Cooperative photoproduction of Xe2+Cl− in liquid Cl2/Xe solutions: Stimulated emission and gain measurements

Wiedeman, L.; Fajardo, Mario E.; Apkarian, V. A.

doi:10.1016/0009-2614(87)80013-1

Cited by 16 publications

(5 citation statements)

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“…(2) can be classified under the general class of cooperative two-photon absorptions, the quantum electrodynamical formulation of which has been presented in a series of papers by Andrews et al 11 The predictable efficiency of these processes in condensed media was first demonstrated in C12, HCI and C1 doped xenon matrices, 1z '13 and subsequently in liquid C12/Xe solutions. 14 '15 The viability of this approach for the design of two-photon pumped, tunable condensed phase exciplex lasers was demonstrated by gain measurements in solid 13 and liquid 14 phase xenon chlorides, and the generalization of the principles to the entire family of xenon halides was reported. 16 The liquid phase spectra of rare gas fluorides had previously been reported, 17 and laser action of liquid phase exciplexes by both optical, TM and electron beam 19 pumping have been demonstrated.…”

Section: Introductionmentioning

confidence: 99%

Condensed Phase Laser InducedHarpoon Reactions

et al. 1988

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Laser induced charge transfer reactions of halogens in rare gas solids and liquids provide a powerful means for the study of condensed phase dynamics. Many-body effects with respect to both electronic and nuclear coordinates, and cooperative interactions with radiation fields, are some of the studied phenomena that are highlighted in this article.The pertinence of these ionic reactions to chemistry in solids is demonstrated in photodissociation studies of molecular halogens in rare gas matrices. The coexistence of both delocalized and localized charge transfer states in solid xenon doped with atomic halogens is presented and dynamical consequences—charge separation, self-trapping and energy storage—are discussed. Static and dynamic solvent effects in liquid phase harpoon reactions are considered. The characterization of cooperative excitations— two-photon, two-electron transitions—in liquid solutions is presented.

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Section: Introductionmentioning

confidence: 99%

Condensed Phase Laser InducedHarpoon Reactions

et al. 1988

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“…Recalcualted using HD's AE. J References 49 and 50 4. Recalculated using experimental AE by the current authors.…”

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confidence: 99%

Quantum Chemical Study of the Potential Energy Curves and Electronic Transition Strengths in HCl, XeCl, and HCl + Xe

Adams¹,

Chabalowski²

1994

J. Phys. Chem.

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Potential energy curves and electronic transition strengths are calculated for selected singlet states in HCl, XeC1, and HCl + Xe using effective core potentials (ECPs) with state-averaged CASSCF-CI techniques. In HCl, the maximum photoabsorption cross section for the A('II) -%(lZ+) transition is calculated to be udt = 3.86 X 10-l8 cm2 for the v" = 0 band, in good agrtement with the experimental value of udf = 3.8 X 10-18 cm2. The oscillator strength for the 0-0 transition in C(lII) -%(lZ+) is calculated to befm = 0.175, differing by 5% from the experimental value offm = 0.185 f 0.037. The calculated oscillator strength for excitation into u' = 1 is significantly larger than the experimental values or those from previous theoretical treatments. In the XeCl, radiative lifetimes, 7, are predicted for selected doublet excited electronic states. This study substantiates earlier theoretical predictions and compares favorably with available experimental lifetimes. In the HCl + Xe system, low-lying singlet states are calculated as a function of the HC1-Xe distance with the H-C1 distance held fixed and the atoms kept collinear. A charge-transfer state is located which represents the excitation of a ?r electron into a u* antibonding orbital. This state offers a simplified model of the photoinitiated charge transfer observed in solid xenon doped with HC1, where the HCl is reported to dissociated after transfer of an electron from Xe to HCl. Other electronic states and electronic transition moments of the HC1 + Xe system are analyzed and related to the isolated HC1 electronic states and transitions when possible.by the xenon. For R < 8.0, the xenon atom begins to have a significant effect on the properties, which is reasonable since the sum of van der Waals radii53 for C1 (1.8 A) and Xe (2.2 A) is 7.6 bohrs (4.0 A). The transition moment shown in Figure 9 appears to be strongly affected by the close proximity of the two species. The calculated properties for this state leads one to Potential Energy Curves for HCl, XeCl, and HCl + Xe

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“…This discovery clearly delineates the underlying mechanism for the process as one in which the synergistic excitation of the two absorbing species results from molecular proximity rather than any collisional effect. The reaction mechanism (1.1) has been further corroborated by Apkarian and co-workers, who have also extended the study to charge transfer reactions in solid and liquid xenon (Fajardo and Apkarian 1986Wiedeman et al 1987Wiedeman et al , 1988. It has additionally been shown to be the predominant reaction route in the case of Xe:Cl, van der Waals complexes generated in seeded molecular beams (Boivineau et al 1986a, b).…”

Section: Introductionmentioning

confidence: 63%