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

Near-resonance three-photon excitation profiles in xenon with segmented conical beams

Viktor E. Peet, W. R. Garrett, Sergei Shchemeljov

Published Jan 8, 2001• 8 citations
Publisher

Abstract

Multiphoton ionization profiles in xenon under three-photon excitation by azimuthally segmented conical laser beams have been studied and analyzed on the basis of the interference-based cooperative shift of the atomic resonance line. Segmentation of the conical wave front with various geometrical slits reduces the possible three-photon azimuthal sub-beam combinations in the third order process and a principal (or ``homogeneous'') Lorentzian component can be selected from the overall excitation profile. This Lorentzian is identical to the pressure-broadened atomic line shifted by the cooperative shift. A possibility of controlling the nonlinear response by spatial selection of interacting waves in conical beams is discussed.

DOI
10.1103/physreva.63.023804

Related papers

Wave-mixing effects in resonance-enhanced multiphoton ionization of xenon in Bessel beams

W. R. Garrett, Viktor E. Peet

Three-photon-resonant excitation and subsequent ionization of xenon at high concentrations has been studied utilizing both Bessel and Gaussian beams. Comparisons of analogous results with the two modes of focusing are made. The excitation-ionization profiles can be analyzed on the basis of the well-studied interference effect involving combined contributions of three- and one-photon transition amplitudes in resonant atomic excitation. We show that the principal features of the excitation problem with Bessel beams can be simulated by a simple picture involving crossed plane-wave beams. Using this approach it has been shown that pressure-broadened and shifted lines that result from the interference-based cooperative Lorentzian line shift constitutes the main pressure-dependent peak of off-resonance excitation profiles produced in Bessel beams.

Physical Review A•May 9, 2000•14 citations

Three-photon resonant atomic excitation in spatially incoherent laser beams

Viktor E. Peet, Sergei Shchemeljov

Two-color excitation by spatially coherent and incoherent laser beams has been used to study three-photon-resonant excitation and subsequent ionization of xenon in conditions, when internally generated sum-frequency field plays an important role in excitation of atomic resonances through interfering one-photon excitation pathway. We show that the incoherence in one of the pumping fields reduces the efficiency of generated sum-frequency field, and thus suppresses the interference between the three- and the one-photon excitation channels. The degree of suppression is controlled by varying the crossing angle between coherent and incoherent laser beams. We show that ionization profiles can be analyzed on the basis of the well-studied interference of one- and three-photon transition amplitudes, but with pumping field decomposed into multiple small-scale uncorrelated domains where coherent process of four-wave mixing occurs. The gain length for a coherent process in these domains depends on the coherence degree and excitation geometry. It gives a possibility of controlling the contribution of coherent processes to the excitation of multiphoton resonances.

Physical Review A•Oct 22, 2003•4 citations

Third-harmonic generation and multiphoton ionization in Bessel beams

Viktor E. Peet, R.V. Tsubin

Three-photon resonance enhancement of third-harmonic generation and multiphoton ionization have been studied in xenon under excitation by the Bessel and the focused annular laser beams. It has been shown that the transformation of a Gaussian beam into a Bessel or an annular one leads to significant changes of third-harmonic excitation profiles and ionization spectra. These changes result from a principal difference of the beams, where either collinear (Gaussian beams) or noncollinear (Bessel and focused annular beams) excitation geometries are realized. It has been shown that the noncollinear ring-type phase matching shifts the maximum of the generated third harmonic to the longer wavelength toward the atomic resonance. Numerical calculations of third-harmonic excitation spectra have been carried out and compared with experimental results. The efficiency of frequency tripling in collinear and noncollinear excitation geometries have been compared. Cancellation of the three-photon $6s$ resonance and the influence of harmonic photons on the excitation of the four-photon $4f$ resonance in the Bessel beams are discussed.

