Femtosecond wave-packet dynamics in cesium dimers studied through controlled stimulated emission Page: 1
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PHYSICAL REVIEW A 81, 053405 (2010)
Femtosecond wave-packet dynamics in cesium dimers studied through
controlled stimulated emission
Luqi Yuan,' Gombojav O. Ariunbold,1'2 Robert K. Murawski,3 Dmitry Pestov,4 Xi Wang,' Anil K. Patnaik,l,*
Vladimir A. Sautenkov,1'5 Alexei V. Sokolov,' Yuri V. Rostovtsev,6 and Marlan O. Scullyl'7'8
'Institute for Quantum Studies and Physics Department, Texas A&M University, College Station, Texas 77843, USA
2Department of Physics, National University of Mongolia, Ulaanbatar 210646, Mongolia
3Department of Physics, Drew University, Madison, New Jersey 07940, USA
4Department of Chemistry, Michigan State University, East Lansing, Michigan 48824, USA
5P. N. Lebedev Institute of Physics, 53 Leninsky prospect, Moscow 119991, Russia
6Department of Physics, University of North Texas, Denton, Texas 76203, USA
7Applied Physics and Materials Science Group, Eng. Quad., Princeton University, Princeton, New Jersey 08544, USA
8Max-Planck-Institute fur Quantenoptik, D-85748 Garching, Germany
(Received 3 March 2010; published 12 May 2010)
We study the dynamics of wave packets in cesium dimers using a femtosecond-controlled pump-probe
technique. We implement configurations with one pulse (pump) or two pulses (pump and control) to produce
vibrational wave packets on the electronic excited state. The transmission of an additional, variable-delay probe
pulse is measured to monitor the time evolution of the wave packets. In the case of the pump-control-probe
configuration, a superposition of two independent wave packets is observed. In order to elucidate the observed
experimental data, we develop a theory based on the Liouville equation for the density matrix associated with
the Franck-Condon factors. Both the numerical and analytical calculations are in good agreement with our
experimental results.DOI: 10.1103/PhysRevA.81.053405
I. INTRODUCTION
Femtosecond dynamics of vibrational and rotational wave
packets of dissociating molecular fragments in chemical
reactions was first reported in Ref. [1]. Since then, the wave
packet generation and evolution have been demonstrated and
thoroughly studied for a number of diatomic molecules,
including I2 [2,3], Na2 [4,5], Li2 [6,7], and many others [8,9].
Besides these successful research works, the two-color, pump-
probe laser experiment has been performed in Refs. [10-12].
The experiments with ~100-fs pulses have been used to
investigate the dynamics of vibrational wave packets in C 1 n,,
B '1 ,, and D 'H electronic excited states in cesium dimers.
In order to study the wave-packet dynamics in the B1 'H
state in Ref. [12], the wave packets have been produced by
exciting the Cs2 dimer with a pump pulse from the X 'E+
ground state to the target state and then photoionizing them
into Cs2 (X) state with a time-delayed probe pulse. All
those experiments have been carried out with a single pair
of pump-probe pulses. It has been shown elsewhere that
one can control the wave-packet dynamics using a sequence
of pump, control, and probe fields [13-16]. In experiments
with copropagating pump and control pulses, wave packets
were shown to interfere coherently throughout an extended
sample [17,18].
Wave-packet dynamics has also been explored theoretically
[19]. Density matrix formalism [20] has been adopted to
describe the observables in the femtosecond pump-probe
experiments [21-24]. Franck-Condon factors are related to the
overlap integrals between vibrational wave functions and give
*Current Address: Air Force Research Laboratory, Wright-Patterson
AFB, OH 45433.PACS number(s): 33.80.-b, 82.53.Hn, 42.50.-p
rise the relative transition probabilities [25]. They have been
used in Refs. [11,12,26] to explain their experimental results.
However, a theory associated with the Liouville-von Neumann
equation for the density matrix with the Franck-Condon factors
has not yet been developed in detail for some generalized
experimental conditions.
In this work, we present an all-optical alternative to
the conventional photoionizing detection scheme [10-12] to
monitor the femtosecond wave-packet dynamics. Namely the
A-type configuration for energy levels is considered. That is,
after the pump pulse creates the wave packet in the excited
electronic state, the probe pulse stimulates this excitation
down to some vibrational levels in the ground state. We use
this method to visualize wave-packet time evolution in B ' H,
state in Cs2, as is reported briefly in Ref. [27]. Furthermore,
we extend it to pump-control-probe case by adding a control
pulse. Instead of collinear setup as in Refs. [17,18], we use
noncollinear beam geometry in both femtosecond pump-probe
and pump-control-probe experiments. It does not require
subfemtosecond stabilization of the time delay between pump
and control pulses and allows for straightforward spatial
filtering of the probe beam. To explain the observed results,
we develop a detailed theoretical model based on the time-
dependent density matrix equations with the Franck-Condon
factors. Both numerical simulations and analytical calculations
for transmission of probe pulse are presented. These results are
compared with experimental data.
The organization of the article is as follows. The pump-
probe and pump-control-probe experimental setup is discussed
in Sec. II. In Sec. III, a theoretical model based on A-type
system is presented and an analytical solution is obtained for
the absorption of the femtosecond probe pulse assuming the
pump and control excitations are independent of each other.
The experimental and corresponding theoretical results on the2010 The American Physical Society
1050-2947/2010/81(5)/053405(8)
053405-1
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Yuan, Luqi; Ariunbold, Gombojav O.; Murawski, Robert K.; Pestov, Dmitry; Wang, Xi; Patnaik, Anil K. et al. Femtosecond wave-packet dynamics in cesium dimers studied through controlled stimulated emission, article, May 12, 2010; [College Park, Maryland]. (https://digital.library.unt.edu/ark:/67531/metadc103267/m1/1/?q=%22Ariunbold%2C+Gombojav+O.%22: accessed July 17, 2024), University of North Texas Libraries, UNT Digital Library, https://digital.library.unt.edu; crediting UNT College of Arts and Sciences.