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Optics Letters

Raman gain measurement in solid parahydrogen

M. Katsuragawa, K. Hakuta

Published Feb 1, 2000• 14 citations
Publisher

Abstract

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.

DOI
10.1364/ol.25.000177

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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.
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.
Using a sodium Raman laser that is pumped by a single-frequency cw dye laser, we have measured the narrow-band Raman gain that exists in the vicinity of the sodium D(1) line. Large gains (>10 cm(-1)) are measured at moderate pump intensities and sodium densities. The high gain allows us to detect directly a 1.772-GHz beat on the pump beam after it makes only a single pass through the sodium cell. By scanning the frequency of the sodium Raman laser while keeping the pump intensity and frequency constant, we are able to map out the Raman gain profile. The narrowness of the Raman gain is consistent with the narrow beat signal between the Raman-laser beam and the pump beam that was reported earlier [Opt. Lett. 16, 1853 (1991)].
We have confirmed, for the first time to our knowledge, the nonexponential character of Raman amplification at the phase matching angle ϕ for which 2kL = ks + kA. The experiments reported here used spatially filtered pump and probe beams at 532 and 633 nm, respectively, of 30-ps duration interacting in a one-half meter cell filled with deuterium at a pressure of 600 psi. The pump and probe beams were crossed at various small angles in the cell and the gain experienced by the probe pulse was measured. At angles below 5 mrad the Stokes amplification was exponential in character and reached levels of 107. At an angle of 7 mrad, the phase matching angle for our conditions, there was no observed amplification of the Stokes pulse. At yet larger angles (~9 mrad) the gain was again exponential in character and reached levels of 107. We have also observed a double ring pattern in the anti-Stokes radiation produced in our experiment. This pattern was predicted by Bloembergen1 with the explanation that a single anti-Stokes ring is split by a region of gain suppression at the phase matching angle. We have verified that the diameter of the dark band in the anti-Stokes emission grows as the square root of the pressure, exactly as would be predicted assuming that the dark region is caused by gain suppression at phase matching.
A stimulated-Raman-gain medium at 1.56-microm wavelength, consisting of molecular deuterium dissolved in low-loss silica optical fiber and pumped by 1.06-microm Nd:YAG laser light, is described. In a 100-m-long fiber with pump power of 130 W, InGaAsP injection-laser probe light at 1.56 microm was amplified by a factor of 4000 to an output power of 150 mW. The measured stimulated-Raman-gain coefficient at 1.56 microm is 7 x 10(-12) cm/W, about equal to the Raman gain of SiO(2) at the same wavelength.
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.
The authors have extended the theory of stimulated Raman scattering to include the effects of laser bandwidths, in both the transient and steady-state regimes. The case of two interacting laser beams, a pump laser and a probe (Stokes) laser, is treated. Using the phase-diffusion model for laser bandwidth, the authors demonstrate that in the absence of dispersion, the forward Raman gain is essentially independent of the laser bandwidths in the high-gain limit, while in the low-gain limit the gain coefficient is inversely proportional to the sum of the bandwidths. It is further shown that when the pump-laser bandwidth is much larger than the linewidth of the Raman medium, the stimulated Stokes output assumes the same spectrum as the pump laser in the high-gain limit. A possible interpretation of these results is discussed assuming a "phase-locking" of the Stokes phase to the fluctuations in the pump-laser phase, due to the nonlinear interaction of the two beams through the Raman medium.