27 November 1998

Chemical Physics Letters 297 1998. 307313

Two-dimensional electronic spectroscopy

John D. Hybl, Allison W. Albrecht, Sarah M. Gallagher Faeder, David M. Jonas

Department of Chemistry and Biochemistry, Uniersity of Colorado at Boulder, Boulder, CO 80309-0215, USA
Received 14 August 1998; in final form 31 August 1998

Abstract
Two-dimensional Fourier transform electronic spectroscopy is demonstrated. Non-collinear three-pulse scattering allows
selection of electronic coherence order by choice of phase-matching geometry, temporal pulse order, and Fourier transform
variables. Detection of the scattered field at the sample allows separation of the real absorptive and emissive. and imaginary
refractive. contributions to the 2D spectra. The experiments reported here are electronic analogs of the 2D magnetic
resonance techniques known as COSY correlated spectroscopy. and NOESY nuclear Overhauser effect spectroscopy. and
should allow detection of electronic multiple quantum coherence. q 1998 Elsevier Science B.V. All rights reserved.

1. Introduction
Despite the many differences between spin flips
and electronic excitations w1,2x, the extension of
magnetic resonance methods to optical spectroscopy
has been fruitful w36x. In magnetic resonance,
Fourier transform spectra with two frequency dimensions 2D spectra. w7,8x can resolve overlapping peaks
by spreading them out in a second dimension, correlate linked spectroscopic transitions using crosspeaks, map excitation transfer pathways and measure
rates by following the growth of new cross-peaks,
and have decisive advantages over double resonance
for the study of multiple quantum transitions. Ernst
and co-workers also suggested that 2D rotational and
vibrational spectroscopy might be useful w7x. In the
last five years, there has been some progress in
extending 2D spectroscopy beyond magnetic resonance. Tanimura and Mukamel examined 2D Raman
spectroscopy theoretically w9x. Tokmakoff et al. w10x
)

Corresponding author. E-mail: jonasd@stripe.colorado.edu

obtained 2D Raman spectra of liquids by fifth-order

femtosecond Raman spectroscopy. Lepetit and Joffre
w11x mapped the absolute value of the 2D secondorder nonlinear response of a KDP crystal. Both of
these experiments recovered difference frequencies
by Fourier transformation of the time delay between
non-collinear pulses. 1 2D electronic spectroscopy
w12x where initial absorption peaks are correlated to
subsequent absorption, emission, and refractive index changes. should be a valuable tool for probing
electronic coupling, energy transfer, electron transfer, and relaxation processes. However, 2D spectra
require recovery of the optical e.g., absorption.
frequency upon Fourier transformation of the detected signal.
While experiments using non-collinear beams can
produce amplitude modulation of the signal at differ1

For the second-order nonlinearity of doubling crystals, measurement of the sum frequency and Fourier transform recovery of
the difference frequency allows calculation of either optical frequency, but difference frequencies are not sufficient to determine
the optical frequency for third-order nonlinearities.

0009-2614r98r$ - see front matter q 1998 Elsevier Science B.V. All rights reserved.
PII: S 0 0 0 9 - 2 6 1 4 9 8 . 0 1 1 4 0 - 3

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J.D. Hybl et al.r Chemical Physics Letters 297 (1998) 307313

ence frequencies equal to the difference between

two frequencies within the pulse spectrum., they do
not produce the amplitude modulation of the signal
at optical frequencies observed using collinear beams
w13x. Non-collinear excitation pulses are desirable for
at least two reasons: 1. weak signals can be spatially isolated from stronger excitation pulses; and
2. choice of the phase-matching geometry and pulse
ordering allows selection of the electronic coherence
order set of density matrix elements. being probed
during each time interval w2x. We have encountered a
pervasive skepticism that Fourier transformation can
recover electronic frequencies from signals produced
by non-collinear pulses. The key to non-collinear
experiments lies in detecting phase modulation of
the signal at the electronic frequency. The distinction
between a phase shift and a delay is important for
understanding how this works. 2 A delay yields exactly the same waveform passing a given point at a
later time, while a phase shift moves the field oscillations relative to the pulse envelope without delaying
the pulse envelope itself. This difference becomes
readily measurable for pulses consisting of a few
optical cycles w14x. Non-collinear crossing-angle
broadening alters only the relative delay between
pulses, while phase differences between pulses remain constant both across the sample and as the
interpulse delay is varied. Detecting phase modulation of the signal at the electronic frequency requires
measurement of the signal electric field, which is
accomplished using a combination w15 x of
frequency-resolved optical gating FROG. w16x and
spectral interferometry w17x. The electronic phase
modulation produced by the first two pulses can be
stored in the position of spatial fringes in a population grating, so that a 2D spectrum can be obtained
even after electronic phase coherence is lost. 2D
electronic spectroscopy should therefore be generally
applicable to the study of electronic coupling and
relaxation processes.

