Challenges
Datasets
Workspaces
Papers
Discussions
Leaderboard
Log inSign up
Challenges
Datasets
Workspaces
Papers
Discussions
Leaderboard
Blog
Job Board
Q3AS

© 2026 Aqora Quantum S.A.S.

TermsPrivacyLegal Notice

Physical Review A

Multiphoton ionization spectra and tunable fifth-harmonic production near five-photon resonances in Xe and Ar

W. R. Garrett, S. Henderson, M. G. Payne

Published Jun 1, 1987• 25 citations
Publisher

Abstract

Through multiphoton ionization measurements, we have observed the interference of five-photon and internally generated fifth-harmonic excitation processes in \ensuremath{\Delta}J=1 even-odd parity resonant transitions in Xe and Ar. In agreement with theory, these five-photon resonances are not observable in single-pass laser beams, but are convincingly observed in counterpropagating beams. In the negatively dispersive regions of the 5d${[3/2]}^{0}$J=1 level of Xe, tunable fifth-harmonic light is generated by phase matching with various buffer-gas mixtures. The fifth-harmonic profiles are in good agreement with calculated phase-matching curves.

DOI
10.1103/physreva.35.5032

Related papers

Cancellation effects in four-photon-resonant five-photon ionization through thenfJ=2 states of Xe

Dimitrios Charalambidis, X. Xing, J. Petrakis +1 more

Partial cancellation of the ionization signal in the four-photon-resonant five-photon ionization via J=2 4f and 5f resonances in Xe has been observed at increased gas pressures. Experiments with one and two counterpropagating laser beams provide strong evidence that cancellation is due to destructive interference at the three-photon step between the coherent three- and one-photon excitation channels, the latter involving one vacuum ultraviolet photon of the third-harmonic generation that occurs above the 6s[3/2${]}_{1}^{\mathit{o}}$ state. The well-known destructive interference for the ``on-resonance'' case is now shown to occur also for large detuning from the resonance (up to 2000 ${\mathrm{cm}}^{\mathrm{\ensuremath{-}}1}$) probed by four-photon-resonant five-photon ionization. This type of cancellation may provide a new insight in interference effects involved in multiphoton-excitation processes.

Physical Review A•Jul 1, 1991•19 citations

CANCELLATION EFFECTS IN 4-PHOTON-RESONANT 5-PHOTON IONIZATION THROUGH THE NF J=2 STATES OF XE

Dimitrios Charalambidis, Xianran Xing, J. Petrakis +1 more

Partial cancellation of the ionization signal in the four-photon-resonant five-photon ionization via J = 2 4f and 5f resonances in Xe has been observed at increased gas pressures. Experiments with one and two counterpropagating laser beams provide strong evidence that cancellation is due to destructive interference at the three-photon step between the coherent three- and one-photon excitation channels, the latter involving one vacuum ultraviolet photon of the third-harmonic generation that occurs above the 6s[3/2]1o state. The well-known destructive interference for the ''on-resonance'' case is now shown to occur also for large detuning from the resonance (up to 2000 cm-1) probed by four-photon-resonant five-photon ionization. This type of cancellation may provide new insight in interference effects involved in multiphoton-excitation processes.

•Jan 1, 1991•0 citations

Observation of laser-induced collisional energy transfer in xenon–argon mixtures

W. R. Garrett, S. Henderson, M. G. Payne

By using a multiphoton ionization technique, we observed a laser-induced energy-transfer process of fifth order in Xe–Ar atoms. Through four-photon excitation of the 4f[5/2]J = 2 level of Xe in collision with a ground-state Ar atom and the absorption of one additional photon, the 5s[3/2]J = 1 level of Ar is excited and subsequently ionized. By coincidence the same photon energy required for four-photon excitation of the chosen state in Xe is also adequate for absorption by Ar during the Xe*–Ar collision, thus permitting observation of a fifth-order laser-induced energy transfer in a simple one-color experiment.

Journal of the Optical Society of America B•Feb 1, 1987•4 citations

Theory of the effect of third-harmonic generation on three-photon resonantly enhanced multiphoton ionization in focused beams

M. G. Payne, W. R. Garrett

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 $n$-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.

Physical Review A•Dec 1, 1983•72 citations

Three-photon resonantly enhanced multiphoton ionization and third-harmonic generation with unfocused laser beams

M. G. Payne, W. R. Garrett, Wanda R. Ferrell

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.

