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Bulletin of the Chemical Society of Japan

m j -Resolved Doppler Spectroscopy of Cs(6p2P3/2,m j) Atoms Predissociated from a Single Level Cs2D1Σu+ (v = 46, J = 54)

Kensuke Matsubara, Yumi Tajima, Masaaki Baba, Jun Kawai, Hajime Katô

Published Oct 1, 1996• 2 citations
Publisher

Abstract

Abstract In a plane perpendicular to a magnetic field a collimated cesium beam was crossed at right angles by a pump laser beam. Cs2 molecules were excited to the D1Σu+ (v = 46, J = 54) level, which predissociated selectively to Cs(6s2S1/2) + Cs(6p2P3/2) atoms. The mj-resolved excitation spectra of the Cs(8s2S1/2,m′j ← 6p2P3/2,mj) transitions at a magnetic field of 1.91 kG were measured using a probe laser beam propagated either along the magnetic field or along the pump beam. The population of Cs(6p2P3/2,mj) atoms was found to be in the ratio 77 : 136 : 100 : 46 for mj = 3/2, 1/2, −1/2, and −3/2 based on an analysis of the line intensities. From the line shapes of the excitation spectra, Cs(6p2P3/2,±1/2) atoms were found to recoil predominantly parallel to the magnetic field H, and Cs(6p2P3/2,±3/2) atoms were found to recoil predominantly perpendicular to H.

DOI
10.1246/bcsj.69.2839

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The saturated absorption spectrum of Cs D 2 line has been measured by using a diode laser.The anomalies of the line intensities in the closed transitions are detected at several polarization configuration of the pump and probe beams.Weak magnetic fields of parallel and perpendicular to the laser beam are applied to identify the population trapping effect in the closed transition of F ′′ = 3 → F ′ = 2 and F ′′ = 4 → F ′ = 5.In case of the F ′′ = 3 → F ′ = 2 transition, the line intensity is controlled by polarization configuration and external magnetic field.