Physical Review A•Aug 1, 1997•61 citations

Wave-mixing interference in three-photon resonant atomic excitation with cross-polarized angled beams

Viktor E. Peet

Three-photon excitation and associated wave mixing near the $6s$ and $6{s}^{\ensuremath{'}}$ resonances of xenon have been studied utilizing resonance-enhanced multiphoton ionization in angled beams with different polarizations. It has been shown that a complete cancellation of three-photon resonant atomic excitation caused by the well-known destructive wave-mixing interference occurs in $s$ and $p$ polarization of angled beams but distinct resonance ionization enhancement is observed when pump beams have orthogonal polarization planes. Pressure-induced evolution of the resonance ionization peak in cross-polarized beams is identical to that observed with counterpropagating beams. The reason for such resonance ionization enhancement is unknown and cannot be explained within the frame work of existing theory. The effect may result from some peculiarities of wave-mixing interference in a multilevel atomic system, where different degenerate magnetic sublevels of the upper atomic state and multiple interfering excitation processes are involved. Another possibility is that the resonance ionization enhancement results from a process where weak counterpropagating light is generated within the excitation region of cross-polarized angled beams.

Physical Review A•Sep 15, 2006•4 citations

Two-color multiphoton ionization of xenon

R. N. Compton, John C. Miller

Two independently tunable, linearly polarized dye lasers have been used to study multiphoton ionization of gaseous xenon. One laser is tuned near three-photon resonance with the allowed 6s[3/2]J=1° resonance, which is not observed with one laser at these pressures because of the destructive interference between the three-photon-excitation and third-harmonic-excitation pathways to the 6s[3/2]J=1° state. The second laser is tuned to resonance with higher allowed np and np′ states of xenon. The missing ionization signal is seen to be dramatically restored by the addition of the second laser beam; however, the signal again disappears as the pressure is increased. These results are discussed in relation to recent experimental and theoretical studies of cancellation effects between three-photon excitation and third-harmonic generation. Spectroscopic information obtained from tuning each dye laser, together with data on the angular distributions resulting from rotating the plane of polarization of one laser relative to that of the second laser, clearly shows that two different ionization mechanisms are operative. In addition, these experiments unambiguously illustrate the importance of dissociative ionization of quasi-dimers of xenon over a rather broad frequency range.

Journal of the Optical Society of America B•Feb 1, 1985•37 citations

Extreme pressure broadening of three-photon resonances in noble gases

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

A pressure-broadening study of three-photon and one-photon resonances was performed using counterpropagating, linearly polarized laser beams. Self-broadening, as well as the collision-induced effects due to the presence of a second noble gas, was investigated for the 6s, 6s′, 5d and 7s of xenon and the 5s′ of krypton. A multiphoton ionization scheme in a calibrated proportional counter is the basis of a new technique by which collisional processes can be investigated for high pressure regimes which have previously been inaccessible to investigation, particularly for self-broadening where the mean free path of the photons is of the order of 10−3 cm for pressures as low as 1 Torr. Using this technique, we have recorded the collision-induced widths and shifts of the resonance for pressures up to 1000 Torr. In the hundreds of torr range, asymmetric, self-broadening line shapes were observed with full widths and shifts which were greater than five times the laser bandwidth (0.002-0.005 nm).

