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Physical Review A

Two-dimensional model for femtosecond pulse conversion and compression using high-order stimulated Raman scattering in solid hydrogen

Nguyen Hong Shon, Fam Le Kien, K. Hakuta, Alexei V. Sokolov

Published Feb 7, 2002• 18 citations
Publisher

Abstract

We present a numerical model for the interaction of a femtosecond probe pulse with a Raman medium excited by two nanosecond laser pulses in solid hydrogen. The model consists of a solution of a system of Bloch equations (for the medium state) and of the two-dimensional wave equation (for the field propagation). It is shown that by optimizing the tilt angle between the two driving pulses and the interaction length, the power of the probe pulse can be converted either into a quasicontinuous broadband spectrum or into a selected high-order sideband. The first situation can be used for generation of subfemtosecond pulses. The second situation can be used for the wavelength conversion of a femtosecond probe pulse from the infrared to the ultraviolet region. Due to the transfer of energy from the driving pulses, the energy conversion efficiency of these processes (with respect to the probe pulse) can be larger than unity.

DOI
10.1103/physreva.65.033809

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We present a numerical model for the interaction of a femtosecond probe pulse with a Raman medium excited by two nanosecond laser pulses in solid hydrogen. The model consists of a solution of a system of Bloch equations (for the medium state) and of the two-dimensional wave equation (for the field propagation). It is shown that by optimizing the tilt angle between the two driving pulses and the interaction length, the power of the probe pulse can be converted either into a quasicontinuous broadband spectrum or into a selected high-order sideband. The first situation can be used for generation of subfemtosecond pulses. The second situation can be used for the wavelength conversion of a femtosecond probe pulse from the infrared to the ultraviolet region. Due to the transfer of energy from the driving pulses, the energy conversion efficiency of these processes (with respect to the probe pulse) can be larger than unity.
We suggest a technique to generate subfemtosecond pulse train in a Raman generator driven by three sufficiently intense single-mode laser beams whose carrier frequencies are tuned off the Raman resonance with two different two-photon detunings. The Raman interaction establishes a molecular modulation through a nonadiabatic process. The simulation based on the first fundamental vibrational Raman transition of solid hydrogen indicates that subfemtosecond pulse train can be generated when the signs of the two-photon detunings are opposite. This opens an experimentally feasible way to observe enhanced generation of broadband Raman sidebands as well as compression of the phase-locked Raman sidebands into subfemtosecond pulse trains in the same Raman media with above- and below-resonance Raman excitations.
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.
Subfemtosecond (sub-fs) pulses can be generated by cascade-stimulated Raman scattering in a Raman medium with modulated Raman excitations, driven by two sufficiently intense laser beams, one of which is amplitude modulated. The nonadiabatic Raman interaction establishes a strong modulated Raman coherence, which supports compression of the generated broadband Raman sidebands to a train of sub-fs pulses regardless of whether the carrier frequencies of the driving lasers are tuned above, below or on two-photon Raman resonance.
We suggest that subfemtosecond pulses can be generated by using high-order stimulated Raman scattering when a Raman transition is driven by three intense single-mode laser beams with two different modulation frequencies. An oscillatory strong Raman coherence is established by the modulated molecular modulation. Numeric simulations based on the first fundamental vibrational Raman transition of gaseous and solid deuterium indicate that subfemtosecond pulses can be generated by Raman excitations with above, below, or opposite Raman detunings.
We investigated the Raman coherence characteristics in the solid hydrogen film deposited on a sapphire substrate. By using Raman coherence prepared with two single-frequency pulsed lasers, we generated the multiorder coherent Raman sidebands in solid hydrogen film. High-order Raman sidebands were obtained under strong pumping conditions (≥230 MW/cm2). The generated anti-Stokes(AS)–Raman sidebands extended from ultraviolet (292 nm for AS5 band) to visible (565 nm for AS1 band) region. The multiorder Raman sideband generation is thought to be due to the parametric coupling of pump and coupling lasers. The frequency conversion efficiency shows the maximum (14%) at the pumping intensity of 360 MW/cm2. From the experiment that makes the multimode probe beam beat with the prepared Raman coherence, we found that the prepared Raman coherence replicates the probe beam to its Raman sidebands.