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Characterization of transient molecular vibrations on the way towards coherently controlled vibrational target state

Stanislav O. Konorov, Xiaoji G. Xu, John W. Hepburn +1 more

Bulletin of the American Physical SocietyMay 20, 20090 citations

Role of coherent effects in the excitation of high vibrational molecular levels

А. Н. Ораевский, A. A. Stepanov, Vladimir A. Shcheglov

Journal of Experimental and Theoretical PhysicsDec 1, 19751 citation

Possibility of coherent excitation of molecular vibrations in a resonance light field

Alexei D. Kiselev

Optics and SpectroscopyJul 1, 19900 citations

Control of excited-state population and vibrational coherence with shaped-resonant and near-resonant excitation

Tiago Buckup, Jürgen Hauer, Carles Serrat +1 more

We investigated numerically and experimentally the enhancement of vibrational coherence and population transfer in solution using tailored pulses. The general control mechanism is based on the precise control of the absorption after excitation with multipulses. Transient absorption was used as an experimental method to quantify the enhancement after the excitation with a shaped pump pulse in the low-pulse energy regime. A density-matrix approach was used to investigate the effect of the shaped excitation of a four-level system (two ground-state vibrational levels + two excited-state vibrational levels). Density-matrix simulation results suggest similar wavelength dependence as observed in the transient absorption experiment. The results show that enhancement of population transfer and vibrational coherence depends crucially on the overlap between the excitation pulse spectrum and the molecular absorption band.We investigated numerically and experimentally the enhancement of vibrational coherence and population transfer in solution using tailored pulses. The general control mechanism is based on the precise control of the absorption after excitation with multipulses. Transient absorption was used as an experimental method to quantify the enhancement after the excitation with a shaped pump pulse in the low-pulse energy regime. A density-matrix approach was used to investigate the effect of the shaped excitation of a four-level system (two ground-state vibrational levels + two excited-state vibrational levels). Density-matrix simulation results suggest similar wavelength dependence as observed in the transient absorption experiment. The results show that enhancement of population transfer and vibrational coherence depends crucially on the overlap between the excitation pulse spectrum and the molecular absorption band.

Journal of Physics B Atomic Molecular and Optical PhysicsMar 26, 200834 citations

Coherent control of the molecular dynamics in a liquid by femtosecond four-pulse excitation

Victor G. Nikiforov, Vladimir S. Lobkov, В. В. Самарцев +1 more

© 2015 Astro Ltd. The laser non-resonant excitation based on the (2 ×2) sequence of the two pairs of the pump pulses with orthogonal linear polarizations is proposed and theoretically considered for the control of the vibrational responses without or with the low amplitude of the rotational responses in a liquid. As an example, we model the optical molecular responses resulting in the optical Kerr effect transients in ortho-dichlorobenzene. Theoretical analysis shows the high efficiency of the (2 ×2) excitation scenarios for the various manipulations of the molecular responses.© 2015 Astro Ltd. The laser non-resonant excitation based on the (2 ×2) sequence of the two pairs of the pump pulses with orthogonal linear polarizations is proposed and theoretically considered for the control of the vibrational responses without or with the low amplitude of the rotational responses in a liquid. As an example, we model the optical molecular responses resulting in the optical Kerr effect transients in ortho-dichlorobenzene. Theoretical analysis shows the high efficiency of the (2 ×2) excitation scenarios for the various manipulations of the molecular responses.

Laser PhysicsDec 15, 20141 citation

Phase coherence control and subcycle transient detection in nonlinear Raman scattering with ultrashort laser pulses

Aleksei M. Zheltikov

A model of two-level weakly interacting quantum systems is used to demonstrate that the phase of molecular vibrations excited through stimulated Raman scattering can be controlled by the relative phase of time-separated laser pulses, allowing synchronization and amplitude control of coherence excitation in a medium. For transients with a phase relaxation time less than the field cycle, the field half-cycle can serve as a subfemtosecond probe of coherent vibrations. In this regime, the high-frequency field-induced modulation of molecular dipole moments gives rise to a detectable modulation of the optical response of a medium at the frequency $2\ensuremath{\omega}$, $\ensuremath{\omega}$ being the frequency of the laser field.A model of two-level weakly interacting quantum systems is used to demonstrate that the phase of molecular vibrations excited through stimulated Raman scattering can be controlled by the relative phase of time-separated laser pulses, allowing synchronization and amplitude control of coherence excitation in a medium. For transients with a phase relaxation time less than the field cycle, the field half-cycle can serve as a subfemtosecond probe of coherent vibrations. In this regime, the high-frequency field-induced modulation of molecular dipole moments gives rise to a detectable modulation of the optical response of a medium at the frequency $2\ensuremath{\omega}$, $\ensuremath{\omega}$ being the frequency of the laser field.

Physical Review ANov 3, 200621 citations

Saturation and transient effects in coherently excited molecular vibrations

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