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Journal of Physics B Atomic and Molecular Physics

Theory of two-photon resonant third-harmonic generation with ultrashort pulses. III. Index mismatching, detuning and spectral effects

J N Elgin, G.H.C. New, J. M. Catherall

Published Aug 14, 1980• 4 citations
Publisher

Abstract

The analysis of two-photon resonant third-harmonic generation is generalised to include, in particular, the effects of imperfect index matching and two-photon tuning. Furthermore, whereas previously the authors considered only the temporal properties of the generated harmonic signal, here is spectral characteristics are also considered. The authors comment on a discrepancy between the predictions of semiclassical and quantised field formalisms. In the semiclassical analysis, it is shown that for large energy input pulses the harmonic spectrum is double peaked even near exact resonance and that this structure can be interpreted in terms of transitions between sets of doublet states of the Autler-Townes (1955) type. In a quantised field formalism, however, the picture is radically altered near exact resonance where a three-peaked spectrum is predicted.

DOI
10.1088/0022-3700/13/15/021

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Effects of four-wave mixing on four-photon resonance excitation and ionization in the presence of a three-photon intermediate state resonance enhancement

M. G. Payne, J. C. Miller, Roger C. Hart +1 more

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}${\mathit{k}}_{\mathit{r}}$L\ensuremath{\Vert}\ensuremath{\gg}1, where \ensuremath{\Delta}${\mathit{k}}_{\mathit{r}}$ 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}${\mathit{k}}_{\mathit{r}}$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.

Physical Review A•Dec 1, 1991•19 citations
The analysis of two-photon resonant third-harmonic generation is generalised to include, in particular, the effects of imperfect index matching and two-photon tuning. Furthermore, whereas previously the authors considered only the temporal properties of the generated harmonic signal, here is spectral characteristics are also considered. The authors comment on a discrepancy between the predictions of semiclassical and quantised field formalisms. In the semiclassical analysis, it is shown that for large energy input pulses the harmonic spectrum is double peaked even near exact resonance and that this structure can be interpreted in terms of transitions between sets of doublet states of the Autler-Townes (1955) type. In a quantised field formalism, however, the picture is radically altered near exact resonance where a three-peaked spectrum is predicted.
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.
Multiphoton ionization in the region near a three-photon resonance is treated for focused, plane-polarized Gaussian beams with diffraction-limited beam divergence. In this situation, a third-harmonic field is generated within the laser beam. At, and very near, three-photon resonance the driving rate for the upper-state probability amplitude due to one-photon absorption of third-harmonic light becomes nearly equal to the corresponding three-photon rate due to the laser field, but these effects are 180\ifmmode^\circ\else\textdegree\fi{} out of phase. As a consequence of this cancellation between two pumping terms, the three-photon resonance line essentially disappears at moderate concentrations and the observed ionization has a line shape that is close to the phase-matching curve for third-harmonic generation. The ionization signal, near but not on the resonance, is due almost entirely to absorption of third-harmonic photons plus other laser photons; three-photon resonantly enhanced multiphoton ionization by the laser is much weaker. This is particularly true on the blue side of the three-photon resonance at detunings where phase matching occurs. The problem is treated quite generally with predictions of the full line shape for nnn-photon ionization and third-harmonic light generation near three-photon resonance, including the rather strong influences of positively dispersive buffer gases. We also show that the cancellation between the one-photon and the three-photon process is partially spoiled in the presence of a counterpropagating beam at the same frequency.
Several extensions are made in theoretical studies of multiphoton ionization associated with third-harmonic fields that are generated near three-photon resonances in gaseous media. The treatment includes the strong coherent cancellation effect which occurs between three-photon pumping of a resonant level and pumping by the third-harmonic field that is generated in the same medium. The incomplete spoiling of the cancellation effect with counterpropagating beams is quantitatively described. Also, treatment of the multiphoton-ionization problem involving phase-matched, third-harmonic fields is generalized to include quantitative effects of index changes due to a buffer gas, absorption due to dimers, and collisional dephasing of coherent excitations. Finally, we show how measurements of linewidths, phase-matching positions, and pressure dependences of ionization yields associated with third-harmonic generation and subsequent absorption can be used to determine oscillator strengths of a resonant level, absorption coefficients for a resonant species and a buffer-gas species, and the refractive index of the buffer gas at the third-harmonic frequency.
This work examines the use of higher order multiphoton resonances in higher harmonic generation together with judicious exploitation of coherent interaction properties to achieve efficient harmonic generation. A detailed experimental study on third harmonic generation in two photon resonant coherent interaction and a theoretical study on four photon resonant coherent interaction have been conducted. Two photon resonant coheren propagation in lithium vapor (2S-4S and 2S-3D interaction) has been studied in detail as a function of phase and delay of the interacting pulse sequence. Under coherent lossless propagation of 90 phase shifted pulse pair, third harmonic generation is enhanced. A maximum energy conversion efficiency of 1% was measured experimentally. This experiment shows that phase correlated pulse sequence can be used to control multiphoton coherent resonant effects. A larger two photon resonant enhancement does not result in more efficient harmonic generation, in agreement with the theoretical prediction. An accurate (to at least 0.5 A°) measurement of intensity dependent Stark shift has been done with the newly developed "interferometric wavemeter." Stark shifts as big as several pulse bandwidths (of picosecond pulses) result in a poor tuning of multiphoton resonance and become a limiting factor of resonant harmonic generation. A complete theory has been developed for harmonic generation in a four photon resonant coherent interaction. A numerical application of the theory to the Hg atom successfully interprets the experimental observations in terms of the phase dependent stimulated Raman scattering. With the intensity required for four photon resonant transition, the calculation predicts a dramatic Stark shift effect which completely destroys the resonance condition. This model provides a basis for the development of future schemes for efficient higher order coherent upconversion.
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.