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Journal of the Optical Society of America B

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

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

Published Feb 1, 1987• 4 citations
Publisher

Abstract

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.

DOI
10.1364/josab.4.000133

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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.
This paper proposes a novel one-colour Xe–Kr laser induced collisional ionization system. Considering the level scheme of the system, it finds that the initial state of the reaction–the four 4f levels with even J of Xe–can be prepared through method of four-photon resonant excitation by dye laser with wavelength of ∼440 nm. Absorption of an additional photon (the transfer laser) of the same wavelength will complete the laser induced collisional ionization process. The resonance enhanced ionization spectrum of Xe by four laser photons at ∼440 nm is measured through time-of-flight mass spectrometry, this aims at the preparation of the initial state of the system proposed. The Stark broadening of the measured spectrum is observed and consistent with the previous study. Analysis of the measured resonance ionization spectrum implies the feasibility of ∼440 nm four-photon resonant excitation of the initial 4f state of the Xe–Kr system proposed in this paper, which prepares for a further experiment of laser induced collisional ionization.
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.
Thermal collisions between laser excited Xe(nf) Rydberg atoms and a variety of neutral atomic and molecular targets have been investigated. In Xe(nf)-HF collisions, n-changing, 4-changing and collisional ionization were observed. For n = 26 and 27, absolute collisional cross sections for these processes have been determined using time-resolved selective field ionization. In addition, the first evidence of molecular rotational excitation through the transfer of energy of electronic excitation from a Rydberg atom is presented. In Xe(nf) - Xe, Kr, Ar, CO2, CO and N2 collisions the dominant mechanism was observed to be 4-changing: no evidence of n-changing or collisional ionization was apparent. Absolute collisional cross sections have been determined for a range of n between 24 and 37. Comparison of these cross sections with those obtained using a theoretical model in which effects due to the Rydberg core are ignored appears to lead to satisfactory results only for Xe, Kr and CO2, whereas when core effects are included satisfactory agreement between experiment and theory is found in all cases.
A novel one-color Xe + -N laser induced collisional charge transfer system is proposed, and preparation of the initial state of the system, i.e., Xe + is experimentally implemented through resonance enhanced multi-photon ionization (REMPI) by ∼440 nm dye laser. The REMPI of Xe is experimentally investigated through time-of-flight (TOF) mass spectrometry and the intensity dependence of Xe + is obtained, aiming at the preparation of Xe + . The resonant ionization spectra of Xe at ∼440 nm under several different conditions are measured, showing the impacts of mode purification and source pressure on the resonant ionization spectrum. The results indicate the feasibility of preparing the initial state of the Xe + -N system by ∼440 nm multi-photon resonant ionization, which prepares for a further experiment of laser-induced collisional charge transfer.
The cross sections for the excitation energy transfer induced by collisions with He, Ar and Na ground-state atoms have been measured. The sodium atoms in the 4D state have been produced by two-photon excitation using cw laser radiation at 578.89 nm. Within a model which takes into account collisional population and depopulation of the 4F level as well as radiative relaxation (direct or cascade) of the 3D, 4P, 4D and 4F states ending in the 3P level, the rate for the collisional transfer turns out to be related to the ratio of the steady-state populations created in 3D and 4D states. They have been determined by measuring the fluorescence intensities of the and transitions. The measurements yield the following cross section values for those processes investigated: , and , at .