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Physical Review Letters

Generation of Single Dispersion Precompensated 1-fs Pulses by Shaped-Pulse Optimized High-Order Stimulated Raman Scattering

Vladimir P. Kalosha, Michael Spanner, Joachım Herrmann, Misha Ivanov

Published Feb 25, 2002• 106 citations
Publisher

Abstract

We propose and theoretically analyze a new approach for generating and shaping 1-fs pulses. It combines the ideas of strong-field molecular optics and optimal control to manipulate light generation in a pump-probe Raman regime. Flexible phase control over the generated spectrum of about 3 eV width is achieved by controlling the input pulses and maximizing the coherence of medium excitation by adiabatically aligning molecules in the medium with a specially shaped pump pulse. The generated pulse is optimized for an output window, precompensating for its dispersion to all orders.

DOI
10.1103/physrevlett.88.103901

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We propose and theoretically analyze a new approach for generating and shaping 1-fs pulses. It combines the ideas of strong-field molecular optics and optimal control to manipulate light generation in a pump-probe Raman regime. Flexible phase control over the generated spectrum of about 3 eV width is achieved by controlling the input pulses and maximizing the coherence of medium excitation by adiabatically aligning molecules in the medium with a specially shaped pump pulse. The generated pulse is optimized for an output window, precompensating for its dispersion to all orders.
High-order stimulated Raman scattering for pumping by ps and sub-ps pulses is studied in the frame of a time-domain approach without the slowly varying envelope approximation. Formation of pulse trains with sub-fs durations in the ps-pump regime is demonstrated using external phase compensation. For sub-ps excitation a novel broadening mechanism of Raman lines is predicted that leads to a quasicontinuous spectrum and permits one to generate single sub-fs pulses. We predict also essential shortening of a delayed fs-probe pulse by the Raman oscillations without phase control.
We have investigated the behavior of high-order stimulated Raman scattering in a highly-transient regime. We demonstrate efficient collinear generation of vibrational sidebands in molecular hydrogen and methane using two-color pumping with pulses of duration $\ensuremath{\tau}\ensuremath{\sim}100\phantom{\rule{0.3em}{0ex}}\mathrm{fs}$ tuned to a vibrational Raman transition. A Raman spectrum with a large bandwidth was observed, ranging from the IR to the UV. Under some conditions strong pump depletion was observed and up to five anti-Stokes sidebands were observed to have energies exceeding 10% of the transmitted pump pulse energies. A numerical simulation reproduces qualitatively and quantitatively the experimental results and allows us to explain key experimental features. The simulation also confirms that the molecular coherence in the medium is substantially increased by the two-color pumping and allows us to deduce values for the degree of material excitation. The use of this technique looks promising for efficient subfemtosecond pulse generation.
A technique is proposed to increase multiplicatively the pulse spacing of a periodic subfemtosecond-pulse train based on molecular modulation, with more pairs of driving lasers to control the higher-order stimulated Raman scattering. We demonstrate that the pulse spacing can be readily doubled, tripled, or even quadrupled by using pairs of off-resonant two-photon Raman transitions driven by laser beams of sufficient intensities and relatively shifted carrier frequencies. A periodic subfemtosecond-pulse train with a pulse width down to 0.53 fs and pulse spacing up to 376 fs can be generated with appropriate molecular coherence control of the fundamental rotational transition in molecular hydrogen.
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.