Supplee et al. Vol. 15, No. 7 / July 1998 / J. Opt. Soc. Am.

B 1833

Response of a two-level atom to a

frequency-modulated
optically coherent pulse train

James M. Supplee
Department of Physics, Drew University, Madison, New Jersey 07940, and Department of Physics and Engineering
Physics, Stevens Institute of Technology, Hoboken, New Jersey 07030

Edward A. Whittaker
Department of Physics and Engineering Physics, Stevens Institute of Technology, Hoboken, New Jersey 07030

Keith Andrew
Department of Physics, Eastern Illinois University, Charleston, Illinois 61920

Received October 14, 1997; revised manuscript received March 16, 1998
We present an analytical expression for the response of a two-level atom to a frequency-modulated optically
coherent pulse train. The optical beam has sinusoidal frequency modulation and is chopped to have a square-
wave envelope. We assume that the laser pulses are short compared with the atomic-decay time, the pulse-
repetition time, and the modulation period. With this short-pulse assumption we are able to use a method
similar to Temkin’s [J. Opt. Soc. Am. B 10, 830–839 (1993)] and solve the optical Bloch equations in closed
form. © 1998 Optical Society of America [S0740-3224(98)02206-1]
OCIS codes: 020.1670, 190.0190, 300.6420.

1. INTRODUCTION become increasingly important as new high-power tun-

1–5
Frequency-modulation (FM) spectroscopy is a useful
method for measuring absorption and dispersion and for
improving the sensitivity of optical spectroscopy measure-
ments. In the linear regime (optical intensity much less
than the saturation intensity) absorption and dispersion
are treated as functions of frequency, and the propagation
of the optical beam is calculated simply by addressing the
absorption and the dispersion of each Fourier component
of the beam.1–4 In the nonlinear regime, however, ab-
sorption and dispersion are not simply functions of fre-
quency, since in this regime the optical beam itself modi-
fies the optical characteristics of the sample. One
therefore needs to calculate the response of the material
to the optical field. This usually involves working with
the quantum-mechanical density matrix, or equivalently
(after a coordinate transformation), with the atomic po-
larization and inversion via the optical Bloch equations.
References 6–15 address the interaction of a frequency-
modulated cw beam with a quantum-mechanical atom.
In this paper, however, we wish to calculate the response
of a two-level atom to a frequency modulated and pulsed
beam.
Our motivation for studying the response of an atom to
a pulsed and modulated beam is this: Modulated absorp-
tion spectroscopy affords a very sensitive means to detect
weakly absorbing species,16 and pulsed laser operation
provides both access to higher peak power and the possi-
bility to detect short-lived species. Understanding the
response of an absorber to a pulsed modulated beam will
able laser sources emerge as a result of advanced semi-
conductor laser research. For example, recent experi-
mental work in our laboratory involved sensitive pulsed
spectroscopic measurements using a frequency-
modulated quantum-cascade semiconductor laser.17 The
quantum-cascade laser is a new laser device18 capable of
delivering tunable high-power pulses at high-repetition
frequency in the infrared spectral region. While the
aforementioned published results were in the linear re-
gime, the power capabilities of the quantum-cascade laser
are steadily improving, and we are interested in deter-
mining the effect that nonlinear optical effects may have
on the use of these devices in high-sensitivity spectro-
scopic applications. This paper presents a technique for
exploring these effects theoretically and will thus provide
a basis for interpreting future experiments that could si-
multaneously involve sensitive detection, time resolution,
and nonlinear optical effects.
A number of authors have studied frequency modula-
tion (or phase modulation) in combination with an optical
pulse train. These authors have addressed quite varied
physical situations (despite having the superficial simi-
larity of involving modulation and pulse trains). For ex-
ample, Gallagher and co-workers19–21 were able to obtain
FM spectra using a multimode pulsed dye laser. They
used large modulation frequencies, typically 1 to 12 GHz,
so that the FM sidebands fell outside the power spectrum
of the (carrier) laser pulse. More recently, Eyler et al.22
have demonstrated FM spectra using pulsed amplifica-

