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Physical Review A

HgIn photoassociation, bound-bound transitions, and excimer emission

Paola Bicchi, C. Marinelli, Robert A. Bernheim

Published Sep 1, 1997• 6 citations
Publisher

Abstract

Laser excitation of In atoms at the $6{}^{2}{S}_{1/2}--5{}^{2}{P}_{1/2}$ atomic resonance transition wavelength of 410.3 nm in the presence of Hg vapor produces several types of emission features: HgIn excimer satellites on the red wings of the In resonance fluorescence transitions at 410.3 and 451.1 nm, bound-bound HgIn molecular fluorescence at 499 and 522 nm resulting from photoassociation of $\mathrm{In}(6{}^{2}{S}_{1/2})$ with $\mathrm{Hg}(6{}^{1}{S}_{0}),$ and UV atomic fluorescence from the $\mathrm{In}(5{}^{2}D)$ states that lie at energies above the $\mathrm{In}(6{}^{2}{S}_{1/2}--5{}^{2}{P}_{1/2})$ excitation. These various spectral features are interpreted in terms of a proposed HgIn potential-energy level diagram with additional information from measured excited-state lifetimes and the power dependence of the laser excitation at 410.3 and 522 nm. Direct excitation of the 499 and 522 nm HgIn bound-bound transitions also produces emission at 410.3 and 451.1 nm resulting from collisional dissociation of the excited HgIn states.

DOI
10.1103/physreva.56.2025

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Laser excitation of In atoms at the 62S1/2−−52P1/26{}^{2}{S}_{1/2}--5{}^{2}{P}_{1/2}62S1/2​−−52P1/2​ atomic resonance transition wavelength of 410.3 nm in the presence of Hg vapor produces several types of emission features: HgIn excimer satellites on the red wings of the In resonance fluorescence transitions at 410.3 and 451.1 nm, bound-bound HgIn molecular fluorescence at 499 and 522 nm resulting from photoassociation of In(62S1/2)\mathrm{In}(6{}^{2}{S}_{1/2})In(62S1/2​) with Hg(61S0),\mathrm{Hg}(6{}^{1}{S}_{0}),Hg(61S0​), and UV atomic fluorescence from the In(52D)\mathrm{In}(5{}^{2}D)In(52D) states that lie at energies above the In(62S1/2−−52P1/2)\mathrm{In}(6{}^{2}{S}_{1/2}--5{}^{2}{P}_{1/2})In(62S1/2​−−52P1/2​) excitation. These various spectral features are interpreted in terms of a proposed HgIn potential-energy level diagram with additional information from measured excited-state lifetimes and the power dependence of the laser excitation at 410.3 and 522 nm. Direct excitation of the 499 and 522 nm HgIn bound-bound transitions also produces emission at 410.3 and 451.1 nm resulting from collisional dissociation of the excited HgIn states.
We report the first observation of laser-induced fluorescence of the CsHg molecule. Cs/Hg vapor mixtures contained in a heat-pipe oven were excited by several different argon ion laser lines. Following these excitations, we observed three distinct peaks at λ=492.8, λ=498.3, and λ=521.5 nm in addition to the well-known fluorescence of the Cs2 molecule. Based on an analysis using ab initio potential energy curves of Cs2 and CsHg, we identified the origin of these three distinct peaks as bound–free transitions of CsHg (λ=492.8: IV3/2→X1/2, λ=498.3: VII1/2→X1/2, and λ=521.5 nm: VI1/2→X1/2). Furthermore, we could show that two different production channels are responsible for the formation of the CsHg molecules in the excited states. The excitation of the Cs/Hg vapor mixtures with wavelengths λexc=476–514 nm of the argon ion laser results in the production of the CsHg molecules via a photoassociation process, whereas the CsHg molecules are produced in a three-body collision following an excitation with λexc=457 nm. These results are confirmed by subsequent quantum-mechanical simulations of the observed laser-induced fluorescence spectra of CsHg.
We have measured the alignment of the photofragments produced by photodissociation of Hg–Ar van der Waals molecules using light around 253.7 nm. The molecules are produced in the X0+ ground state in a supersonic expansion. Tunable laser light close to the Hg 6 1S0–6 3P1 transition is then used to excite the molecule to the B1± state, in which it dissociates. The alignment of the resulting Hg(3P1) asymptotic atoms is probed by tuning a delayed second laser to the 435.8 nm Hg 6 3P1–7 3S1 atomic transition and monitoring the subsequent fluorescence on the 7 3S1–6 3P2 transition around 546.1 nm. These measurements have been made, we believe for the first time, as a function of dissociating energy from very close to threshold to higher energies. The alignment shows a significant rise with increasing photon energy in line with a semiclassical picture of orbital locking at lower energies and rapid decoupling at higher energies. The results exhibit good agreement with the results of a fully quantum mechanical theory of the system.
A continuous excitation band of a free-bound photoassociation transition of ytterbium atoms is observed as a red wing of the $^{1}S_{0}\text{\ensuremath{-}}^{1}P_{1}$ atomic line at 399 nm for a hot thermal vapor. The excitation to the 0u+{0}_{u}^{+}0u+​ molecular state is observed by monitoring fluorescence from the 3P1^{3}P_{1}3P1​ state atoms, which allows us to detect the production of Yb2{\mathrm{Yb}}_{2}Yb2​ molecules with high sensitivity. The photoassociation is characterized in comparison with transitions to atomic Rydberg states. The time profile of the fluorescence signal suggests that the 0u+{0}_{u}^{+}0u+​ molecular state predissociates with states correlating to the 1S0+3D2^{1}S_{0}+^{3}D_{2}1S0​+3D2​ atomic states.