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AIP conference proceedings

Effect of the coherent cancellation of the two-photon resonance on the generation of vacuum ultraviolet light by two-photon resonantly enhanced four-wave mixing

M. G. Payne, W. R. Garrett, J. P. Judish, Rainer Wunderlich

Published Jan 1, 1989• 0 citations
Publisher

Abstract

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.

DOI
10.1063/1.38564

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Physical Review A•Dec 1, 1991•19 citations
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.
Vacuum ultraviolet light in the range 116 nm to 117 nm was produced by using a two‐photon resonant four‐wave mixing scheme in Xe. The buildup of coherent cancellation of the two‐photon resonant transition employed in the generation of the vacuum ultraviolet, with resulting limitations imposed on the achievable vacuum ultraviolet intensity was investigated. Under certain predicted conditions, increases in the intensity of one of the pumping beams, ≊1500 nn infrared, or tuning this beam towards resonance with the 5p 57s(3/2)1 level of Xe led, not to increases, but decreases in the vacuum ultraviolet generated.
Vacuum ultraviolet light in the range 116 nm to 117 nm was produced by using a two-photon resonant four-wave mixing scheme in Xe. The buildup of coherent cancellation of the two-photon resonant transition employed in the generation of the vacuum ultraviolet, with resulting limitations imposed on the achievable vacuum ultraviolet intensity was investigated. Under certain predicted conditions, increases in the intensity of one of the pumping beams, approx.1500 nm infrared, or tuning this beam towards resonance with the 5p/sup 5/7s(3/2)/sub 1/ level of Xe led, not to increases, but decreases in the vacuum ultraviolet generated. 3 refs., 3 figs.
We present experimental data on the coherent control of frequency conversion toward the vacuum-ultraviolet regime in xenon atoms, applying intense ultrashort picoseconds (ps) radiation pulses. We report on quantum interference between two resonantly enhanced frequency conversion processes (i.e., fifth harmonic generation and four-wave mixing). The conversion processes are driven by a fundamental (ps) laser pulse at 530 nm and the phase-locked second harmonic at 265 nm. Both fifth harmonic generation and four-wave mixing yield vacuum-ultraviolet radiation at 106 nm. The two frequency conversion pathways interfere with each other---either constructively or destructively, depending on the relative phase of the driving laser pulses. Thus, by variation of the relative phase, we substantially enhance or reduce the conversion efficiency (i.e., the yield of generated vacuum-ultraviolet radiation).
Coherent radiation at several wavelengths in the vacuum ultraviolet (VUV) has been generated by four-wave parametric oscillation in mercury vapor. When a powerful ultraviolet pump laser of frequency omega(p) is tuned to a two-photon resonance, VUV signal photons at frequency omega(s), as well as idler photons at frequency omega(i), are generated such that omega(s) + omega(i) = 2omega(p). A frequency-doubled dye laser tuned to two-photon resonance with the 6s6d(1)D(2) level near 280.3 nm produced output at 184.9 and 143.5 nm. A tunable krypton fluoride excimer laser tuned to two-photon resonance with the 6s10s (1)S(0) level near 248.7 nm produced output at 140.1, 130.7, 130.1, 125.9, and 125.0 nm. Approximately 1-microJ, 200-W pulses were observed at 143.5 and 125.9 nm.
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 ${4p}^{5}5p[0,\frac{1}{2}]{\ensuremath{-}4p}^{5}5s[1,\frac{1}{2}]$ 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 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 consider effects which occur when four-wave sum frequency generation and multiphoton ionization are induced by lasers tuned near a three-photon resonance and simultaneously near or at a dipole allowed four-photon resonance. In studies with unfocused laser beams, if the phase mismatch of the generated four-wave-mixing field is large and the related two-photon resonance for the absorption of a four-wave-mixing photon and a laser photon results in strong absorption of the four-wave-mixing field, a coherent cancellation occurs between the pumping of the resonance by two- and four-photon processes. This interference effect occurs when the first laser is tuned on either side of the three-photon resonance and \ensuremath{\Vert}\ensuremath{\Delta}kr{\mathit{k}}_{\mathit{r}}kr​L\ensuremath{\Vert}\ensuremath{\gg}1, where \ensuremath{\Delta}kr{\mathit{k}}_{\mathit{r}}kr​ is the mismatch and L is the length of the path of the laser beams in the gas. With focused laser beams large differences occur between ionization with unidirectional beams and with counterpropagating laser beams when \ensuremath{\Vert}\ensuremath{\Delta}kr{\mathit{k}}_{\mathit{r}}kr​b\ensuremath{\Vert}\ensuremath{\gg}1, where b is the confocal parameter of the focused laser beams. Strong absorption of the four-wave-mixing field is shown not to be necessary for strong destructive interference with focused laser beams when the phase mismatch is large. This work also suggests an explanation for earlier experiments where the presence of a four-photon resonance enabled the generation of third-harmonic light in a positively dispersive wavelength region. We argue that this process can occur when the laser used to achieve the four-photon resonance is focused on the small z (z is the coordinate in the direction of propagation) side of the focal point of the laser responsible for the third-harmonic generation. In this way the absorption of the third-harmonic light on one side of the focal point is made much stronger than on the other side. Correspondingly, contributions to the third-harmonic field from the two sides of the focal point are unequal and cannot undergo complete destructive interference as would otherwise occur in a positively dispersive region.