Physical Review A•Aug 1, 1986•46 citations

Interference between nearly resonant three-photon excitation and third-harmonic generation probed by the cancellation of four-photon resonances

X. Xing, Dimitrios Charalambidis, E. Koutsourelaki +1 more

The destructive interference between the three-photon and the third-harmonic one-photon absorption in the vicinity of the 6s[3/2${]}_{1}$ state of Xe has been studied in the resonantly enhanced multiphoton ionization via nf states, through the cancellation of the nf, J=2 resonances of the spectrum, accessible by four-photon absorption. The gas-pressure, i.e., phase-matching, dependence of the three-photon detuning range from the 6s[3/2${]}_{1}$ state for which cancellation occurs has been investigated in one- and two-color experiments, including positive detuning from this state in positively dispersive regions. For obtaining cancellation, the theoretically predicted requirement of optically thick medium at the third-harmonic frequency is corroborated by present observations for negative detunings. The different cancellation behavior of the nf[3/2${]}_{2}$ and nf[5/2${]}_{2}$ states observed indicates the dependence of the effect on the atomic parameters of the coupled four-photon resonance. The experimental results are found to be in partial agreement with existing theoretical models.

Physical Review A•Mar 1, 1993•9 citations
Through multiphoton ionization measurements, we have observed the interference of five-photon and internally generated fifth-harmonic excitation processes in \ensuremath{\Delta}J=1 even-odd parity resonant transitions in Xe and Ar. In agreement with theory, these five-photon resonances are not observable in single-pass laser beams, but are convincingly observed in counterpropagating beams. In the negatively dispersive regions of the 5d[3/2]0{[3/2]}^{0}[3/2]0J=1 level of Xe, tunable fifth-harmonic light is generated by phase matching with various buffer-gas mixtures. The fifth-harmonic profiles are in good agreement with calculated phase-matching curves.
Partial cancellation of the ionization signal in the four-photon-resonant five-photon ionization via J=2 4f and 5f resonances in Xe has been observed at increased gas pressures. Experiments with one and two counterpropagating laser beams provide strong evidence that cancellation is due to destructive interference at the three-photon step between the coherent three- and one-photon excitation channels, the latter involving one vacuum ultraviolet photon of the third-harmonic generation that occurs above the 6s[3/2]1o{]}_{1}^{\mathit{o}}]1o​ state. The well-known destructive interference for the ``on-resonance'' case is now shown to occur also for large detuning from the resonance (up to 2000 ${\mathrm{cm}}^{\mathrm{\ensuremath{-}}1}$) probed by four-photon-resonant five-photon ionization. This type of cancellation may provide a new insight in interference effects involved in multiphoton-excitation processes.
Partial cancellation of the ionization signal in the four-photon-resonant five-photon ionization via J = 2 4f and 5f resonances in Xe has been observed at increased gas pressures. Experiments with one and two counterpropagating laser beams provide strong evidence that cancellation is due to destructive interference at the three-photon step between the coherent three- and one-photon excitation channels, the latter involving one vacuum ultraviolet photon of the third-harmonic generation that occurs above the 6s[3/2]1o state. The well-known destructive interference for the ''on-resonance'' case is now shown to occur also for large detuning from the resonance (up to 2000 cm-1) probed by four-photon-resonant five-photon ionization. This type of cancellation may provide new insight in interference effects involved in multiphoton-excitation processes.
By using a multiphoton ionization technique, we observed a laser-induced energy-transfer process of fifth order in Xe–Ar atoms. Through four-photon excitation of the 4f[5/2]J = 2 level of Xe in collision with a ground-state Ar atom and the absorption of one additional photon, the 5s[3/2]J = 1 level of Ar is excited and subsequently ionized. By coincidence the same photon energy required for four-photon excitation of the chosen state in Xe is also adequate for absorption by Ar during the Xe*–Ar collision, thus permitting observation of a fifth-order laser-induced energy transfer in a simple one-color experiment.
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.
The destructive interference between the three-photon and the third-harmonic one-photon absorption in the vicinity of the 6s[3/2]1{]}_{1}]1​ state of Xe has been studied in the resonantly enhanced multiphoton ionization via nf states, through the cancellation of the nf, J=2 resonances of the spectrum, accessible by four-photon absorption. The gas-pressure, i.e., phase-matching, dependence of the three-photon detuning range from the 6s[3/2]1{]}_{1}]1​ state for which cancellation occurs has been investigated in one- and two-color experiments, including positive detuning from this state in positively dispersive regions. For obtaining cancellation, the theoretically predicted requirement of optically thick medium at the third-harmonic frequency is corroborated by present observations for negative detunings. The different cancellation behavior of the nf[3/2]2{]}_{2}]2​ and nf[5/2]2{]}_{2}]2​ states observed indicates the dependence of the effect on the atomic parameters of the coupled four-photon resonance. The experimental results are found to be in partial agreement with existing theoretical models.