Quasi-monochromatic approximations have usually been

used to treat three-pulse scattering theoretically the work by
Hartmann and co-workers w3,29x is a notable exception.. In these
approximations e.g., E r, t . s e t .cos v t y kPr .. the envelope
e t . is not retarded by propagation at the speed of light. These
approximate fields have an incorrect spatially varying phase.

2. Theory
In order to understand 2D electronic spectroscopy, it is necessary to include the phase of the
signal field. Since signal phases had not been experimentally measured, previous theoretical work on
three-pulse scattering w4,6x did not calculate the
phase. For simplicity, three-pulse scattering signals
will be discussed using a Bloch model. This is
followed by examination of the spatial storage of the
phase information at long times when spectral diffusion w4,6x eliminates frequency gratings and only
population gratings remain.
A three-pulse scattering experiment w4,6x uses
pulses with wavevectors k a , k b , and k c to generate
a signal in the direction k c q k b y k a . For a two-level
system, physical pictures based on scattering of pulse
c off a grating formed by pulses a and b are helpful.
The origin of time is chosen so that pulse c is
centered at time t s 0, and the pulse delays are
t ' t b y t a and T ' min< t a <, < t b <.. When pulses a and
b overlap in the sample, interference creates a spatially periodic intensity pattern w4,6x. The resulting
spatially periodic excitation probability acts as both
an amplitude and phase diffraction grating w18x. For
inhomogeneously broadened transitions, the spatial
population grating is gradually replaced by a joint
spatial-frequency grating when pulses a and b no
longer overlap in time w6x. The spatial-frequency
grating produces delayed echo signals and decays by
spatial diffusion and spectral diffusion.
Examination of the signal field obtained for a
two-level system in the optical Bloch limit using d
function excitation pulses provides some insight into
2D spectra. The third-order nonlinear polarization
with wave-vector k c q k b y k a is readily calculated
from the response functions given by Mukamel w19x.
A frequency-independent pr2 phase shift between
the emitted field and the source polarization, predicted by Maxwells equations, has been included.
For t G 0, the signal field is given by
E t , t , T . A exp yG t q <t < . exp w yTrT1 x
=cos veg t y t . x t y t . ,

1.

where veg is the electronic transition frequency, G

is the dipole decay rate, T1 is the population grating

J.D. Hybl et al.r Chemical Physics Letters 297 (1998) 307313

lifetime, and x is the Fourier transform of the

inhomogeneous lineshape. No signal is emitted before t s 0. The delay between the first two pulses
encodes the electronic frequency onto the phase of
the emitted field referenced to t s 0.. In the absence
of inhomogeneous broadening, inverse Fourier transformation 3 of the emitted field as a function of t
over the interval y` to `. and t from y` to `.
for fixed T yields a 2D spectrum with two electronic
frequency dimensions
S v t , vt .
s

G 2 q i G v t q veg .
2
2
v t q veg . q G 2 vt y veg . q G 2

G 2 q i G v t y veg .
2
2
v t y veg . q G 2 vt q veg . q G 2

2.
This complex 2D single quantum spectrum has real
2D absorption lineshapes peaked at v t s yvt s
"veg and imaginary dispersion lineshapes along
v t . Inhomogeneous broadening yields a convolution with the 2D inhomogeneous lineshape
x v t y vt . r'2 . d v t q vt . r'2 . , which broadens the signal along the diagonal line v t s yvt but
not perpendicular to the diagonal.
Storage of the electronic frequency dependent
phase in a population grating can be illuminated by
considering interference between monochromatic
plane waves. Crossing waves produce a spatial intensity grating
I r . s 2 I 1 q cos k a y k b . P r y vt

.,

3.

where I is the intensity of a single beam, v is the

frequency, and t is the delay produced by pathlength
differences. As t increases, the grating maxima move
continuously along the direction k a y k b , and vt
can be regarded as the phase of the grating. For
broadband pulses, the absorbed frequencies produce

3
This definition of the Fourier transform matches Ref. w15x and
seems to be most common in optical spectroscopy e.g., Ref. w2x..
Unfortunately, the sign of i is reversed from Ref. w8x, requiring
complex conjugation before comparison with most work on 2D
NMR.

