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arXiv:quant-ph/0312175 · Physical Review Letters

Control of Raman Lasing in the Nonimpulsive Regime

Brett J. Pearson, P. H. Bucksbaum

Published Jun 18, 2004• 25 citations
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Abstract

We explore coherent control of stimulated Raman scattering in the nonimpulsive regime. Optical pulse shaping of the coherent pump field leads to control over the stimulated Raman output. A model of the control mechanism is investigated.
DOI
10.1103/physrevlett.92.243003

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Recent adaptive feedback control experiments demonstrated control of transient (i.e. nonimpulsive) Stokes emission from two closely spaced Raman-active modes in liquid methanol [e.g., B. J. Pearson et al., Phys. Rev. A 63, 063412 (2001)]. Optimally shaped pulses were found that selectively excited one of the two Stokes lines alone, optimized emission from both modes together, or completely suppressed all Stokes emission. Here, two general control mechanisms capable of affecting the ratio of intensities of the Stokes lines are identified. The first is operational when the duration of the pump pulse (tp)({t}_{p})(tp​) is on the order of the collisional dephasing time (td)({t}_{d})(td​). The ratio of the peak heights of the two Stokes lines can then be controlled by simply varying the duration and/or intensity of the pump pulse. The second operates when 1∕tp1∕{t}_{p}1∕tp​ is on the order of the energy separation of the two Raman modes, and hence when the two Raman modes are coupled due to overlapping nonlinear polarizations that drive the stimulated Raman scattering. In this regime, asymmetry in the spectral amplitudes within the pump pulse can control the asymmetry in the peak heights of the Stokes emission. Both these mechanisms have the same clear physical interpretation: shaping the pump pulse controls the nonlinear optical response of the medium, which in turn controls the stimulated Stokes emission, itself a ${\ensuremath{\chi}}^{(3)}$ nonlinear effect. In neither mechanism does the ratio of peak heights in the Stokes spectrum reflect directly the ratio of excited-state populations associated with the two Raman modes, as was assumed in the experiments, nor does the control involve coherent quantum interference effects.
Experimental results on adaptive feedback control of transient (i.e., nonimpulsive) Stokes emission in liquid methanol [Pearson and Bucksbaum, Phys. Rev. Lett. 92, 243003 (2004)] are analyzed. In the experiment, a pump pulse comprising two frequency-shifted Gaussian pulses was used to control the ratio of two Stokes emission lines by varying the relative phase ${\ensuremath{\phi}}_{L}$ between the pulses. Extending the theory of stimulated Raman scattering to accommodate two coupled levels, we show that control of this type is possible, in the strongly driven regime, using Raman coupling alone. Control via variation of ${\ensuremath{\phi}}_{L}$ is shown to also result from self- and cross-phase-modulation of the pump and Stokes pulses as well as via the focused-beam geometry of the pump pulse. In all cases, the general control mechanism is nonlinear optical modulation between the pump and the Stokes pulse; no coherent quantum interference effects are involved. Finally, although the vibrational populations are affected by the same control mechanisms that affect the Stokes spectra, the ratio of the Stokes spectra peak heights does not directly reflect the ratio of the level populations, as was assumed in the experiment.
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.