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Japanese Journal of Applied Physics

Stimulated Raman Scattering in Vapor-Deposited Solid Hydrogen Film

Geon Joon Lee, Kento Hara, M. Katsuragawa, K. Hakuta

Published Oct 9, 2003• 1 citation
Publisher

Abstract

The solid para-hydrogen film was prepared by depositing the para-hydrogen vapor onto a sapphire substrate. From the stimulated Raman scattering experiment using two ns-lasers whose laser-frequency difference is equal to the fundamental vibrational transition of the solid para-hydrogen, we observed the collinear generation of Raman sidebands. The high-order Raman sidebands were obtained under the strong pumping intensity (≥230 MW/cm 2 ). The generated five anti-Stokes(AS)-Raman sidebands extend from ultraviolet (292 nm for AS 5 band) to visible (565 nm for AS 1 band) region. Also, we found that the first AS-Raman signal shows weak rotational components as well as a strong vibrational line. 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. The frequency conversion efficiency from the probe beam to the first AS-Raman sideband rises to the maximum (4.7%) at 284 MW/cm 2 , and then falls with the increase of the pumping intensity. This is thought to be due to the fact that some molecules in the first vibrational level incline to go to the higher vibrational level under the higher pumping intensity. For the strong pumping intensity (290 MW/cm 2 ), four anti-Stokes and one Stokes Raman sidebands of the probe beam were generated.

DOI
10.1143/jjap.42.6450

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The solid para-hydrogen film was prepared by depositing the para-hydrogen vapor onto a sapphire substrate. From the stimulated Raman scattering experiment using two ns-lasers whose laser-frequency difference is equal to the fundamental vibrational transition of the solid para-hydrogen, we observed the collinear generation of Raman sidebands. The high-order Raman sidebands were obtained under the strong pumping intensity (≥230 MW/cm 2 ). The generated five anti-Stokes(AS)-Raman sidebands extend from ultraviolet (292 nm for AS 5 band) to visible (565 nm for AS 1 band) region. Also, we found that the first AS-Raman signal shows weak rotational components as well as a strong vibrational line. 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. The frequency conversion efficiency from the probe beam to the first AS-Raman sideband rises to the maximum (4.7%) at 284 MW/cm 2 , and then falls with the increase of the pumping intensity. This is thought to be due to the fact that some molecules in the first vibrational level incline to go to the higher vibrational level under the higher pumping intensity. For the strong pumping intensity (290 MW/cm 2 ), four anti-Stokes and one Stokes Raman sidebands of the probe beam were generated.
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.
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.
Summary form only given. Recently we have shown using solid hydrogen that stimulated Raman scattering (SRS) can evolve spontaneously from the weak-coupling regime to the strong-coupling regime in which parametric anti-Stokes generation occurs without the restriction of phase-matching. In the present work, we extend this strong-coupling SRS to a more general parametric Raman sideband generation. We show using solid hydrogen as a nonlinear medium that the adiabatically-prepared Raman-coherence can beat with broadband incoherent fluorescence light and efficiently replicate the incoherence nature to the Raman sideband.
Summary form only given. There has been increasing interest in optical processes using strong-coupling and induced transparency, termed electromagnetically induced transparency (EIT). Although the idea of EIT started for resonant /spl and/h-scheme (Raman scheme), the idea has now been extended to far-off resonance Raman system. We have reported the spontaneous evolution of strong-coupling through stimulated Raman scattering (SRS) using solid hydrogen. In the present work, we extend the strong-coupling SRS to a more general parametric Raman sideband generation. We show using solid hydrogen as a test medium that, in tile far-off resonance Raman scheme, the strongly-coupled Raman coherence can beat with very broad-band laser radiation and can efficiently copy the broadband nature to Raman sidebands without restriction of the phase-matching, and that this efficient copying occurs on the negative Raman detuning for which the strongly-coupled eigenstate evolves to the anti-phased state (dark state).
We report a steady-state Raman gain measurement of the Q(1)(0) transition (v = 1 ? 0, J = 0 ? 0) in solid parahydrogen. We carry out measurements by pumping with a continuous-wave frequency-doubled YAG laser at 532 nm and observing the direct amplification of a probe-laser beam for the first Stokes transition at 683 nm. A large single-pass amplification coefficient of 2.3 +/- 0.2 is obtained at a pump intensity of 46 kW/cm(2), with an interaction length of 1 cm, giving a steady-state Raman gain coefficient of 18 +/- 3 cm/MW.