0740-3224/98/071833-06$15.00 © 1998 Optical Society of America

1834 J. Opt. Soc. Am. B / Vol. 15, No. 7 / July 1998
tion of a phase-modulated cw laser. This method allows
for a narrow (unmodulated) pulse, so that a modest 400-
MHz modulation is sufficient to place the sidebands well
outside the power spectrum of the carrier pulse. Both of
these groups19–22 addressed cases that essentially in-
volved the interaction of a ground-state atom with a
single modulated pulse; subsequent pulses repeat the
same experiment and are used for signal averaging. The
case we will consider below is quite different in that the
atom will not have time to return to the ground state be-
tween pulses, so that we are considering coherent effects
as later pulses interact with the still excited atom. For
our calculation then, optical coherence from pulse to pulse
is essential.
Other authors have presented calculations addressing
various cases (again different from our case) of the inter-
action of an atom with a phase-modulated and pulsed op-
tical field. Peterson and Gavrielides23 use Fourier series
to calculate the periodic response of the Bloch variables to
a train of quadratically chirped Gaussian pulses. Vi-
tanov and Knight24 calculate the response of a two-level
atom to N identical pulses; they neglect relaxation and
are able to address a wide variety of pulse envelopes in-
cluding chirped pulses. They present a formalism for ex-
tending single-pulse interaction results to the N-pulse
case. Hioe25 calculates the response of a two-level atom
to a single pulse with hyperbolic secant amplitude modu-
lation and with hyperbolic tangent frequency modulation.
Bradley26 is interested in the backscatter from mesos-
pheric sodium and calculates the response of both two-
level atoms and sodium atoms to a resonant, coherent
Gaussian pulse train. Bradley also considers the possi-
bility of phase modulation and concludes that modulation
can increase sodium backscatter by reducing velocity hole
burning. Thomas27 considers the interaction of a multi-
level system with a train of identical Gaussian pulses.
Milonni and Thode28 consider the response of a two-level
atom to a perfectly coherent and unmodulated pulse
train.
In this paper we consider a situation different from
those addressed by the authors mentioned above. We
consider an optical beam with sinusoidal frequency modu-
lation. The beam is first modulated, then chopped, but
leaving the pulses optically coherent from pulse to pulse.
Our pulses therefore simply consist of different sections
chopped from one continuous wave given in Eq. (1) below.
This is not the same as the case of time-delayed identical
pulses. (Even without modulation this distinction is cru-
cial. For example, a chopped sine wave has the same
carrier phase in each pulse, whereas with identical but
time-delayed copies of one pulse, the optical phase is to-
tally determined by the time delay. This distinction is
further discussed by Vitanov and Knight.24) The electric
field in our case (while the pulse is on) is a plane wave
given by the real part of
E ~ t ! 5 E 0 exp@ i ~ v 0 t 1 M sin v m t !#
5 E 0 exp~ iM sin v m t ! exp~ i v 0 t ! .
The last arrangement shows the field written as a slowly
varying envelope, E(t), times the carrier,
E ~ t ! 5 E ~ t ! exp~ i v 0 t ! ,
Supplee et al.
E ~ t ! 5 E 0 exp~ iM sin v m t ! . (3)
For the FM case addressed in this paper, the envelope
E (t) describes the sinusoidal phase modulation. For
later use we note that the real and imaginary parts of
E (t) are
Re~ E ! 5 E 0 cos~ M sin v m t ! ,
Im~ E ! 5 E 0 sin~ M sin v m t ! . (4)
If this field is used in the optical Bloch equations, the
terms shown in Eqs. (4) will enter as time-dependent co-
efficients in coupled differential equations. Such equa-
tions are not always amenable to simple, closed-form
analysis for arbitrary field strength (nonlinear regime)
and arbitrary modulation index M. How tractable the
answers are depends largely on what additional assump-
tions and approximations can be applied to the circum-
stances at hand. (See, for example, Refs. 6–15.)
For a frequency-modulated beam the additional com-
plexity of treating a pulsed beam can result, perhaps
ironically, in simpler Bloch equations than the case of a
frequency-modulated continuous beam. This brings us to
the central point of this paper: If the laser pulses are
sufficiently short [Eqs. (8) and (9) below], the real and
imaginary parts of the envelope (4) will not vary signifi-
cantly during the pulse. Therefore, as elaborated below,
the optical Bloch equations that apply during the pulse
are coupled differential equations with constant coeffi-
cients (albeit different constants for each pulse). The
equations can therefore easily be solved in closed form.
During the time that the pulse is off, the field is zero and
the Bloch equations have their simple free decay solu-
tions. The solutions for ‘‘pulse off’’ and the solutions for
‘‘pulse on’’ can be joined continuously at the boundary.
The net result is that, with the short-pulse restriction, we
are able to find solutions to the optical Bloch equations for
all time. The solutions apply for arbitrary intensity and
for any modulation index that does not violate the short-
pulse restriction [Eq. (8) below].
2. THEORY AND CALCULATIONS
A. Model
How a two-level atom responds to an optical field can be
studied via the optical Bloch equations29 in the dipole ap-
proximation and the rotating-wave approximation,
u̇ 5 2b u 2 Dv 1 k Im~ E ! w,
v̇ 5 Du 2 b v 1 k Re~ E ! w,
ẇ 5 2k Im~ E ! u 2 k Re~ E ! v 2 g ~ w 1 1 ! . (5)
(1)
u and v are, respectively, the (slowly varying) in-phase
and in-quadrature parts of the atomic dipole moment; w
is the (slowly varying) atomic inversion. The 1 in the
(2) third Bloch equation arises because in this form of the
Supplee et al. Vol. 15, No. 7 / July 1998 / J. Opt. Soc. Am. B 1835

