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Research in Optical Sciences

Control of quantum fluctuation of atomic displacements by femtosecond laser pulses

Jianbo Hu, O. V. Misochko, Kazutaka G. Nakamura

Published Jan 1, 2012• 0 citations
Publisher

Abstract

By employing a two pump- one probe technique, we have realized coherent control of quantum fluctuation of atomic displacements via exciting two-phonon bound states generated by off-resonant impulsive stimulated second-order Raman scattering.
DOI
10.1364/hilas.2012.jt2a.33

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Two-phonon bound states have been excited exclusively in ZnTe(110) via impulsive stimulated second-order Raman scattering, essentially being squeezed states due to phase coherent excitation of two identical components anticorrelated in the wave vector. By using coherent control technique with a pair of femtosecond laser pulses, the manipulation of squeezed states has been demonstrated in which both the amplitude and lifetime of coherent oscillations of squeezed states are modulated, indicating the feasibility to control the quantum noise and the quantum nature of phonon squeezed states, respectively.
Efficient excitation of an ensemble of atoms and molecules to a desired state is of fundamental importance not only for spectroscopy but also for quantum control of molecular dynamics in chemical and biological processes. The latter usually occurs on a much shorter time scale (in the femtosecond range) giving rise to steadily advanced problem how to excite one of the nearby levels, even when they are well within the broad fs pulse spectrum. We propose a new effective method for selective excitation of atoms based on the atomic coherence and discuss a sensitive method to verify experimentally the proposed mechanism using the technique of quantum beating in pump-probe experiments.
Resonant and near-resonant two-photon excitations with ultrashort laser pulses of forbidden atomic transitions give access to a wide class of nonlinear-optical processes such as two-photon absorption, stimulated Raman scattering, four-wave sum- and difference-frequency mixing. The latter has proofed to be a powerful tool for efficient femtosecond pulse generation in the VUV-spectral range [1]. Nevertheless, up to now only few experimental results have been obtained which allow the direct observation of the coherent dynamics in two-photon induced radiation-matter interactions (see experimental papers [2-5] and monograph [6]).
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.