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Physical Review A

Measurement of high conversion efficiency to 123.6-nm radiation in a four-wave-mixing scheme enhanced by electromagnetically induced transparency

C. Franklin Dorman, İbrahim Küçükkara, J. P. Marangos

Published Dec 8, 1999• 50 citations
Publisher

Abstract

We report measurements of the absolute yield of 123.6-nm vacuum ultraviolet (VUV) radiation produced in a resonant four-wave-mixing scheme in krypton enhanced by electromagnetically induced transparency. One of the mixing fields, in the ultraviolet (UV) at 212.55 nm, was in two-photon resonance with the ${4p}^{6}{}^{1}{S}_{0}--{4p}^{5}5p[0,\frac{1}{2}]$ transition of krypton, while a second field (the coupling field) at 759 nm was resonant with the ${4p}^{5}5p[0,\frac{1}{2}]{\ensuremath{-}4p}^{5}5s[1,\frac{1}{2}]$ transition. Electromagnetically induced transparency has been predicted to be induced by this coupling field and to enhance the efficiency of the generation of the field at 123.6 nm, on the ${4p}^{5}5s[1,\frac{1}{2}]$ to ${4p}^{6}{}^{1}{S}_{0}$ transition. This was confirmed by measurements of the absolute VUV radiation yield using a calibrated photodiode in the limit of a large density-length product. Energies of \ensuremath{\sim}30 nJ were produced, which gave a conversion efficiency, from the coupling field energy of \ensuremath{\sim}1%. Higher yields are thought to be achievable by increasing the coupling laser intensity, the path length of the medium, and by the use of a transform-limited UV pulse of the same duration as the coupling field.

DOI
10.1103/physreva.61.013802

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We report measurements of the absolute yield of 123.6-nm vacuum ultraviolet (VUV) radiation produced in a resonant four-wave-mixing scheme in krypton enhanced by electromagnetically induced transparency. One of the mixing fields, in the ultraviolet (UV) at 212.55 nm, was in two-photon resonance with the 4p61S0−−4p55p[0,12]{4p}^{6}{}^{1}{S}_{0}--{4p}^{5}5p[0,\frac{1}{2}]4p61S0​−−4p55p[0,21​] transition of krypton, while a second field (the coupling field) at 759 nm was resonant with the 4p55p[0,12]\ensuremath−4p55s[1,12]{4p}^{5}5p[0,\frac{1}{2}]{\ensuremath{-}4p}^{5}5s[1,\frac{1}{2}]4p55p[0,21​]\ensuremath−4p55s[1,21​] transition. Electromagnetically induced transparency has been predicted to be induced by this coupling field and to enhance the efficiency of the generation of the field at 123.6 nm, on the 4p55s[1,12]{4p}^{5}5s[1,\frac{1}{2}]4p55s[1,21​] to 4p61S0{4p}^{6}{}^{1}{S}_{0}4p61S0​ transition. This was confirmed by measurements of the absolute VUV radiation yield using a calibrated photodiode in the limit of a large density-length product. Energies of \ensuremath{\sim}30 nJ were produced, which gave a conversion efficiency, from the coupling field energy of \ensuremath{\sim}1%. Higher yields are thought to be achievable by increasing the coupling laser intensity, the path length of the medium, and by the use of a transform-limited UV pulse of the same duration as the coupling field.
We report experiments investigating a resonant sum-difference frequency mixing scheme in krypton producing coherent radiation at 123.6nm (i.e. in the vacuum ultraviolet (VUV)). Owing to the resonant nature of this scheme, electromagnetically induced transparency (EIT) plays a crucial role in the generation of this coherent radiation, resulting in a greatly enhanced conversion efficiency. This is the first time a resonant sum-difference mixing scheme involving EIT, that generates VUV radiation, has been investigated experimentally. Our results are in broad agreement with theoretical predictions. Measurements are presented of the dependence of VUV generation on laser detuning (in the range ± cm−1) and laser powers. In particular the dependence on the coupling field strength has been studied in the range of coupling field Rabi frequencies Ωc = 0.05−3 cm−1. We estimate an enhancement in the conversion efficiency, compared with the non-resonant case, of greater than 102.
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.
Summary form only given.Resonant sum-difference frequency mixing has been investigated in krypton. A two-photon resonant field tuned to 212.55 nm drove transitions between the ground state and the excited state. This excited state was coupled by a near-resonant field at 759 nm. The infrared coupling field was near transform limited and under these conditions should result in electromagnetically induced transparency (EIT) at the frequency of the generated VUV field (123.6 nm). The predicted enhancement in the conversion efficiency of the scheme was investigated by studying the dependence of the VUV signal on intensity and detuning of the coupling field.
Summary form only given. The techniques of electromagnetically induced transparency (EIT) may be employed in order to create an effective nonlinear response at a given wavelength which is equal in magnitude to the linear response at that wavelength. Physically, this allows frequency converters wherein 100% photon-to-photon conversion occurs in a single coherence length, i.e., in that distance which causes a /spl pi/ phase slip between the driving polarization and the generated electromagnetic wave. These ideas were first implemented by Jain et al. (1996), to convert 425 nm to 293 nm, in a medium consisting of a single isotope of Pb. This paper reports the demonstration of a vapor-phase VUV frequency converter from 233 nm to 186 nm with an energy conversion efficiency exceeding 35%; the maximum generated signal energy and power were 250 /spl mu/J and 25 kW. The net conversion efficiency to 186 nm, including all beams, is roughly 2%. These wavelengths were chosen to demonstrate the utility of this type of frequency converter to generate wavelengths outside the transparency window of most crystalline media. Our technique involves the application of two strong laser fields which are almost two-photon resonant with a Raman transition of the Pb atoms.
We present a time-dependent calculation for four-wave mixing using a combination of long, short, and time delayed laser pulses in the context of electromagnetically induced transparency. Two transform limited nanosecond lasers are used to create a highly coherent mixture of the ground state and an excited state via a two-photon process. Once the induced transparency is established, a laser with short pulse length is injected after a suitable delay to generate four-wave mixing. We show that the wave mixing process is phase matched for all detunings, and with appropriately selected atomic coherence and populations, near 100% photon flux conversion efficiency can be obtained, independent of the intensity of the short pulse laser. In addition, we show that for small detunings for the short pulse laser, the four-wave mixing field travels with the speed of light in vacuum and suffers no pulse distortion even though the medium is highly dispersive at the frequency of the generated wave. These advantages open a door for future applications of the scheme for highly efficient, very stable UV generation.
Many of the most impressive demonstrations of the efficient generation of vacuum ultraviolet (VUV) light have made use of two‐photon resonantly enhanced four‐wave mixing to generate light at ωVUV =2ωL1±ωL2. The two‐photon resonance state is coupled to the ground state both by two photons from the first laser, or by a photon from the second laser and one from the generated VUV beam. We show here that these two coherent pathways destructively interfere once the second laser is made sufficiently intense, thereby leading to an important limiting effect on the achievable conversion efficiency.