equations we assume that all atoms would be in the decay, terms involving g and b disappear. (When we
ground state (w 5 21) in the absence of an external field. treat decay in the following subsection, we will consider a
We use a frame rotating at the carrier frequency v 0 . collisionless atom and set b 5 g /2. One need not neces-
Background information is given, for example, in texts by sarily commit to that restriction here, provided the pulse
Milonni and Eberly,30 Meystre and Sargent,31 Allen and time is short compared with all decay times.) The Bloch
Eberly,32 and Shore.33 We use detuning equations further simplify because, as discussed above,
Im(E ) and Re(E ) are approximately constant for the du-
D [ v atom 2 v 0 , (6) ration of one pulse. The optical Bloch equations there-
where v 0 is the laser carrier frequency and v atom is the fore become
atomic transition energy divided by \. k is the electric
dipole moment of the transition divided by \. g is the to-
u̇ 5 2Dv 1 b n w,
tal decay rate for all decay processes connecting the upper
and lower levels; b is the dipole-moment decay rate (1 /g
is often called T 1 , or the longitudinal lifetime, and 1 /b is v̇ 5 Du 1 a n w,
often called T 2 , or the transverse lifetime).
As mentioned above, if the optical Bloch Eqs. (5) in-
volve time-dependent coefficients, the resulting coupled ẇ 5 2b n u 2 a n v,
differential equations are intractable to various degrees
depending on what other assumptions apply to the model
or
at hand. For a pulsed FM optical field, both Im( E ) and

Re( E ) are time dependent; the pulsing alone would
make Re( E ) a square wave, and the modulation affects
both the real and the imaginary parts of E via Eqs. (4).
We overcome the square-wave difficulty by using
Temkin’s34 approach; that is, we solve the Bloch Eqs. (5)
separately for the time the pulse is on and for the time the
pulse is off, then match values at the boundary. We
overcome the second difficulty, the time-dependent modu-
lation, by making use of the short-pulse requirement; for
adequately short pulses, the values of Re(E ) and Im(E )
[Eqs. (4)] will change negligibly during the time that the
pulse is on.
B. Optical Bloch Solution during the Pulse
The key simplification in our model involves noting that
the real and the imaginary parts of E, given by Eqs. (4),
will vary little during the pulse provided that the pulse
time is short enough that the argument of sine and cosine
does not vary much during the pulse. We are therefore
addressing the case where the variation of the argument
satisfies the condition
d ~ M sin v m t ! ! 2 p . (7)
This condition is satisfied provided that the pulse dura-
tion t p (which equals the variation in time d t) satisfies
2p
tp ! . (8)
Mvm
Since we are considering short pulses, it is also acceptable
to neglect atomic decay (following Temkin34) during the
time that the pulse is on, provided that the pulse is much
shorter than the atomic lifetime:
1
FG F GF G
0 2D bn
u u
d
v 5 D 0 an v . (10)
dt
w 2b n 2a n 0 w
We introduce the abbreviations
a n [ k Re@ E ~ t !# 5 x cos~ M sin v m t n ! ,
b n [ k Im@ E ~ t !# 5 x sin~ M sin v m t n ! , (11)
where x 5 k E 0 is the Rabi frequency on resonance for the
unmodulated beam. Recalling that the change in t is
negligible during the pulse, we simply replace the vari-
able t with the particular time at which the pulse of in-
terest is centered. We number the pulses, so that the
first pulse starts at t 5 0 and is centered on t p / 2; the nth
pulse is centered on t n 5 (n 2 1)t r 1 t p / 2. The net re-
sult is that a n and b n are constant, but different con-
stants for each pulse. a n and b n are, of course, not inde-
pendent since a n 2 1 b n 2 5 x 2 .
The ‘‘pulse on’’ optical Bloch Eqs. (10) are in the form
we sought: coupled differential equations with constant
coefficients. What is more, the matrix in Eqs. (10) is an
antisymmetric 3 3 3 matrix, so it has especially simple
eigenvalues, 0 and 6 iV, where V [ ( x 2 1 D 2 ) 1/2 is the
generalized Rabi frequency. This means that the trans-
formation matrix A n (below) will be orthogonal, and will
show oscillations at the familiar generalized Rabi fre-
quency. The solution to Eqs. (10) is

