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Optics Letters

Continuous-wave stimulated Raman scattering in microdroplets

Hsing‐An Lin, Jay D. Eversole, A. J. Campillo

Published Jun 1, 1992• 62 citations
Publisher

Abstract

Continuous-wave stimulated Raman scattering was observed in 11-13-microm-diameter benzene and toluene microdroplets at pump intensities as low as 8 and 24 kW/cm(2), respectively. Low thresholds were achieved by exploiting simultaneous pump and Stokes wave resonance in the droplets and Raman gains that were cavity QED enhanced ~50 times with respect to bulk liquid values. Based on a photon-state conservation argument, the cavity gain enhancement factor may be approximated by the ratio of the spectral spacing between resonant modes of the same order to that of the homogeneous Raman linewidth. This relation appears to be consistent with the relative experimental behavior of benzene, ethanol, and toluene.

DOI
10.1364/ol.17.000828

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Continuous-wave stimulated Raman scattering was observed in 11-13-microm-diameter benzene and toluene microdroplets at pump intensities as low as 8 and 24 kW/cm(2), respectively. Low thresholds were achieved by exploiting simultaneous pump and Stokes wave resonance in the droplets and Raman gains that were cavity QED enhanced ~50 times with respect to bulk liquid values. Based on a photon-state conservation argument, the cavity gain enhancement factor may be approximated by the ratio of the spectral spacing between resonant modes of the same order to that of the homogeneous Raman linewidth. This relation appears to be consistent with the relative experimental behavior of benzene, ethanol, and toluene.
A variety of stimulated nonlinear optical processes are observed under relatively low intensity cw excitation in droplet spherical microcavities. These include stimulated Raman and Rayleigh-wing scattering as well as four-wave parametric oscillation. The low thresholds for these stimulated processes are accounted for by all waves being in resonance with high-QQQ droplet modes and by the existence of a significant cavity QED enhancement (> 100 times) in the nonlinear gain coefficients.
Cavity-QED-enhanced stimulated visible emission was observed in 14-\ensuremath{\mu}m-diam rhodamine-6G--ethanol droplets pumped by cw 514.5-nm radiation. Use of droplets provides an excellent test of cavity QED theory for spherical geometries. The mode number and order of the spherical-cavity resonances responsible for the observed emission peaks were identified and their Q values calculated from Lorenz-Mie theory. By equating stimulated gain to calculated/measured cavity losses, it was determined that spherical-cavity Q's of only 103−−{10}^{3--}103−−104{10}^{4}104 lead to cavity QED enhancements in excess of 120 in the emission cross section of rhodamine 6G, consistent with theory.
Stimulated Brillouin scattering in a micrometer-sized liquid droplet is treated theoretically using recently developed techniques, with emphasis on the doubly resonant case, in which the frequencies of both the laser field and the scattered Brillouin field fall within a morphology-dependent resonance, leading to input and output enhancement. An important difference from a bulk medium is the replacement of the selection rules based on momentum conservation by those based on angular momentum conservation, with the latter most conveniently expressed through the spherical wave modes. Special attention is paid to the eigenvalue equation defining the gains and Brillouin shifts, in particular to the difference between small and large droplets. For large droplets, and for given angular momenta of the laser field and the scattered field, there is only one allowed shift with a positive gain. Numerical results for gain and threshold are shown for a droplet of size parameter about 30, and a simple approximate analytic formula for the gain is presented.
Significant cavity QED enhancement have been observed of both spontaneous and stimulated emission in 10- to 14-micrometers diameter liquid microdroplets containing fluorophors. Direct emission lifetime reduction was observed as well as greatly enhanced lasing gain. Use of droplets provides an excellent test of cavity QED theory for spherical geometries. The mode number and order of the spherical cavity resonances responsible for the observed emission peaks were identified and their Q values calculated from Lorenz-Mie theory. An experimental procedure, based on equating stimulated gain to cavity losses, is used to estimate the magnitude of the enhancement. Spherical cavity Qs of only 2600 were found to lead to cavity enhancements of over 100 in the emission cross-section of Rhodamine 6G in agreement with theory.
Micrometer-sized transparent droplets act as natural high-Q cavities to visible light, and this paper shows them to exhibit strongly enhanced dye emission owing to cavity quantum-electrodynamic effects. A vibrating-orifice aerosol generator1 was used to produce a linear stream of virtually identical (less than 2 parts in 105 diameter variation) falling droplets 14 μm diameter, 10-5 M solution of Rhodamine 6G in ethanol; the droplets were excited by a cw argon-ion laser. Droplet emission was examined with a double 1 m Spex spectrograph and a photomultiplier. Recent development of elastic-scattering-size spectroscopy1,2 allowed identification of the various cavity modes contributing to the emission. This was necessary because of the different Q values and spatial properties of the resonant modes. Q values were calculated from Lorenz-Mie theory and were found to be consistent with observed fluorescence linewidths for the experimentally resolvable fourth-order modes. It was experimentally determined that Q's of only 103 were sufficient to observe sizable enhancements in the A coefficient. Lasing was observed to occur at reduced thresholds, e.g., 400 W/cm2 for fourth order modes having Q's of 2 × 103. This corresponds to a cavity induced enhancement in the B coefficient of 103.