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Chemical Physics Letters

A numerical study on vibronic and vibrational dynamics generated by chirped laser pulses in the presence of relaxation processes

K. Mishima, Michitoshi Hayashi, J. Lin, Koichi Yamashita, S. H. Lin

Published Aug 1, 1999• 14 citations
Publisher
DOI
10.1016/s0009-2614(99)00669-7

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Changes in the modulus and phase of a slowly varying envelope of an ultrashort pulse are calculated for the case of propagation across a saturable absorber. Vibronic relaxation of the optical transition in the absorber is allowed for. A study is made of the dependences of the duration of a pulse transmitted by a nonlinear absorber on the vibrational relaxation time of dye molecules and on the detuning of the carrier frequency of a pulse relative to the maximum of the equilibrium absorption spectrum. It is shown that a chirp appears even in the absence of such detuning provided the energy of lf quanta of optically active vibrations is comparable with the thermal excitation energy. This chirp originates from partial completion of the vibrational relaxation process during a pulse, so that absorption and refraction occur in a system which is not in a vibrational equilibrium.
We discuss a novel method to create maximum coherence in a two-level system that is selectively excited among many having similar frequencies by making use of two specifically chirped pulses in the Raman configuration. The feasibility of the method is analyzed in the presence of decoherence caused by vibrational energy relaxation and collisional dephasing. It has been demonstrated that a high value of coherence may be sustained by the implementation of two chirped pulse trains prepared in accordance with the proposed method and having the same period as the vibrational energy relaxation time. Maximum coherence between predetermined states in atoms and molecules is an important aspect of many problems in quantum optics. One possible example is the generation of optimal CARS signal in the CARS microscopy aiming to reveal structures constituted of particular molecular groups. Presently, in experiments on biological imaging, the CARS signal is generated with implementation of picosecond laser pulses (1), a narrow spectral bandwidth of which allows one to address a particular molecular group with a good accuracy. Aiming to improve chemical sensitivity and to get optimal CARS signal for given pulse intensity we propose to use the quantum control methods for selective excitation of required vibrations in complex molecular systems. We developed a novel method that allows one to achieve maximum coherence in a predetermined vibrational mode in a multimode mole- cular system via the Raman transitions induced by the pump and Stokes chirped pulses. According to the Maxwell-Bloch equations, maximum coherence is the condition for the CARS signal to acquire the highest intensity upon propagation through a molecular medium (2). The mechanism of creation of maximum coherence underlying the proposed method is based on the adiabatic passage. An important aspect in the investigations asso- ciated with a condense phase is decoherence. Two main sources of decoherence, the vibrational energy relaxa- tion and collisional dephasing, may significantly affect the CARS signal intensity. The phase control of molecular processes in the presence of collisions was
In this paper, we investigate coherent control of nonadiabatic dynamics at a conical intersection (CI) using engineered ultrafast laser pulses. Within a model vibronic system, we tailor pulse chirp and temporal profile and compute the resulting wave-packet population and coherence dynamics using projections along the reaction coordinate. This approach allows us to resolve the detailed evolution of wave-packets as they traverse the degeneracy region with strong nonadiabatic coupling. By systematically varying pulse parameters, we demonstrate that both chirp and pulse duration modulate vibrational coherence and alter branching between competing pathways, leading to controlled changes in quantum yield. Our results elucidate the dynamical mechanisms underlying pulse-shaped control near conical intersections and establish a general framework for manipulating ultrafast nonadiabatic processes.