309

a population grating with phase veg t . This phase

modulation of the population grating translates directly into the phase modulation of the scattered
signal field in Eq. 1..
Since t defines the time interval over which the
experiment is sensitive to single quantum electronic
coherence between the ground and excited states,
choice of t as the second Fourier transform time
variable produces a 2D electronic spectrum. Scanning through t s 0 avoids transformation of truncated signals and produces real. absorption spectra
in the indirectly detected vt . dimension. If the
ground and excited electronic state Hamiltonians
commute and the Condon approximation is made,
peaks in the 2D spectrum are centered on the diagonal vt s yv t . However, different ground and excited electronic state potential surfaces are common
so that the two Hamiltonians may not commute.
Electronic transitions can then peak off the diagonal
at < vt < G < v t < after vibrational and solvent relaxation
on the excited state have lowered the emission frequency Stokes shift.. 4
It is also possible to simultaneously scan the delay
of pulses a and b and Fourier transform the signal
with respect to T, when the experiment is sensitive
to vibrational motion and electronic population decay. This produces a 2D spectrum of electronic
frequency vs. Raman frequency. Raman coherence
may be classifiable as zero quantum coherence since
equal phase shifts of the preparation pulses a and b
cancel w21x.
In degenerate four-wave mixing, only frequencies
within the pulse bandwidth can scatter off the grating
and be detected in the signal. The directly detected
dimension of the 2D spectrum is thus filtered by the
excitation pulse spectrum. Similar filtering occurs in
the indirectly detected frequency dimension when
only one pulse delay is scanned. When two pulse
delays are scanned simultaneously, peaks can appear
in the 2D spectrum at either sums of frequencies
within the pulse spectrum or at differences between

Since peaks with unusual indirectly detected frequencies are

observed under some circumstances in 2D NMR w20x it is conceivable that unexpected indirectly detected frequencies might appear
in 2D electronic spectra.

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J.D. Hybl et al.r Chemical Physics Letters 297 (1998) 307313

frequencies within the pulse spectrum, depending on

the phase-matching geometry.

3. Experiment
Three-pulse scattering signals w4x were generated
by pulses from a 10 kHz cavity dumped mode-locked
Ti:sapphire laser. Prisms pre-compensated for dispersion in the five-beam interferometer w15x. Excitation
pulses had a 41 nm wide spectrum centered at 797
nm and a 29 fs pulse duration determined by
second-harmonic FROG w16x. Beams a, b, and c
; 270 pJrpulse. were aligned to three corners of a
square and focused to a 40 mm spot in the sample to
generate a four-wave mixing signal with wave-vector
k s s k c q k b y k a on the fourth corner w15x. After
collimation, the signal was spatially combined with a
temporally non-overlapping reference at a beamsplitter and imaged into a spectrograph with a CCD array
which measured the spectral interferogram w17,22,23x.
This spectral interferogram determined the signal
field amplitude e v . and the phase difference
D f v . between the signal and reference at the
beamsplitter. Characterization of a tracer beam focused into the sample along the path of signal emission k t s k s . and measurement of the tracer-reference phase difference by spectral interferometry determined the signal amplitude and phase at the sample exit w15x.
A 0.4 mM solution of IR144 in methanol w24x
flowed at 2 mrs through a 100 mm pathlength
sample cell nominal OD f 0.15.. The experimental
conditions reproduced previous three-pulse echo peak
shift results w25x, yielded signal fields linear in each
excitation field, and produced signal spectra and
phases which are independent of pulse energy. To
reference the phase to t s 0, the delay of pulse c and
the tracer were fixed at t s 0 while the delays for
pulses a and b were scanned in 0.66 fs steps so as to
vary only t or only T. At each delay, a spectral
interferogram was recorded using 0.11 s CCD exposures, depending on T. Recording 601 spectral
interferograms as t was scanned from y200 to
q200 fs for a 2D electronic spectrum took a total of
315 min. After recovery of the signal field in the
frequency domain at each delay w15x, the data were

