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Applied Optics

Nonresonant third harmonic generation and the parametric process in Zn vapor

Shuo-Yan Zhao, Peilin Zhang, Guangzhi Zhang, Wenzheng Zhao

Published Nov 1, 1989• 2 citations
Publisher

Abstract

Nonresonant third harmonic generation with tuning range between 157.0-158.8 nm and 210.4-214.0 nm in zinc vapor is reported. Using two-photon excitation of Zn 4s4d(1)D(2), 4s6s(1)S(0), and 4s6d(1)D(2) states, parametric processes with signal waves 213.8 nm, 159.0 nm, and 145.8 nm are also investigated.
DOI
10.1364/ao.28.004521

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The authors present a detailed theoretical analysis of two-photon resonant third- and fifth-harmonic generation in metal vapors with picosecond laser pulses. These processes are described by self-consistent Maxwell-Bloch equations which take into account the effects of optical Stark shifts, multiphoton ionization, Doppler broadening, two-photon absorption, the reaction of the third-harmonic field on the fundamental, and a nonlinear index of refraction. As an example, a quantitative analysis of third- and fifth-harmonic generation in lithium vapor ($2s\ensuremath{-}4s$ transition) is presented. The limitations on energy conversion efficiency and the temporal as well as spectral characteristics of the harmonic pulses are investigated for two kinds of low-loss propagation fundamental pulses. It is shown that 90\ifmmode^\circ\else\textdegree\fi{} phase-shifted fundamental pulses (zero area) are more efficient than $2\ensuremath{\pi}m$ pulses. Energy conversion efficiencies of 6.5% for third-harmonic (190 nm) and 0.07% for cascade fifth-harmonic (114 nm) pulses are predicted.
We have investigated three resonant nonlinear processes in atomic cesium vapor. They are third harmonic generation, two photon absorption, and parametric frequency conversion. Resonant enhancement of each is provided by tuning the ruby laser half the 6S - 9D transition frequency of 28828.90 cm. The parametric process involves, in addition, a resonance with one of the P states. We have studied the variation of each of the three processes with laser intensity and frequency. At exact resonance the THG is found to be proportional to the square of the laser intensity and the TPA is proportional to laser intensity over a large power range. The resonance lineshape for both processes is found to be power dependent. A detailed analysis of these two processes based on steady state density matrix calculations and including A. C. Stark shifts, photoionization, and beam geometry is shown to accurately describe most of our observations.
The density-matrix formalism is used to develop the theory of two-photon-resonant third-harmonic generation in metal vapors taking into account saturation, ionization, laser-induced Stark shifts, and variations in the wave-vector mismatch as a result of population redistribution. It is shown that for third-harmonic generation in the ultraviolet and the vacuum-ultraviolet regions, where $3\ensuremath{\omega}$ exceeds the ionization limit of the metal vapor, two-photon-resonant three-photon ionization will be the main limiting process. This will also be true for four-wave parametric processes. For efficient energy conversion, the two-photon-resonant metal vapor must be phase matchable to allow large vapor density and cell length. Otherwise, the low incident intensity limits, set by the saturation and the ionization effects, cannot be efficiently converted in only one coherence length. The theory is applied to two-photon-resonant tripling of the ruby laser in cesium vapor.