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Optics Letters

Exclusive anti-Stokes Raman scattering using coherent material excitation

Satoshi Wada, Masashi Kurachi, Tadamitsu Arasaki, Akinari Kasai, Hideo Tashiro

Published Oct 15, 1991• 3 citations
Publisher

Abstract

A new process capable of scattering intense anti-Stokes waves that uses stimulated electronic Raman scattering in metal vapor is proposed. The coherent material excitation produced by a prepump pulse couples with the forthcoming main pulse exclusively to create polarization that radiates the anti-Stokes wave. The selection rule governed by angular momentum conservation is the key to cause such strong coupling to induce unidirectional upconversion without any population inversion. The power conversion efficiency from the pump wave to the anti-Stokes wave is theoretically expected to reach 100% in this process.

DOI
10.1364/ol.16.001581

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A new process capable of scattering intense anti-Stokes waves that uses stimulated electronic Raman scattering in metal vapor is proposed. The coherent material excitation produced by a prepump pulse couples with the forthcoming main pulse exclusively to create polarization that radiates the anti-Stokes wave. The selection rule governed by angular momentum conservation is the key to cause such strong coupling to induce unidirectional upconversion without any population inversion. The power conversion efficiency from the pump wave to the anti-Stokes wave is theoretically expected to reach 100% in this process.
The generation of 145.6-nm radiation by stimulated anti-Stokes Raman scattering in inverted atomic selenium was first reported by Ludewigt et al. 1 We have performed experimental studies of this process in similar excitation conditions, which allow us to compare some of the results in the two studies. The inverted population of the selenium (4p4)1S0 metastable state relative to the (4p4)3P0 state was prepared by photodissociation of COSe vapor using broadband 193-nm radiation from an ArF excimer laser. The pump beam at 205.1 nm was generated by the first-order Stokes shift in deuterium of narrowband (0.27-cm–1), 193-nm radiation from a separate, tunable ArF laser. The pump beam was tuned near the selenium (4p4)1S0–(4p35s)3P1 intermediate resonance to generate tunable, coherent radiation at 145.6 nm. We have studied the process in a variety of experimental conditions. Factors affecting the conversion efficiency and tunability include the initial COSe pressure, the intensities and relative timing of the photolyzing and pump beams, and the presence of buffer gases. The experimental results are compared with theoretical calculations based on a recently developed three-level model2 which incorporates Doppler broadening and arbitrary decay times.
In the correlated Stokes--anti-Stokes scattering (SAS) an incident photon interacts with a Raman-active material, creating a Stokes photon and exciting a quantum vibrational mode in the medium, which is posteriorly annihilated on contact with a second incident photon, producing in turn an anti-Stokes photon. This can be accomplished by real and virtual processes. In the real process the quantum mode shared between the Stokes and anti-Stokes events is a real particle, whereas in virtual processes the pair formation is mediated by the exchange of virtual particles. Here, we introduce a Hamiltonian to describe the pair production in SAS scattering, for both types of process, when stimulated by two orthogonally polarized laser pulses in a pump-and-probe configuration. We also model the effect of the natural decay of the vibration created in the Stokes event and compute the probability of producing SAS pairs. Additionally, we follow the dynamics of the vibration by considering the Stokes and anti-Stokes fields as external reservoirs, obtaining thus a master equation for the reduced density matrix for the vibrational population. Finally, we compare our theoretical results to recently published experimental data.
In transient stimulated Raman scattering (SRS), efficient conversion of short pump pulses to Stokes radiation is difficult to obtain. A short seed pulse at the Stokes frequency increases the efficiency and may induce full depletion of the pump pulse, even when the pump power is too low to scatter efficiency without seed. However, for low pump powers the Ra­man polarizability induced by the pump and seed pulse decays, which results in a terminating Stokes pulse, even when the pump pulse itself is long. Nevertheless, the Stokes pulse can be wider than the dephasing time of the Raman polarizability or the width of the seed pulse by an order of magnitude. Applying a second seed may once again induce a sufficiently large Raman polarizability but only if the phase of the Stokes seed matches the phase difference between the pump and remaining Raman polarizability. If not, the polarizability induced by the first pulse and consequently the conversion efficiency for the Stokes radiation decreases. Therefore, it is possible to switch off the Stokes pulse by applying a second seed with appropriate phase and intensity.
Transient stimulated rotational Raman scattering induced by a polarization-modulated femtosecond pulse whose polarization varies with time is reported. The peak intensity of the polarization-modulated pulse produced in this study is low compared to that of a pulse without polarization variation, and this leads to the low efficiency of self-phase-modulation and thus the high efficiency of stimulated Raman scattering compared to the case of a pump pulse without polarization modulation. The scattering process is unique in terms of the high peak ratio of the anti-Stokes to Stokes emissions compared to the ratio in the case of the scattering induced by linearly, circularly, and elliptically polarized pump pulses. Under optimum conditions, the ratio approaches 1, which is not realized in the general case of stimulated rotational Raman scattering.