F G FG
tp ! . (9)
g
u~ t ! u n8
In many cases it is justified to think of Eqs. (8) and (9) as v~ t ! v n8
roughly one restriction, not two, because experimental 5 A n~ t ! , (12)
w~ t ! w n8
situations meeting condition (9) will often meet condition 1 1
(8) as well.
We now rewrite the Bloch Eqs. (5) in the simplified
form that applies during the pulse. Because we neglect where
1836 J. Opt. Soc. Am. B / Vol. 15, No. 7 / July 1998 Supplee et al.

F G
a 2n 1 ~ D 2 1 b 2n ! cos V t 2a n b n ~ 1 2 cos V t ! 2 DV sin V t 2Da n ~ 1 2 cos V t ! 1 Vb n sin V t 0
1 2a n b n ~ 1 2 cos V t ! 1 DV sin V t b 2n 1 ~D 1
2
a 2n ! cos Vt Db n ~ 1 2 cos V t ! 1 Va n sin V t 0
A n~ t ! 5 .
V 2 2Da n ~ 1 2 cos V t ! 2 Vb n sin V t Db n ~ 1 2 cos V t ! 2 Va n sin V t D 2 1 x 2 cos V t 0
0 0 0 V2
(13)

The four by four format seems superfluous here, but it 3. RESULTS

will be needed in the next subsection when we include de-
The matrices A n and B above show how the Bloch vari-
cay as an inhomogeneous term in the optical Bloch equa-
ables evolve with time. We can consider time as a con-
tions. Equations (12) and (13) give u, v, and w during
tinuous variable, and use the dummy variable t to track
the nth pulse. u n8 , v 8n , and w 8n refer to the values of u, v,
the Bloch variables’ continuous evolution. In some cases,
and w at the beginning of the nth pulse. Also, in this
however, one might just need to calculate the effect of
particular context, t refers to the time elapsed since the
complete pulses on the atom. In that case, one can use
beginning of the nth pulse.
t 5 t p in Eq. (12), and a simple matrix multiplication
propagates the Bloch variables through one complete
C. Optical Bloch Solution between Pulses (Decay)
pulse. Similarly, using t 5 t r 2 t p in Eq. (15) will
Between pulses the optical field is zero and the atom de-
propagate the Bloch variables through one ‘‘dead time’’
cays. With zero field present, and considering a collision-
between pulses. For example, if an atom starts in the
less atom with b 5 g /2, the Bloch Eqs. (5) simplify to
ground state, then at a time t after the jth pulse turns off,
the atom’s Bloch vector is given by

FG FG
g
u̇ 5 2 u 2 Dv,

F) G
2 u 0
1
v 0
5 B ~ t ! A j~ t p ! B ~ t r 2 t p ! A n~ t p ! .
g w n5j21 21
v̇ 5 Du 2 v, 1 1
2
(17)
The matrix A, which propagates the Bloch variable
ẇ 5 2g ~ w 1 1 ! . (14) through a pulse, contains a time dependence conveyed via
the subscript. This is because the pulse period and the
The solution to these equations is modulation period are different, so each pulse arrives

