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Physical Review A

Cavity-modified spontaneous-emission rates in liquid microdroplets

H.‐B. Lin, J. D. Eversole, Charles D. Merritt, A. J. Campillo

Published May 1, 1992• 105 citations
Publisher

Abstract

We observe significant lifetime modification (both reduction and lengthening) of 610--620-nm light spontaneously emitted by chelated europium ions in 10-\ensuremath{\mu}m-diam dimethylformamide-alcohol solution droplets. The enhancement or inhibition of the Einstein A coefficient over the familiar free-space value is direct evidence of cavity quantum-electrodynamic effects taking place in microdroplets.

DOI
10.1103/physreva.45.6756

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Annual Meeting Optical Society of America•Jan 1, 1993•0 citations
We observe significant lifetime modification (both reduction and lengthening) of 610--620-nm light spontaneously emitted by chelated europium ions in 10-\ensuremath{\mu}m-diam dimethylformamide-alcohol solution droplets. The enhancement or inhibition of the Einstein A coefficient over the familiar free-space value is direct evidence of cavity quantum-electrodynamic effects taking place in microdroplets.
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.
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.
Measurements of the integrated fluorescence yield per molecule of Rhodamine 6G (R6G) in 4–16-μm-diameter levitated microdroplets show a size dependence that is attributed to a net increase in the fluorescence decay rate for the smaller (4–5-μm) droplets. The average fluorescence yield in 4-μm droplets (for which we have previously observed emission-rate enhancement) is approximately a factor of 2 larger than the yield measured for larger droplets for which emission-rate enhancement does not occur. These results suggest that there is little emission-rate inhibition in this system, even though the fluorescence emission spectrum overlaps several cavity resonances. A mechanism based on spectral diffusion is postulated for the apparent absence of cavity-inhibited emission and is illustrated by Monte Carlo calculations using time-dependent line-shape functions.
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.