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Laser Physics

Experimental preparation of the initial state of Xe+-N laser-induced collisional charge transfer system: Multi-photon resonant ionization of xenon

Hongying Zhang, Zhenzhong Lu, Rongwei Fan, Deying Chen

Published May 1, 2009• 3 citations
Publisher

Abstract

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.

DOI
10.1134/s1054660x09050090

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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.
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.
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.
Collisional relaxation of the 6s[3/2]10{[3/2]}_{1}^{0}[3/2]10​ and 6s'[1/2]10{[1/2]}_{1}^{0}[1/2]10​ mJ{m}_{J}mJ​ levels of Xe has been investigated both experimentally and theoretically. Collisional disalignment and dephasing of the mJ{m}_{J}mJ​ levels have been studied by measuring the pressure and laser intensity dependence of the ratio of the ionization from selectively excited mJ{m}_{J}mJ​=0 and \ifmmode\pm\else\textpm\fi{}1 sublevels in a three-photon resonant-ionization experiment via the 6s and 6s' states of Xe. The selective ionization is achieved by a novel use of two counterpropagating laser beams having parallel and orthogonal polarization, respectively. The pressure dependence of the ionization ratio has been calculated by solving a system of rate equations derived from a full set of density-matrix equations pertaining to the particular experimental conditions. Collisional-relaxation cross sections of the investigated levels have been estimated by fitting the calculated results to the experimental data. The ionization ratio is found to be sensitive to both disalignment and dephasing of the mJ{m}_{J}mJ​ levels.
Neutral Rydberg state excitation in strong UV laser fields of Xe atoms has been studied and compared with direct ionization. The yields of both strong-field excitation and ionization have been measured as a function of UV laser intensity and ellipticity. The underlying physical mechanism has been discussed based on the experimental results, indicating that the Rydberg states are populated via multi-photon resonance excitation in strong 400 nm laser fields. Finally, a comparative study of Xe and O2O_2O2​ with similar ionization potentials have been performed, showing the suppressed excitation of molecules in strong UV laser fields.
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.