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• W2054584192 abstract "Two new Rydberg series in H2S and D2S habe been characterized as three-photon resonances in four-photon ionisation spectrometry. Members of the two series exhibit sufficient rotational structure to permit characterisation of their electronic symmetries as, respectively. A2 and B1. The first Rydberg series is identified with the (one-photon forbidden) excitations npb2 ← 2b1 (1A2 ← X1A1) on the basis of the observed quantum defects. Geometry considerations indicate that second series, of 1B1 states, also arises as a result of electronic promotion from the highest occupied 2b1 orbital. The acceptor (a1) Rydberg orbitals possess substanial s character, but the polarisation dependence of the various 1B1-X1A1 three-photon transition probabilities their hybrid I character, d (and quite possibly p) functions contribute also. The results provide further clear demonstration of the way in which multiphoton excitations, and MPI techniques in particular, can complement conventional one-photon absorption techniques. Members of both series are predissociated. Vibronic predissociation rates are found generally to decline with increasing n and to be slower in D2S than in H2S. The lowest (n = 4) member of the 1A2 series in both isotopic species appears immune from rovibronic predissociation but higher members show evidence of a (Ja2)-dependent rotationally-induced predissociation, the severity of which increases dramatically with n. This observation is explained in terms of electronic-rotational Coriolis coupling to a dissociated 1B2 state is presumed to be responsible for the observed (Jb2)-dependent heterogeneous predissociation of the 1B1 (n = 6) member in H2S. However, the dominant rotationally-induced predissociation mechanism that affects the counterpart in D2S scales with (Ja2). Wherever possible comparisons are drawn with the known spectroscopy and photophysics of the isovalent molecules H2O and D2O." @default.
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• W2054584192 date "1985-09-01" @default.
• W2054584192 modified "2023-09-23" @default.
• W2054584192 title "Molecular predissociation dynamics revealed through multiphoton ionisation spectroscopy. III. New 1A2 and 1B1 rydberg states in H2S D2S" @default.
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• W2054584192 doi "https://doi.org/10.1016/0301-0104(85)80142-7" @default.
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