inverse Fourier transformed with respect to delay at

each frequency to produce a 2D spectrum. The translation stages which delayed pulses a and b were
calibrated by spectral interferometry. These calibrations uncovered periodic errors that transformed into
reproducible ghost peaks w26x in the vt dimension,
random errors that transformed into a roughly constant magnitude noise background ; 8% of peak.,
and reproducible local variations in the average stepsize which can cause ; 2% errors in vt if uncompensated. To check for scattered light artifacts, 2D
spectra were recorded with each excitation beam
blocked in turn: such spectra did not produce peaks
above the random noise level. Because differences in
fused silica beamsplitter, compensating block, or
lens thickness add a phase shift of ; p radr30 mm
w14x, the 2D spectra were phased multiplied by
expi u . with u chosen to produce a real and positive
absorption lineshape on one vt f yveg slice. w7x in

Fig. 1. 2D power spectrum square of the inverse Fourier transform with respect to t and T . of a transient grating scan t s 0.
extending to the Nyquist frequency of the indirectly detected
dimension v T .. The directly detected dimension v t . extends
from 1.994 to 2.750 radrfs spectrograph bandwidth. and is
filtered by the excitation pulse spectra. This scan is sensitive to
population relaxation and vibrational coherence within each electronic state, but not sensitive to electronic coherence. This 2D
spectrum represents an electronic v t . Raman v T . correlation
spectrum. Contours are at 10%, 50%, and 90% of the maximum.

J.D. Hybl et al.r Chemical Physics Letters 297 (1998) 307313

311

order to separate the real and imaginary parts of the

2D spectrum.

4. Results
Fig. 1 shows the 2D power spectrum of a transient grating experiment T scanned at fixed t s 0,
Fourier transformations with respect to t and T ..
During T, the experiment is sensitive to population
dynamics and vibrational wavepacket motion on each
electronic surface, but is blind to single quantum
electronic coherence. The resulting 2D spectrum
peaks around zero frequency in the indirectly detected dimension v T .. Fig. 2 shows the 2D power
spectrum of a three-pulse echo experiment t scanned
at T s 0, Fourier transformations with respect to t
and t .. During t , the experiment is sensitive to
single quantum electronic coherence, and the resulting 2D spectrum is peaked on or near the diagonal at
v t f yvt f 2.34 radrfs see Fig. 3..
Fig. 3 shows the real absorptiveremissive. and
imaginary dispersive. parts of the 2D spectrum obFig. 3. Real top. and imaginary bottom. parts of the 2D spectrum of a three-pulse echo scan with T s 0. The real part represents signal caused by changes in absorption and stimulated
emission. Contours are at 20%, 30%, 40%, 50% bold., 60%,
70%, 80%, and 90% of the maximum. The imaginary part represents signal caused by refractive index changes. Contours are
drawn at "30%, "40%, "50% bold., "60%, and "70% of
the absorptive real. maximum. Dotted contours indicate negative
values and solid contours indicate positive values. The half-maximum contour of the 2D absorption signal is overlaid as a dashed
curve. The interferometric stage calibration was not in register
with the scan so the indirectly detected frequencies vt . have
error bars of ; 0.04 radrfs. The 2D absorption peak is elongated
along the diagonal, suggesting the presence of inhomogeneous
broadening.

Fig. 2. 2D excitation vs. scattering. electronic spectrum of IR144

in methanol. 2D power spectrum with respect to t and t . of a
three-pulse echo scan T s 0. extending to the Nyquist frequency
in the indirectly detected dimension vt .. The only peak occurs at
y vt f v t f veg in agreement with Eq. 2.. The contours are at
10%, 50%, and 90% of the maximum.

tained at T s 0. The 2D absorption is elongated

roughly along the diagonal. The Bloch theory suggests this elongation indicates partial inhomogeneous
broadening on the timescale of the excitation pulses.
For each vt , the dispersion lineshape as a function
of v t . matches the expected 2D absorptiondispersion relation w8x when spectral filtering is taken into
account. Preliminary results indicate a transition to
nearly homogeneous 2D spectra as T is increased, as