F G FG
when the modulation is at a different phase. Informa-
tion about the phase of the modulation at the arrival of
u~ t ! u n9
the nth pulse is conveyed through the t n by using Eqs.
v~ t ! v n9
5 B~ t ! , (15) (11) and (13). (We use t as a dummy variable to track
w~ t ! w 9n the time since the last change in the square-wave ampli-
1 1 tude envelope, but we use t to represent the total elapsed
time in the experiment.) We make no assumptions about
where whether or not the modulation period and pulse period

F G
have an integer ratio. Because each pulse is slightly dif-
ferent, it is not possible (at least in general) to find the
x cos D t 2x sin D t 0 0 steady-state behavior of the atom by finding the eigenvec-
x sin D t x cos D t 0 0 tor of BA having eigenvalue 1. With identical pulses or
B~ t ! 5 . (16) with simply commensurate periods, the eigenvalue analy-
0 0 x2 x2 2 1
sis can be helpful.26,34
0 0 0 1 Equation (17), along with the equations giving A and
B, is the main result of this paper. With Eq. (17), one
Here x [ exp(2gt /2), simply for abbreviation. The no- can study the Bloch vector behavior while varying the pa-
tation used in these pulse-off equations is parallel to that rameters of interest. There is a large parameter space to
of the previous pulse-on equations. That is, Eqs. (15) and explore, since one can vary M, v m , D, g, t r , t p , and pulse
(16) give u, v, and w during the pulse-off time between area. We give examples in Figs. 1–3.
the nth pulse and the next. u n9 , v n9 , and w n9 refer to the Figure 1 shows inversion w versus detuning for fixed
values of u, v, and w at the end of the nth pulse; that is, values of the other parameters. The results are plotted
they are the ‘‘initial’’ values for the purposes of this time after 30 complete pulse cycles and also after 50 complete
interval. In a fashion parallel to that above, the t of Eqs. pulse cycles. The similarity of the two curves shows that
(15) and (16) refers to the time elapsed since the end of the overall structure is not critically sensitive to the num-
the nth pulse. Of course Eqs. (15) and (16) simply de- ber of pulses, provided one waits long enough for tran-
scribe the decay of the atom in the absence of an optical sients to die away. Transients are gone after a number
field. of pulses greater than ;4/g t r (Ref. 34). However, it is
Supplee et al.
Fig. 1. Inversion versus detuning. M 5 0.25, v m
5 0.15 GHz, g 5 0.02 GHz, t r 5 10 ns, t p 5 0.2 ns, pulse area
is p /8. The major peaks are at zero detuning and the first opti-
cal Ramsey fringe (t r D 5 2 p ). The modulation sidebands are
clearly visible. The solid curve shows w after 30 complete cycles
(the instant the 31st pulse turns on). The dashed curve shows
w after 50 complete cycles.
Fig. 2. Inversion (after 30 complete cycles) versus modulation
frequency. M 5 0.25, D 5 0.314 GHz, g 5 0.02 GHz, t r
5 10 ns, t p 5 0.2 ns, pulse area is p /8. w remains near 21 un-
til the modulation frequency is sufficient to make one sideband
nearly resonant with the atom. This curve is very sensitive to
the number of pulses.
Fig. 3. Inversion versus time. M 5 0.25, D 5 0.314 GHz, v m
5 0.307 GHz, g 5 0.02 GHz, t r 5 10 ns, t p 5 0.2 ns, pulse area
is p /8. (Parameters correspond to a peak in Fig. 2.) The main
oscillation, period 439 ns, is the beating of the pulse-repetition
frequency with the second harmonic of the modulation frequency.
not possible to plot genuine steady-state results for this
problem, because the problem is not strictly periodic.
Figure 2 shows inversion versus modulation frequency,
with the other parameters fixed. Figure 2 (unlike Fig. 1)
is extremely sensitive to the number of pulses even after a
