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Conference on Lasers and Electro-Optics

70,000 cm−1 wide Raman sideband spectrum generated by vibrational molecular modulation in room temperature H2

A. H. Kung, Wei-Jan Chen, Shu Wei Huang

Published Jan 1, 2006• 0 citations
Publisher

Abstract

Dicke narrowing dominates over collisional dephasing in gas phase H2up to 500 Torr, permitting the efficient production of a record 70,000 cm−1broad Raman sideband spectrum by molecular modulation at room temperature.
DOI
10.1109/cleo.2006.4628891

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Detailed numerical modeling of using the vibrational coherence of H2{\mathrm{H}}_{2}H2​ for molecular modulation is presented. The focus of the calculation is on a strongly driven system aimed at producing many sidebands in the presence of Doppler broadening and the effects of collisions at room temperature. It is shown that Dicke narrowing that reduces the Doppler width plays a critical role in high order sideband generation in room temperature H2{\mathrm{H}}_{2}H2​. In addition, the calculation shows that generation of many sidebands favors the phased state as has been reported in all gas phase experiments and is primarily a consequence of the Stark shifts that result from the applied high intensities. The influence of self-focusing in the gas medium that has been conjectured in previous studies is only secondary. The numerical results agree with experimental data obtained in our laboratory, where we have succeeded in generating collinearly propagating Raman sidebands with wavelengths that range from 2216nm2216\phantom{\rule{0.3em}{0ex}}\mathrm{nm}2216nm in the infrared to 133nm133\phantom{\rule{0.3em}{0ex}}\mathrm{nm}133nm in the vacuum ultraviolet. The frequencies covered by these sidebands span over four octaves for a total of more than $70\phantom{\rule{0.2em}{0ex}}600\phantom{\rule{0.3em}{0ex}}{\mathrm{cm}}^{\ensuremath{-}1}$ in the optical region of the spectrum.
We demonstrate the efficient modulation of an approximately 100-femtosecond pulse in a Raman medium coherently prepared by nanosecond pulses. Raman sidebands of the ultrashort pulse spanning 360 THz are generated with an efficiency of >5%. We show that the mechanism permitting the sidebands to be generated is the preparation of a significant vibrational coherence in the medium that is robust to disturbance by an intense short pulse. If the observed sidebands were phase compensated, they would form a short train of approximately ten 3-fs pulses. Focusing would permit the realization of a peak intensity of >10(13) W cm(-2).
Summary form only given. A new way to reach the Lamb-Dicke regime in molecular gases has been reported in [1]. This is achieved by trapping H2molecule during Stimulated Raman Scattering (SRS) in a photonic band gap hollow-core fiber (PBG HC-PCF) pumped with a high power CW laser [1]. The molecular trapping process occurs in a self-assembled manner, whereby the Raman active molecules are confined in nanometer-wide sections by a periodic and ultra-deep potential thanks to a spatially modulated Raman saturation. It has permitted to obtain sub-recoil linewidths as low as 14 kHz which is 5 orders of magnitude lower than the expected H2Doppler-broadened linewidth for a product of the input power and the pressure below 1000 W.bar. Above this threshold the linewidth broadens due to the generation of the second-order Stokes.Here, we report a further linewidth narrowing down to 2.7 kHz by increasing the length and decreasing the gas pressure. Longer fiber lowers the pump power required for the SRS generation and enables formation of the trapping potential for lower gas pressure, which in turn reduces the molecular collision rate. The Stokes generation was obtained using a set-up similar to the one used in [1]. The PBG fiber has been tailored in order to have a spectral window between 1000 and 1200 nm in order to filter out any other Raman generation except the first rotational Stokes S00(1) at 1131.4 nm. The range of pressure of H2 with which we filled the PBG fiber is from 5 to 50 bars. The pump laser is a narrow linewidth (400 kHz) CW laser with a maximum pump power Pin of 100 W. Figure 1(a) shows the typical linewidth trace of the forward emitted Stokes for a fiber length of 30 m, a gas pressure of 20 bar and a pump power of 12 W. Figure 1(b) shows a resolved spectrum of the Stokes central line, which demonstrates a linewidth of 2.7 kHz. This line is nearly 30 times narrower than the hydrogen molecule recoil frequency Vrecο1 = πh(mλs2) of ~78 kHz, 5 orders of magnitude narrower than the Doppler width and almost 6 orders of magnitude narrower than the H2 pressure broadened line. Linewidth(kHz)
Trapping or cooling molecules has rallied a long-standing effort for its impact in exploring new frontiers in physics and in finding new phase of matter for quantum technologies. Here we demonstrate a system for light-trapping molecules and stimulated Raman scattering based on optically self-nanostructured molecular hydrogen in hollow-core photonic crystal fibre. A lattice is formed by a periodic and ultra-deep potential caused by a spatially modulated Raman saturation, where Raman-active molecules are strongly localized in a one-dimensional array of nanometre-wide sections. Only these trapped molecules participate in stimulated Raman scattering, generating high-power forward and backward Stokes continuous-wave laser radiation in the Lamb-Dicke regime with sub-Doppler emission spectrum. The spectrum exhibits a central line with a sub-recoil linewidth as low as ∼14 kHz, more than five orders of magnitude narrower than conventional-Raman pressure-broadened linewidth, and sidebands comprising Mollow triplet, motional sidebands and four-wave mixing.