this peak is defined as the vacuum shift, .
consistent to 0.15% and vacuum shifts to 0.05%.
Figure 3 shows our results of the vacuum shift as a
function of cavity detuning: circles correspond to the
complete density matrix solution, the dashed curve to the
same calculation but with no ac Stark shift (i.e., ac 0),
and the solid curve to a fictitious case of no Lamb shift
(i.e., L 0) yet with 1 and 2 nonzero. Clearly, the ac
Stark effect alters the location of the vacuum shifts ex-
trema, relocating them from cav 0 to cav acI peak .
While this is intuitively reasonable, Eqs. (2) indicate that
it is a direct consequence of the non-Markovian nature of
the atomvacuum interaction. Notice, however, that
even with the ac Stark effect present there is an enhance-
ment of the vacuum shift at cav 0. This is better il-
lustrated in Fig. 4, where a similar effect is apparent in
the L 0 case, indicating that the enhancement in the
vacuum shift at cav 0 is primarily related to spontane-
ous decay (i.e., 1 or 2 ).
In Fig. 5 we plot the peak photoionization probability,
P 0 , as a function of cavity detuning. Again, circles cor-
respond to the complete density matrix solution, the
dashed curve to ac 0, and the solid curve to L 0.
As the figure shows, the position of P 0 s minimum is un-
affected by the ac Stark effect, maintaining its location at
cav 0. Additionally, however, there is a subsidiary

Fig. 3. Vacuum shift versus cav . Circles, complete compu-

tational results; dashed curve, fictitious case of ac 0 (refer-
enced to the scale on the right), solid curve, fictitious case of
L ( ; t) 0.