long time. This is because changing v m can cause sig-
nificant beating between the modulation frequency and
the pulse-repetition frequency. To illustrate the impor-
tance of this beating, we plot w(t) in Fig. 3, and we choose
the modulation frequency that corresponds to one of the
large maxima in Fig. 2. Figure 3 therefore illustrates
two interesting points. First, we see beating with a pe-
riod of 439 ns, which is the beat period between the pulse-
repetition frequency and twice the modulation frequency.
Second, Fig. 3 helps us understand the structure in Fig. 2:
It is not the case that v m 5 0.307 achieves much higher
average inversion than, say, v m 5 0.314; it is rather that
Vol. 15, No. 7 / July 1998 / J. Opt. Soc. Am. B 1837
v m 5 0.307 simply rigs the beating so that the inversion
will instantaneously be high after 30 cycles, which was
the number of cycles chosen in plotting Fig. 2.
4. CONCLUSION
The results above give the Bloch-vector behavior for a
two-level atom interacting with a frequency-modulated
pulse train. They can be used to explore parameter
space by varying M, v m , D, g, t r , t p and pulse area over
a wide range, subject only to the short-pulse restriction
given in Eqs. (8) and (9). In Figs. 1–3 we have illustrated
some of the ways that varying parameters can affect in-
version. This formalism can also be used to investigate
the potential for using frequency-modulated pulse trains
in sensitive spectroscopic measurements of transient
atomic and molecular states.
ACKNOWLEDGMENTS
This work was partially supported by the National Sci-
ence Foundation under grant DMI-9313320.
REFERENCES
1. G. C. Bjorklund, ‘‘Frequency-modulation spectroscopy: a
new method for measuring weak absorption and disper-
sion,’’ Opt. Lett. 5, 15–17 (1980); G. C. Bjorklund, ‘‘Method
and device for detecting a specific spectral feature,’’ U.S.
patent 4,297,035 (October 27, 1981).
2. J. M. Supplee, E. A. Whittaker, and W. Lenth, ‘‘Theoretical
description of frequency modulation and wavelength modu-
lation spectroscopy,’’ Appl. Opt. 33, 6294–6302 (1994), and
references therein.
3. G. C. Bjorklund, M. D. Levenson, W. Lenth, and C. Ortiz,
‘‘Frequency modulation (FM) spectroscopy: theory of line-
shapes and signal-to-noise analysis,’’ Appl. Phys. B: Photo-
phys. Laser Chem. 32, 145–152 (1983).
4. J. A. Silver, ‘‘Frequency-modulation spectroscopy for trace
species detection: theory and comparison among experi-
mental methods,’’ Appl. Opt. 31, 707–717 (1992).
5. Xiang Zhu and D. T. Cassidy, ‘‘Modulation spectroscopy
with a semiconductor diode laser by injection-current
modulation,’’ J. Opt. Soc. Am. B 14, 1945–1950 (1997).
6. G. S. Agarwal, ‘‘Frequency-modulated spectra of coherently
driven systems,’’ Phys. Rev. A 23, 1375–1381 (1981).
7. N. Nayak and G. S. Agarwal, ‘‘Absorption and fluorescence
in frequency-modulated fields under conditions of strong
modulation and saturation,’’ Phys. Rev. A 31, 3175–3182
(1985).
8. H.-R. Xia, J. I. Cirac, S. Swartz, B. Kohler, D. S. Elliott, J.
L. Hall, and P. Zoller, ‘‘Phase shifts and intensity depen-
dence in frequency-modulation spectroscopy,’’ J. Opt. Soc.
Am. B 11, 721–730 (1994).
9. W. M. Ruyten, ‘‘Magnetic and optical resonance of two-level
quantum systems in modulated fields. I. Bloch equation
approach,’’ Phys. Rev. A 42, 4226–4245 (1990).
10. M. A. Kramer, R. W. Boyd, L. W. Hillman, and C. R. Stroud,
Jr., ‘‘Propagation of modulated optical fields through
saturable-absorbing media: a general theory of modula-
tion spectroscopy,’’ J. Opt. Soc. Am. B 2, 1444–1455 (1985).
11. A. Schenzle, R. G. DeVoe, and R. G. Brewer, ‘‘Phase-
modulation laser spectroscopy,’’ Phys. Rev. A 25, 2606–
2621 (1982).
