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Physical Review A

Selection rules for angular momentum transfer via impulsive stimulated Raman scattering

Takuya Higuchi, Hiroharu Tamaru, Makoto Kuwata‐Gonokami

Published Jan 9, 2013• 11 citations
Publisher

Abstract

Impulsive stimulated Raman scattering (ISRS) plays a key role in coherent control of low-energy rotational resonances. Femtosecond laser pulses are widely employed to utilize ISRS because they are broadband and can cover the needed frequencies in a single pulse. Here, we show theoretically that the ISRS process is expressed as a linear response to the instantaneous Stokes parameters (ISPs) of the laser pulse. These IPSs expressed in rotational coordinates are then shown to be responsible for the angular momentum transfer from light to matter. These relationships have led to the designs of spectral profiles and polarization states of light pulses that should selectively excite particular rotational modes.

DOI
10.1103/physreva.87.013808

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Impulsive stimulated Raman scattering (ISRS) plays a key role in coherent control of low-energy rotational resonances. Femtosecond laser pulses are widely employed to utilize ISRS because they are broadband and can cover the needed frequencies in a single pulse. Here, we show theoretically that the ISRS process is expressed as a linear response to the instantaneous Stokes parameters (ISPs) of the laser pulse. These IPSs expressed in rotational coordinates are then shown to be responsible for the angular momentum transfer from light to matter. These relationships have led to the designs of spectral profiles and polarization states of light pulses that should selectively excite particular rotational modes.
Abstract The interaction between ultrashort light pulses and non-absorbing materials is dominated by impulsive stimulated Raman scattering (ISRS). The description of ISRS in the context of pump&probe experiments is based on effective classical models describing the interaction between the phonon and pulsed electromagnetic fields. Here we report a theoretical description of ISRS where we do not make any semi-classical approximation and we treat both photonic and phononic degrees of freedom at the quantum level. The results of the quantum model are compared with semiclassical results and validated by means of spectrally resolved pump&probe measurements on α-quartz.
Multiphoton transitions can be manipulated by tailoring the ultrashort laser pulse. In this paper, we propose two schemes for achieving precise control of the selective excitation between two excited states in stimulated Raman-scattering process. We theoretically demonstrate that by properly designing the spectral phase distribution, the stimulated Raman transition probability for one excited state is kept at zero or a maximal value, while that for the other excited state can be continuously tuned over a wide range. Furthermore, the influence of the spectral bandwidth on the tunable range by the two schemes is discussed. We conclude that these schemes have significant application to the selective excitation of femtosecond coherent anti-Stokes Raman scattering.
Transient stimulated rotational Raman scattering induced by a polarization-modulated femtosecond pulse whose polarization varies with time is reported. The peak intensity of the polarization-modulated pulse produced in this study is low compared to that of a pulse without polarization variation, and this leads to the low efficiency of self-phase-modulation and thus the high efficiency of stimulated Raman scattering compared to the case of a pump pulse without polarization modulation. The scattering process is unique in terms of the high peak ratio of the anti-Stokes to Stokes emissions compared to the ratio in the case of the scattering induced by linearly, circularly, and elliptically polarized pump pulses. Under optimum conditions, the ratio approaches 1, which is not realized in the general case of stimulated rotational Raman scattering.
We introduce a theoretical framework to describe the interaction of an electromagnetic radiation field and a molecular system, such as a single molecule or a molecular crystal. By knowing in advance which electronic transitions are in resonance with the frequencies of the incident radiation, we propose a procedure to reduce the full problem to a description in terms of an effective Hamiltonian that fully takes into account the vibrational (nuclear) degrees of freedom, but that explicitly involves only those electronic states that meet the resonance condition. The influence of the rest of the electronic states appears as the polarizability of the system. We keep only those terms that give rise to Raman scattering but the scheme allows for a systematic inclusion of higher-order multiphoton processes. The resulting effective Hamiltonian is used to study the interaction of ultrashort laser pulses with a single molecule and with a molecular crystal. As applications, we study the interaction of a single ultrashort nonresonant pulse, and a train of such pulses, with a single molecule; we show that via Raman scattering the pulse impulsively transfers momentum to the molecule leaving it in a vibrational coherent state. We also study the interaction of two crossed laser pulses with a molecular crystal and show that a diffraction grating of lattice vibrations is impulsively created.
We investigated the coherent phonon generation mechanism by irradiation of an ultrashort pulse with a simple two-level model. Our derived formulation shows that both impulsive stimulated Raman scattering (ISRS) and impulsive absorption (IA) simultaneously occur, and phonon wave packets are generated in the electronic ground and excited states by ISRS and IA, respectively. We identify the dominant process from the amplitude of the phonon oscillation. For short pulse widths, ISRS is very small and becomes larger as the pulse width increases. We also show that the initial phase is dependent on the pulse width and the detuning.