placed at the center of the cavity, the relevant free spec-

tral range is 3 GHz. We note that a 0.7 mirror reflectiv-
ity is not unreasonable for UV wavelengths,14 and we as-
sume that the reflectivity of this mirror is narrow band,
so that it affects only vacuum modes in the vicinity of the Fig. 4. Enhancement of Fig. 3 about cav 0. Circles, com-
5p 6 1 S 0 6s 3/2 1 transition. plete computational results; solid curve, fictitious case of
We compute the total ionization probability at the end L ( ; t) 0; dashed line, an aid to guide the eye.
of the pulse as a function of laser detuning, 0 , thereby
obtaining the REMPI line shape. Two representative
line shapes are shown in Fig. 2 for cav 800 and 1300
MHz. The oscillations seen in the line shapes wings are
due to the transient nature of the laser pulse along with
the concomitant ac Stark shift. The peak photoioniza-
tion probability is defined as P 0 , and the laser detuning
corresponding to this peak is defined as . This laser
detuning represents a shift in the multiphoton resonance
condition away from its unperturbed value; therefore
(and in particular its dependence on cavity detuning, cav)
is our measure of the line shapes vacuum shift, and we
refer to it as such for ease of discussion. [For clarity, we
use the term vacuum shift when referring to the multi-
photon line shape, reserving the term Lamb shift for Eq.
(2c).] We tested the validity of our computational proce- Fig. 5. Peak photoionization probability P 0 versus cav .
dure by decreasing the error criterion in the Runge Circles, complete computational results; dashed curve, fictitious
KuttaFehlberg method, decreasing T and decreasing case of ac 0; solid curve, fictitious case of L ( ; t) 0.
1172 J. Opt. Soc. Am. B / Vol. 19, No. 5 / May 2002
minimum at cav acI peak . Since there is little differ-
ence between the complete density matrix results and
those obtained with L 0, we conclude that this subsid-
iary minimum is also a manifestation of the ac Stark
shifts influence on spontaneous decay.
To clarify the ac Stark shifts role in spontaneous decay,
we can take advantage of the convolution and shift
theorems15 to argue heuristically from Eqs. (2a) and (2b)
that
1 ; t
s
2
22 exp i t d ,
2 ; t
s
2
12 0 exp i t d .
Here 22( ) and 12( ) are the Fourier transforms of the
population, 22 , and coherence, 12 , density matrix ele-
ments, respectively, while () is the Fourier transform of
the real part of the vacuum field, F(t):
s
s s s cav
s cav . (7)
Then, using Eq. (7) in relation (6), converting the sum
over modes to an integral, and recognizing that peak sig-
nals occur for 0 acI peak , we obtain
1 exp i cavt x x cav 21
0
22 x
exp ixt dx c.c.,
2 exp i cav acI peak t x x cav 21
12 x cav acI peak exp ixt dx c.c.
Thus, in nonsaturating fields, where 22 and 12 are not
expected to have an oscillatory character, we anticipate
that 1 will be maximized when cav 0, and that 2 will
be maximized when cav acI peak . Moreover, from this
line of argument we can identify the enhancement in the
vacuum shift at cav 0 with an enhancement in the
rate of spontaneous-emission population decay, and the
minimum in the photoionization probability at cav
acI peak with an enhancement in the rate of
spontaneous-emission dephasing.
Taken together, Figs. 3 and 5 demonstrate that for non-
linear fieldatom interactions occurring in a low-Q cavity
it is impossible to disentangle vacuum effects from real-
field effects. Not only does the observed vacuum shift of
an atomic transition depend on both the Lamb and the ac
Stark shifts, but also the real field affects spontaneous de-
cay (i.e., 1 and 2 ). We note that a similar conclusion
was reached by Lewenstein et al.16,17 regarding the abil-
ity of a strong field to dynamically suppress spontaneous
emission in a colored vacuum. As with the work of Le-
wenstein et al., the coupling we observe between the ac
Stark effect and the Lamb shift on the one hand and spon-
taneous decay on the other is a consequence of the atoms
non-Markovian interaction with the colored vacuum.
Moreover, though further investigation is warranted, it
J. Camparo and P. Lambropoulos
would appear that there is a real-fieldinduced decou-
pling between spontaneous-emission population and co-
herence decay. Though such a decoupling seems counter-
intuitive, since it implies a condition (i.e., cav 0) for
which population is returned to the ground state faster
than the decay of atomic coherence, it is to be noted that
Lewenstein et al. also found distinct vacuum effects on
differing density matrix relaxation terms.
In summary, we point out that our motivation for the
present work came from the realization that the context
(6a)
of multiphoton transitions in colored vacuums provides
an unusual situation in which ac Stark and vacuum ef-
fects become entwined. As our results indicate, the in-
(6b)
herent ac Stark shift of a multiphoton transition leads to
radiative characteristics that differentiate these pro-
cesses from multiphoton transitions occurring in free
space. As stated above, we do recognize that multipho-
ton ionization is not studied in cavities, since the objective
of multiphoton processes using lasers of some intensity is
entirely different from the objectives of cavity QED inves-
tigations. Thus we do not present our results for their
practical relevance to multiphoton ionization, but rather
for the unusual interplay between vacuum and laser-
induced effects that they demonstrate. We point out,
however, that, so far as we can tell, contemplating an ex-
periment along these lines is not unrealistic. Though
such an experiment would primarily be of academic inter-
est, the unusual interplay of effects that it would demon-
strate could have value in providing further insight into
cav the general fieldatom interaction.
(8a)
ACKNOWLEDGMENTS
0
The authors thank W. F. Buell for a critical reading of the
manuscript and several informative discussions. This
(8b) work was supported under U.S. Air Force contract
F040701-00-C-0009.
Address correspondence to J. Camparo at the address
on the title page or by e-mail, james.camparo@aero.org.
REFERENCES
1. P. W. Milonni, The Quantum Vacuum (Academic, Boston,
1994).
2. A. Kastler, Displacement of energy levels of atoms by
light, J. Opt. Soc. Am. 53, 902910 (1963).
3. M. Brune, P. Nussenzveig, F. Schmidt-Kaler, F. Bernardot,
A. Maali, J. M. Raimond, and S. Haroche, From Lamb shift
to light shifts: vacuum and subphoton cavity fields mea-
sured by atomic phase sensitive detection, Phys. Rev. Lett.
72, 33393342 (1994).
4. M. Marrocco, M. Weidinger, R. T. Sang, and H. Walther,
Quantum electrodynamic shifts of Rydberg energy levels
between parallel metal plates, Phys. Rev. Lett. 81, 5784
5787 (1998).
5. D. J. Heinzen and M. S. Feld, Vacuum radiative level shift
and spontaneous-emission linewidth of an atom in an opti-
cal resonator, Phys. Rev. Lett. 59, 26232626 (1987).
6. J. C. Camparo, Semiclassical random electrodynamics:
spontaneous emission and the Lamb shift, J. Opt. Soc. Am.
B 16, 173181 (1999).
7. J. C. Camparo, Semiclassical description of spontaneous
decay in a colored vacuum, Phys. Rev. A 65, 013815-1
013815-12 (2002).
J. Camparo and P. Lambropoulos
8. A. T. Georges and P. Lambropoulos, Aspects of resonant
multiphoton processes, Adv. Electron. Electron Phys. 54,
191240 (1980).
9. L. Allen and C. R. Stroud, Jr., Broadening and saturation
in n-photon absorption, Phys. Rep. 91, 129 (1982).
10. C. M. Korendyke and D. G. Socker, Measured optical
performance of three FabryPerot interferometers for use
in a tunable ultraviolet filter, Opt. Eng. 32, 22812285
(1993).
11. T. H. Boyer, General connection between random electro-
dynamics and quantum electrodynamics for free electro-
magnetic fields and for dipole oscillator systems, Phys.
Rev. D 11, 809830 (1975).
12. W. Cheney and D. Kincaid, Numerical Mathematics and
Computing (Brooks Cole, Monterey, Calif., 1985), Chap. 8.
Vol. 19, No. 5 / May 2002 / J. Opt. Soc. Am. B 1173
13. W. H. Press and S. A. Teukolsky, Adaptive stepsize Runge
Kutta integration, Comput. Phys. 6, 188191 (1982).
14. J. F. Osantowski, R. A. M. Keski-Kuha, H. Herzig, A. R.
Toft, J. S. Gum, and C. M. Fleetwood, Optical coating tech-
nology for the EUV, Adv. Space Res. 11(11), 185201
(1991).
15. A. Papoulis, The Fourier Integral and Its Applications
(McGraw-Hill, New York, 1962), Chap. 2.
16. M. Lewenstein, T. W. Mossberg, and R. J. Glauber, Dy-
namical suppression of spontaneous emission, Phys. Rev.
Lett. 59, 775778 (1987).
17. M. Lewenstein and T. W. Mossberg, Spectral and statisti-
cal properties of strongly driven atoms coupled to
frequency-dependent photon reservoirs, Phys. Rev. A 37,
20482062 (1988).