12. W. M. Ruyten, ‘‘Comment on absorption and fluorescence in
strong frequency–modulated and amplitude-modulated
fields,’’ Phys. Rev. A 39, 442–444 (1989).
13. A. V. Alekseev and N. V. Sushilov, ‘‘Analytic solutions of
Bloch and Maxwell–Bloch equations in the case of arbitrary
field amplitude and phase modulation,’’ Phys. Rev. A 46,
351–355 (1992).
1838 J. Opt. Soc. Am. B / Vol. 15, No. 7 / July 1998
14. Ping Koy Lam and C. M. Savage, ‘‘Complete atomic popu-
lation inversion using correlated sidebands,’’ Phys. Rev. A
50, 3500–3504 (1994).
15. S. Feneuille, M.-G. Schweighofer, and G. Oliver, ‘‘Response
of a two-level system to a narrow-band light excitation com-
pletely modulated in amplitude,’’ J. Phys. B 9, 2003–2009
(1976).
16. Jun Ye, Long-Sheng Ma, and J. L. Hall, ‘‘Ultrasensitive de-
tections in atomic and molecular physics: demonstration
in molecular overtone spectroscopy,’’ J. Opt. Soc. Am. B 15,
6–15 (1998).
17. K. Namjou, S. Cai, E. A. Whittaker, J. Faist, C. Gmachl, F.
Capasso, D. L. Sivco, and A. Y. Cho, ‘‘Sensitive absorption
spectroscopy with a room-temperature distributed-feedback
quantum-cascade laser,’’ Opt. Lett. 23, 219–221 (1998).
18. J. Faist, F. Capasso, C. Sirtori, D. L. Sivco, A. L. Hutchin-
son, and A. Y. Cho, Appl. Phys. Lett. 70, 2670–2672 (1997).
19. T. F. Gallagher, R. Kachru, F. Gounand, G. C. Bjorklund,
and W. Lenth, ‘‘Frequency-modulation spectroscopy with a
pulsed dye laser,’’ Opt. Lett. 7, 28–30 (1982).
20. N. H. Tran, R. Kachru, T. F. Gallagher, J. P. Watjen, and G.
C. Bjorklund, ‘‘Pulsed frequency-modulation spectroscopy
at 3302 Å,’’ Opt. Lett. 8, 157–159 (1983).
21. N. H. Tran, R. Kachru, P. Pillet, H. B. van Linden van den
Heuvell, T. F. Gallagher, and J. P. Watjen, ‘‘Frequency-
modulation spectroscopy with a pulsed dye laser: experi-
mental investigations of sensitivity and useful features,’’
Appl. Opt. 23, 1353–1360 (1984).
22. E. E. Eyler, S. Gangopadhyay, N. Melikechi, J. C. Bloch,
and R. W. Field, ‘‘Frequency-modulation spectroscopy with
transform-limited nanosecond laser pulses,’’ Opt. Lett. 21,
225–227 (1996).
23. P. Peterson and A. Gavrielides, ‘‘Periodic response of the
Supplee et al.
Bloch equations to a phase modulated pulse train; an appli-
cation to mesospheric sodium,’’ Opt. Commun. 104, 53–56
(1993).
24. N. V. Vitanov and P. L. Knight, ‘‘Coherent excitation of a
two-state system by a train of short pulses,’’ Phys. Rev. A
52, 2245–2261 (1995).
25. F. T. Hioe, ‘‘Solution of Bloch equation involving amplitude
and frequency modulations,’’ Phys. Rev. A 30, 2100–2103
(1984).
26. L. C. Bradley, ‘‘Pulse-train excitation of sodium for use as a
synthetic beacon,’’ J. Opt. Soc. Am. B 9, 1931–1944 (1992).
27. G. F. Thomas, ‘‘Excitation of a multilevel system by a train
of identical phase-coherent Gaussian-shaped laser pulses,’’
Phys. Rev. A 41, 1645–1652 (1990).
28. P. W. Milonni and L. E. Thode, ‘‘Theory of mesospheric so-
dium fluorescence excited by pulse trains,’’ Appl. Opt. 31,
785–800 (1992).
29. R. P. Feynman, F. L. Vernon, Jr., and R. W. Hellwarth,
‘‘Geometrical representation of the Schrödinger equation
for solving maser problems,’’ J. Appl. Phys. 28, 49–52
(1957).
30. P. W. Milonni and J. H. Eberly, Lasers (Wiley, New York,
1988), especially Chaps. 6 and 8.
31. P. Meystre and M. Sargent III, Elements of Quantum Op-
tics (Springer-Verlag, New York, 1990).
32. L. Allen and J. H. Eberly, Optical Resonance and Two-Level
Atoms (Dover, New York, 1987).
33. B. W. Shore, The Theory of Coherent Atomic Excitation:
Simple Atoms and Fields (Wiley, New York, 1990), Vol. 1,
especially Chap. 8.
34. R. J. Temkin, ‘‘Excitation of an atom by a train of short
pulses,’’ J. Opt. Soc. Am. B 10, 830–839 (1993).