Annual Meeting Optical Society of America•Jan 1, 1985•1 citation
Multiphoton ionization profiles in xenon under three-photon excitation by azimuthally segmented conical laser beams have been studied and analyzed on the basis of the interference-based cooperative shift of the atomic resonance line. Segmentation of the conical wave front with various geometrical slits reduces the possible three-photon azimuthal sub-beam combinations in the third order process and a principal (or ``homogeneous'') Lorentzian component can be selected from the overall excitation profile. This Lorentzian is identical to the pressure-broadened atomic line shifted by the cooperative shift. A possibility of controlling the nonlinear response by spatial selection of interacting waves in conical beams is discussed.
Three-photon-resonant excitation and subsequent ionization of xenon at high concentrations has been studied utilizing both Bessel and Gaussian beams. Comparisons of analogous results with the two modes of focusing are made. The excitation-ionization profiles can be analyzed on the basis of the well-studied interference effect involving combined contributions of three- and one-photon transition amplitudes in resonant atomic excitation. We show that the principal features of the excitation problem with Bessel beams can be simulated by a simple picture involving crossed plane-wave beams. Using this approach it has been shown that pressure-broadened and shifted lines that result from the interference-based cooperative Lorentzian line shift constitutes the main pressure-dependent peak of off-resonance excitation profiles produced in Bessel beams.
Two-color excitation by spatially coherent and incoherent laser beams has been used to study three-photon-resonant excitation and subsequent ionization of xenon in conditions, when internally generated sum-frequency field plays an important role in excitation of atomic resonances through interfering one-photon excitation pathway. We show that the incoherence in one of the pumping fields reduces the efficiency of generated sum-frequency field, and thus suppresses the interference between the three- and the one-photon excitation channels. The degree of suppression is controlled by varying the crossing angle between coherent and incoherent laser beams. We show that ionization profiles can be analyzed on the basis of the well-studied interference of one- and three-photon transition amplitudes, but with pumping field decomposed into multiple small-scale uncorrelated domains where coherent process of four-wave mixing occurs. The gain length for a coherent process in these domains depends on the coherence degree and excitation geometry. It gives a possibility of controlling the contribution of coherent processes to the excitation of multiphoton resonances.
Three-photon resonance enhancement of third-harmonic generation and multiphoton ionization have been studied in xenon under excitation by the Bessel and the focused annular laser beams. It has been shown that the transformation of a Gaussian beam into a Bessel or an annular one leads to significant changes of third-harmonic excitation profiles and ionization spectra. These changes result from a principal difference of the beams, where either collinear (Gaussian beams) or noncollinear (Bessel and focused annular beams) excitation geometries are realized. It has been shown that the noncollinear ring-type phase matching shifts the maximum of the generated third harmonic to the longer wavelength toward the atomic resonance. Numerical calculations of third-harmonic excitation spectra have been carried out and compared with experimental results. The efficiency of frequency tripling in collinear and noncollinear excitation geometries have been compared. Cancellation of the three-photon 6s6s6s resonance and the influence of harmonic photons on the excitation of the four-photon 4f4f4f resonance in the Bessel beams are discussed.
Three-photon excitation and associated wave mixing near the 6s6s6s and $6{s}^{\ensuremath{'}}$ resonances of xenon have been studied utilizing resonance-enhanced multiphoton ionization in angled beams with different polarizations. It has been shown that a complete cancellation of three-photon resonant atomic excitation caused by the well-known destructive wave-mixing interference occurs in sss and ppp polarization of angled beams but distinct resonance ionization enhancement is observed when pump beams have orthogonal polarization planes. Pressure-induced evolution of the resonance ionization peak in cross-polarized beams is identical to that observed with counterpropagating beams. The reason for such resonance ionization enhancement is unknown and cannot be explained within the frame work of existing theory. The effect may result from some peculiarities of wave-mixing interference in a multilevel atomic system, where different degenerate magnetic sublevels of the upper atomic state and multiple interfering excitation processes are involved. Another possibility is that the resonance ionization enhancement results from a process where weak counterpropagating light is generated within the excitation region of cross-polarized angled beams.
Two independently tunable, linearly polarized dye lasers have been used to study multiphoton ionization of gaseous xenon. One laser is tuned near three-photon resonance with the allowed 6s[3/2]J=1° resonance, which is not observed with one laser at these pressures because of the destructive interference between the three-photon-excitation and third-harmonic-excitation pathways to the 6s[3/2]J=1° state. The second laser is tuned to resonance with higher allowed np and np′ states of xenon. The missing ionization signal is seen to be dramatically restored by the addition of the second laser beam; however, the signal again disappears as the pressure is increased. These results are discussed in relation to recent experimental and theoretical studies of cancellation effects between three-photon excitation and third-harmonic generation. Spectroscopic information obtained from tuning each dye laser, together with data on the angular distributions resulting from rotating the plane of polarization of one laser relative to that of the second laser, clearly shows that two different ionization mechanisms are operative. In addition, these experiments unambiguously illustrate the importance of dissociative ionization of quasi-dimers of xenon over a rather broad frequency range.
A pressure-broadening study of three-photon and one-photon resonances was performed using counterpropagating, linearly polarized laser beams. Self-broadening, as well as the collision-induced effects due to the presence of a second noble gas, was investigated for the 6s, 6s′, 5d and 7s of xenon and the 5s′ of krypton. A multiphoton ionization scheme in a calibrated proportional counter is the basis of a new technique by which collisional processes can be investigated for high pressure regimes which have previously been inaccessible to investigation, particularly for self-broadening where the mean free path of the photons is of the order of 10−3 cm for pressures as low as 1 Torr. Using this technique, we have recorded the collision-induced widths and shifts of the resonance for pressures up to 1000 Torr. In the hundreds of torr range, asymmetric, self-broadening line shapes were observed with full widths and shifts which were greater than five times the laser bandwidth (0.002-0.005 nm).