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J.D. Hybl et al.r Chemical Physics Letters 297 (1998) 307313

Fig. 4. 2D power spectrum with respect to t and t . of a

three-pulse echo scan with T s100 ps. The contour interval is
10%. Interferometric stage calibrations which are in register with
the scan yield errors in vt of ; 0.01 radrfs and exhibit an
asymmetrical tail extending to smaller < vt < upon Fourier transformation, suggesting the asymmetrical tail in the 2D spectrum is a
translation stage artifact. The displacement of the maximum off
the diagonal vt ) v t . by ; 0.04 radrfs may represent a Stokes
shift. Note that the signal spectrum is also red-shifted 0.04 radrfs
in the directly detected dimension v t . compared to the signal
spectrum at T s 0.

expected from three-pulse echo peak shift measurements w25x.

At T s 100 ps the 2D spectrum still exhibits only
a single peak near the diagonal. The 2D power
spectrum is shown in Fig. 4. Correction for local
translation stage errors yields estimated errors in vt
of ; 0.01 radrfs. The 2D spectrum has a greater
width in the directly detected v t dimension than at
T s 0 and is red-shifted in v t . The increased spectral
width and red-shift in the scattered light probably
arise from superposing scattering from the ground
state grating and Stokes shifted scattering from the
excited state grating.

5. Discussion
Electric field detection should allow direct transposition of 2D NMR techniques to electronic and
infrared. spectroscopy. Transitions with a common
initial or intermediate level will produce cross-peaks
at T s 0, analogous to correlation spectroscopy
COSY 2D NMR. w8x. The diagonal 2D absorption at

T s 0 results from the limited homogeneous width of

this correlation. Energy transfer and electron transfer
would then produce cross-peaks which grow with T,
similar to nuclear Overhauser effect spectroscopy
NOESY 2D NMR. w8x. The red-shift at T s 100 ps
suggests that 2D cross-peaks can be generated by
relaxation but may not be symmetrical about the
diagonal. Although the 2D spectra shown here involve a single electronic transition, the changing
peakshapes demonstrate the growth of ibronic
cross-peaks. Detection of weak electronic cross-peaks
will require compensation or simultaneous calibration of translation stage errors which should eliminate ghosts, increase the signal to noise, and yield
more accurate vt frequencies. and consideration of
the transient grating phase-matching bandwidth
w27,28x. Other new capabilities include probing electronic dephasing between singly excited states during
the T period.
The analog of multiple quantum NMR, which
would shift spectra of transitions between singly
excited states and doubly excited states to the sum of
the two transition frequencies in the indirectly detected dimension, should be very powerful. Combining field detection with three-level echo w29x and
two-photon interferometry w30x methods could yield
double quantum 2D electronic spectra. Independently
of our work w12x, Mukamel and co-workers w31x have
developed a theoretical treatment of the role of coupling between chromophores in the 2D electronic
spectra of aggregates and 2D vibrational spectroscopy.

6. Conclusions
Although the experiments reported here are in
some respects preliminary, there is sufficient agreement between the data and models of the 2D spectra
to confirm the basic theory. A non-collinear geometry is possible for 2D electronic spectroscopy if the
signal field is measured so that phase modulation at
the initial absorption frequency can be used to correlate excitation and scattering frequencies. This phase
modulation is stored in the robust position of population grating maxima. A non-collinear geometry can
probe a selected electronic coherence order w8x or

J.D. Hybl et al.r Chemical Physics Letters 297 (1998) 307313

set of density matrix pathways. w2x, effectively substituting for the phase cycling procedures used in
NMR w8x. 2D studies of excitonic coupling and
energy transfer in aggregates are feasible with available femtosecond lasers. The prospect of following
electrons with extremely broadband 2D or 3D. 5
electronic spectroscopy is tantalizing.

Acknowledgements
We thank Arthur Pardi and Warren Warren for
helpful discussions of 2D NMR. This work was
supported by the Petroleum Research Fund administered by the American Chemical Society, the Camille
and Henry Dreyfus Foundation, the David and Lucile
Packard Foundation, and the National Science Foundation.

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