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Optics Letters

Efficient two-photon-resonant frequency conversion in mercury: the effects of amplified spontaneous emission

Arlee V. Smith, George Ronald Hadley, P. Esherick, W. J. Alford

Published Sep 1, 1987• 8 citations
Publisher

Abstract

Numerical modeling of two-photon-resonant sum-frequency mixing in mercury vapor predicts efficiencies >10% for generation of 130.2-nm oxygen resonance light. The modeling indicates that power broadening of the two-photon resonance due to amplified spontaneous emission from the pumped level strongly influences the mixing process. Measurements of the broadening and the efficiencies for difference-frequency mixing are presented as a check of the model calculations.

DOI
10.1364/ol.12.000708

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Previously we showed1 that two-photon-resonant sum- and difference-frequency mixing in Hg vapor is a practical means of generating coherent light over the 140-120- and 230-185-nm wavelength ranges. Here we consider optimization of the conversion efficiency for such a two-photon-resonant mixing process in general and for generation of 130.2-nm atomic oxygen resonance light in particular. We predict that conversion efficiencies (defined as the energy of the sum frequency divided by the total input light energy) of 5-10% should be possible for 130.2-nm production using unfocused mixing beams. This prediction is being tested in experiments at Spectra Technologies, Inc. Their results are described in a companion paper.

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Physical Review A•Feb 1, 1993•14 citations
Numerical modeling of two-photon-resonant sum-frequency mixing in mercury vapor predicts efficiencies >10% for generation of 130.2-nm oxygen resonance light. The modeling indicates that power broadening of the two-photon resonance due to amplified spontaneous emission from the pumped level strongly influences the mixing process. Measurements of the broadening and the efficiencies for difference-frequency mixing are presented as a check of the model calculations.
Previously we showed1 that two-photon-resonant sum- and difference-frequency mixing in Hg vapor is a practical means of generating coherent light over the 140-120- and 230-185-nm wavelength ranges. Here we consider optimization of the conversion efficiency for such a two-photon-resonant mixing process in general and for generation of 130.2-nm atomic oxygen resonance light in particular. We predict that conversion efficiencies (defined as the energy of the sum frequency divided by the total input light energy) of 5-10% should be possible for 130.2-nm production using unfocused mixing beams. This prediction is being tested in experiments at Spectra Technologies, Inc. Their results are described in a companion paper.
A detailed model of two-photon-resonant four-wave mixing that includes the consideration of efficiency-limiting processes is presented. The model provides a generally applicable systematic approach for maximizing conversion efficiencies for both exact and near two-photon resonance. For exact two-photon resonance, an interference effect limits efficiency to a value determined by ratios of nonlinear susceptibilities and input intensities. For near two-photon resonance, nonlinear refractive indices limit efficiencies unless input intensities are properly balanced. For the specific case of 130.2-nm generation in Hg, we examine a number of potential additional efficiency-limiting processes, including amplified spontaneous emission, stimulated Raman and hyper-Raman gain, parametric gain, linear absorption, and population transfer. We include isotopic effects and Gaussian-profile beams. From our analysis, we conclude that efficiencies of approximately 10% should be feasible by using collimated light beams in an energy-scalable system.
Two-photon-resonant excitation of the sodium 3d3d3d level can lead to the generation of new frequencies either by amplified spontaneous emission at the $3d\ensuremath{\rightarrow}3p$ transition frequency or by a resonantly enhanced four-wave mixing process. Competition between these two processes has been observed. The four-wave mixing process can suppress amplified spontaneous emission by preventing the excitation of the 3d3d3d level due to an interference between two different pathways connecting the ground (3s3s3s) and 3d3d3d states.
We report experiments that investigate the generation of coherent VUV radiation at 123.6 nm via a resonant sum-difference frequency mixing scheme in Kr. One of the mixing fields at 212.55 nm was in two-photon resonance with the transition between the 4p61S{4p}^{6}{}^{1}S4p61S ground state and the 4p55p[0,12]{4p}^{5}5p[0,\frac{1}{2}]4p55p[0,21​] excited state $(94093.7 {\mathrm{cm}}^{\ensuremath{-}1}).$ The second field (the coupling field) at 759 nm was in single-photon resonance with the transition between the 4p55p[0,12]{4p}^{5}5p[0,\frac{1}{2}]4p55p[0,21​] state and the 4p55s[1,12]{4p}^{5}5s[1,\frac{1}{2}]4p55s[1,21​] state at $80917.6 {\mathrm{cm}}^{\ensuremath{-}1}.$ The presence of the coupling field leads to electromagnetically induced transparency (EIT) at the wavelength of the generated field, 123.6 nm. This is predicted to enhance the four-wave-mixing efficiency by a large factor. We have studied the dependence of the four-wave mixing process on the detuning and strength of the coupling field. The efficiency for four-wave mixing was found to be enhanced by a significant factor (>5) by the EIT effect when the resonant coupling field strength exceeded about half the Doppler width $(0.1 {\mathrm{cm}}^{\ensuremath{-}1}).$ A calculation for monochromatic fields and a uniform slab of gas provided qualitative agreement with the results of experiment. The relative conversion efficiency for this resonant mixing scheme is found to be 104{10}^{4}104 times greater than that for a similar scheme where the coupling laser is tuned far $(1270 {\mathrm{cm}}^{\ensuremath{-}1})$ off resonance. A substantial part of this resonant enhancement can thus be attributed to the EIT effect.
An experimental and theoretical study of magnetic-field-induced sum-frequency mixing in sodium vapor has been carried out using two single-frequency, continuous-wave dye lasers as the sources of the fundamental radiation. In addition to the usual two-photon resonant enhancement of the three-wave-mixing nonlinear-optical process, the use of near- or on-resonant single-photon transitions for further resonant enhancement was investigated. The macroscopic phase-matching behavior of the sum-frequency mixing was examined with the intermediate states off resonance. Experimental and theoretical results are presented to illustrate the differences that occur between the coherent quadrupole emission and the incoherent cascade fluorescence when the intermediate states in the two-photon absorption are resonant. Control over the single-photon resonant enhancement and the sum-frequency-mixing phase matching was achieved to increase the power conversion efficiency to 1.2\ifmmode\times\else\texttimes\fi{}${10}^{\mathrm{\ensuremath{-}}5}$.