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Journal of the Optical Society of America B

Application of chirped ultrashort pulses for generating large-amplitude ground-state vibrational coherence: a computer simulation

Sanford Ruhman, Ronnie Kosloff

Published Aug 1, 1990• 114 citations
Publisher

Abstract

Computer simulations are presented to show that frequency-chirped ultrashort pulses, when properly employed, may be more effective than their compressed analogs for generating large-amplitude vibrational coherence in molecular systems. A one-dimensional model, which was used previously to simulate impulsive optical excitation of CsI, is used [ Chem. Phys. Lett.158, 238 ( 1988)]. A negatively chirped pulse (for which the light is red-shifted with time) is devised to excite the population initially onto the excited surface. As this population propagates in the repulsive upper state, the later red-shifted portions of the pulse follow the change in the resonance conditions and effectively dump the population back down into excited vibrational states of the ground surface. These results are compared with the dynamics simulated with the compressed and positively chirped analogs, and the experimental realization of this scheme is discussed.

DOI
10.1364/josab.7.001748

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•Jan 1, 2010•0 citations
Computer simulations are presented to show that frequency-chirped ultrashort pulses, when properly employed, may be more effective than their compressed analogs for generating large-amplitude vibrational coherence in molecular systems. A one-dimensional model, which was used previously to simulate impulsive optical excitation of CsI, is used [ Chem. Phys. Lett.158, 238 ( 1988)]. A negatively chirped pulse (for which the light is red-shifted with time) is devised to excite the population initially onto the excited surface. As this population propagates in the repulsive upper state, the later red-shifted portions of the pulse follow the change in the resonance conditions and effectively dump the population back down into excited vibrational states of the ground surface. These results are compared with the dynamics simulated with the compressed and positively chirped analogs, and the experimental realization of this scheme is discussed.
Detailed theoretical analysis and numerical simulation indicate that nearly complete electronic population inversion of molecular systems can be achieved with intense positively chirped broadband laser pulses. To provide a simple physical picture, a two-level model is used to examine the condition for the so-called π pulses and a four-level model is designed to demonstrate for molecular systems the correlation between the sign of the chirp and the excited state population. The proposed molecular π pulse is the combined result of vibrational coherence in the femtosecond regime and adiabatic inversion in the picosecond regime. Numerical results for a displaced oscillator, for LiH and for I2, show that the proposed molecular π pulse scheme is robust with respect to changes in field parameters such as the linear positive chirp rate, field intensity, bandwidth, and carrier frequency, and is stable with respect to thermal and condensed phase conditions including molecular rotation, rovibronic coupling, and electronic dephasing.
This theoretical paper investigates the formation of ground state molecules from ultracold cesium atoms in a two-color scheme. Following previous work on photoassociation with chirped picosecond pulses [Luc-Koenig et al., Phys. Rev. A, 70, 033414 (2004)], we investigate stabilization by a second (dump) pulse. By appropriately choosing the dump pulse parameters and time delay with respect to the photoassociation pulse, we show that a large number of deeply bound molecules are created in the ground triplet state. We discuss (i) broad-bandwidth dump pulses which maximize the probability to form molecules while creating a broad vibrational distribution as well as (ii) narrow-bandwidth pulses populating a single vibrational ground state level, bound by $113\phantom{\rule{0.3em}{0ex}}{\mathrm{cm}}^{\ensuremath{-}1}$. The use of chirped pulses makes the two-color scheme robust, simple, and efficient.
Recent calculations [1, see also 2-5] indicate that suitably timed sequences of electronically preresonant femtosecond laser pulses can induce large amplitude coherent molecular vibrations of dilute chromophores in low temperature hosts, without undue electronic absorption or other loss processes. Here we demonstrate that frequency modulation, in the forms of variable pulse center frequency and variable chirp rate, can significantly further enhance the efficiency of impulsive stimulated Raman preparation of coherent vibrations in the electronic ground state.
We study the dynamics of two-photon nonresonant electronic excitation of diatomic molecules driven by chirped pulses. While the majority of the experimental results address the role of the chirp for fixed pulse bandwidth, we analyze the possibility of selective excitation for fixed time, as a function of the pulse bandwidth, depending on the sign of the chirp. With strong picosecond pulses and positive chirp it is shown that the dynamics always prepare the molecule in the ground vibrational level of the excited electronic state. The robustness of the dynamics inherits the properties of an effective Landau–Zener crossing. For negative chirp the final state is very sensitive to the specific pulse bandwidth. The dynamics of the system follow a complex convoluted behavior, and the final state alternates between low vibrational levels of the excited electronic state and excited vibrational levels of the ground potential, which become increasingly more excited with increasing bandwidth. The final electronic populations follow a double-period oscillatory behavior. We present a model based on sequential independent crossings which correlates the long-oscillation period with changes in the final vibrational state selected. We show that the short-oscillation period is related with nonadiabatic effects that give rise to fast dynamic Rabi flipping between the electronic states, providing only information of the field–molecule effective coupling. Although the short-oscillation period partially masks the expected results of the final populations, we show that it is still possible to retrieve information from the long-oscillation period regarding the frequencies of the electronic potentials. In order to do so, or in order to control the outcome of the dynamics, it is necessary to perform experiments scanning very different pulse bandwidths, and we propose a possible experimental implementation. All the numerical results of the paper are calculated for a model of the Na2 dimer.
Using the concept of light-induced potentials introduced by Garraway and Suominen [Phys. Rev. Lett. 80, 932 (1998)], we study alternative schemes of adiabatic population transfer in a diatomic molecule from the lowest vibrational level of the ground electronic state to the lowest vibrational level of a third electronic state via allowed optical transitions from the ground and third electronic states to a second electronic state. Our chirped-pulse rapid adiabatic passage scheme is implemented with short-duration optical pulses, and can be understood in terms of ``road design engineering'' of the light-induced time-dependent adiabatic potential upon which the dynamics occurs. We explicitly show that complete adiabatic vibronic population transfer occurs using chirped picosecond-duration pulses in the sodium dimer example.
We present results on coherent control of ultracold trap-loss collisions and molecule formation using frequency-chirped light. The chirps, either positive or negative, sweep 1 GHz in 100 ns and are red-detuned below the D2 line in either 85Rb or 87Rb. The pulses are Gaussian and have a full-width at half-maximum (FWHM) of 40 ns. In our collision experiments, we demonstrate coherent control of ultracold 85Rb collisions using nonlinear (either concave-down or concave-up) frequency chirps in the region of pulse detunings where coherent collision blocking occurs. We attribute this to the excitation radius of the negative chirp following the excited-wavepacket trajectory. We find that this process is dependent on the nonlinearity of the negative chirp. Specifically, the concave-down negative chirp yields a higher value of the collisional loss rate constant β than those of the concave-up and linear negative chirps. For nonlinear positive chirps, we find no significant dependence of β on the nonlinearity of the chirp. Our measurements are supported by quantum mechanical simulations of the collisional process. ^ In our molecule formation experiments, we use resonantly-enhanced multi- photon ionization to directly detect ground-state 87Rb 2 formed though photoassociation (PA) by linearly frequency-chirped pulses and subsequent spontaneous decay. In particular, we measure the rates of formation (R) and photodestruction (Γ PD) for positive and negative frequency-chirped pulses, as well as for unchirped pulses. We find that the unchirped pulse yields higher values of both R and ΓPD than those of the positively-chirped pulse, whose values in turn are greater than those of the negatively-chirped pulse. Our results are important steps towards coherent control of ultracold ground-state molecule formation. ^