•Jan 1, 2012•0 citations
Abstract In a plane perpendicular to a magnetic field a collimated cesium beam was crossed at right angles by a pump laser beam. Cs2 molecules were excited to the D1Σu+ (v = 46, J = 54) level, which predissociated selectively to Cs(6s2S1/2) + Cs(6p2P3/2) atoms. The mj-resolved excitation spectra of the Cs(8s2S1/2,m′j ← 6p2P3/2,mj) transitions at a magnetic field of 1.91 kG were measured using a probe laser beam propagated either along the magnetic field or along the pump beam. The population of Cs(6p2P3/2,mj) atoms was found to be in the ratio 77 : 136 : 100 : 46 for mj = 3/2, 1/2, −1/2, and −3/2 based on an analysis of the line intensities. From the line shapes of the excitation spectra, Cs(6p2P3/2,±1/2) atoms were found to recoil predominantly parallel to the magnetic field H, and Cs(6p2P3/2,±3/2) atoms were found to recoil predominantly perpendicular to H.
In a magnetic field, the wave number of a pump laser light polarized along the field was fixed to the isolated ${\mathrm{Cs}}_{2}D{}^{1}{\ensuremath{\Sigma}}_{u}^{+}(v=46,J=54)\ensuremath{\leftarrow}X{}^{1}{\ensuremath{\Sigma}}_{g}^{+}(v=0,J=55)$ line, and the excitation spectrum of the dissociated Cs(6p2P3/2)\mathrm{Cs}(6p{}^{2}{P}_{3/2})Cs(6p2P3/2​) atoms was measured by scanning the wave number of a probe laser light polarized perpendicular to the field. The population of each sublevel 6p2P3/2,mj6p{}^{2}{P}_{{3/2,m}_{j}}6p2P3/2,mj​​ of the dissociated atoms was determined from the line intensities in the mj{m}_{j}mj​-resolved excitation spectrum. The unequal population between the 6p2P3/2,+∣mj∣6p{}^{2}{P}_{3/2,+|{m}_{j}|}6p2P3/2,+∣mj​∣​ and $6p{}^{2}{P}_{3/2,\ensuremath{-}|{m}_{j}|}$ levels (atomic orientation) was observed and it was enhanced as the magnetic-field strength was increased. The atomic orientation is shown to be induced by the interference between the indirect predissociation, which occurs by a combination of the spin-orbit coupling of the $D{}^{1}{\ensuremath{\Sigma}}_{u}^{+}$ state with the ${(2)}^{3}{\ensuremath{\Pi}}_{0u}$ state and the L-uncoupling and Zeeman interactions between the ${(2)}^{3}{\ensuremath{\Pi}}_{0u}$ and dissociative ${(2)}^{3}{\ensuremath{\Sigma}}_{u}^{+}$ states, and the dissociation following a direct excitation to the ${(2)}^{3}{\ensuremath{\Sigma}}_{u}^{+}$ state, which is allowed by spin-orbit coupling of the ${(2)}^{3}{\ensuremath{\Sigma}}_{u}^{+}$ state with the $B{}^{1}{\ensuremath{\Pi}}_{u}$ state. It is demonstrated that the atomic orientation is produced by the photodissociation in the presence of an external magnetic field even when all degenerated molecular $M=J,\dots{},0,\dots{},\ensuremath{-}J$ sublevels are excited by a light polarized linearly along the field.
Preferential population of the magnetic sublevels of Cs(6p 2P3/2) atoms produced by predissociation of the C 1Πu state of the Cs2 molecule along the repulsive molecular state b 3Σ+u , has been found by observing the polarization of the atomic fluorescence Cs(6p 2Pm3/2→6s 2S1/2). By applying an external magnetic field, we have determined the population of the magnetic sublevels Cs(6p 2Pm3/2) directly from the intensities of the fluorescence lines Cs(6p 2Pm3/2 →6s 2Sm±11/2 ) split by the Zeeman effect. The results are analyzed theoretically by assuming the separability of electronic and nuclear motion for the dissociation along the repulsive potential curve. The effect of the external magnetic field on the photodissociation has been made clear, and the observed results could be fully explained on the basis of the adiabatic approximation.
Populations of the n 2L(nL=7p,6D)states of Cs atoms by photodissociation of Cs_2 molecules through the use of the fixed frequence line 441.6nm of a He-Cd laser radiation are produced.Combining ratios of atomic to molecular fluorescence at the Cs density range between 1 and 9×10 15 cm -3 ,the ratios of collisional excitation transfer rate coefficients and the predissociation rates are obtained.The cross section for the fine-structure-changing collision [i.e,Cs(7P_ 1/2 )+Cs(6S)Cs(7P_ 3/2 )+Cs(6S)]is 3.5×10 -14 cm 2.
The cross sections for disorientation of magnetically oriented 62P126^{2}P_{\frac{1}{2}}62P21​​ cesium atoms, induced in collisions with noble gases, have been determined using Zeeman-scanning techniques at kilogauss magnetic fields. The ${m}_{J}=\ensuremath{-}\frac{1}{2}$, ${m}_{I}=\ensuremath{-}\frac{7}{2}$ hyperfine Zeeman substate was populated selectively by irradiating the cesium-vapor-noble-gas mixture with cesium-resonance radiation, and collisional transitions to the mJ=+12{m}_{J}=+\frac{1}{2}mJ​=+21​, ${m}_{I}=\ensuremath{-}\frac{7}{2}$ substate were monitored by measurements of the relative intensities of the ${\ensuremath{\sigma}}^{\ensuremath{-}}$ and ${\ensuremath{\sigma}}^{+}$ components in resonance fluorescence observed in the direction parallel to the magnetic field. The following cross sections were obtained: Cs-He, 11.8 A˚2{\mathrm{\AA{}}}^{2}A˚2; Cs-Ne, 4.7 A˚2{\mathrm{\AA{}}}^{2}A˚2; Cs-Ar, 10.7 A˚2{\mathrm{\AA{}}}^{2}A˚2; Cs-Kr, 37.9 A˚2{\mathrm{\AA{}}}^{2}A˚2; Cs-Xe, 71.7 A˚2{\mathrm{\AA{}}}^{2}A˚2.
The line shape of the saturated absorption spectra of the 133Cs D2 line was examined. In particular, the resonance signal for the transition from 6S1/2, F=4 to 6P3/2, F ′=5 was carefully examined and found to be very sensitive to the saturating beam intensity and magnetic field, which was due to the population redistribution of the ground hyperfiue level. When the polarizations of the saturating and probing beams were linear and their directions were parallel, even the chage of sign was observed. The magnitude and linewidth of the signal were controlled by adjusting the saturating beam intensity and the magnetic field as well as the laser polarization.
The saturated absorption spectrum of Cs D 2 line has been measured by using a diode laser.The anomalies of the line intensities in the closed transitions are detected at several polarization configuration of the pump and probe beams.Weak magnetic fields of parallel and perpendicular to the laser beam are applied to identify the population trapping effect in the closed transition of F ′′ = 3 → F ′ = 2 and F ′′ = 4 → F ′ = 5.In case of the F ′′ = 3 → F ′ = 2 transition, the line intensity is controlled by polarization configuration and external magnetic field.