The complementary techniques of high-resolution vacuum ultraviolet absorption spectroscopy and resonance-enhanced multiphoton ionisation spectroscopy have been employed in a reinvestigation of the vertical electronic spectra of the molecules H2S and D2S. In accord with previous, lower-resolution, absorption studies of H2S the major part of the spectra of both isotopic species may be understood in terms of Rydberg series that arise from promotion of an electron from the highest occupied 2bl molecular orbital. The electronic symmetries of states involved in six Rydberg series have been established unambiguously through observation of the (partially resolved) rotational structure that accompanies their excitations. A number of additional resonances observed only in the multiphoton ionisation spectra are tentatively attributed to excitations involving Rydberg orbitals comprised predominantly o f f and/or g functions. Several of the absorption features (most notably those involving excited sites of B, symmetry) exhibit anomalous intensity distributions between the various rotational branches. L-uncoupling and/or rovibronic level dependent predissociation are suggested as contributory causes.
The influence of collisions on magneto-optical rotation spectra is considered By using a Rydberg state and nearby doublyexcited perturbers of the barium spectrum as probes, it is shown that, for a given spectral resolution, the broadening of the lines as a function of pressurecan be determined in a sensitive way at lower pressures of the perturbing gases than in conventional photoabsorption experiments. The relativefivalues of the lines (which do not change significantly in the pressure range investigated) are also accurately monitored by the same method. For the SdSp doubly excited states in Ba and the Rydberg member which lies between them, thefivalues are found to be constant to an accuracy of 5% as the pressure of rare gas is increased in the range up to 100 mb. We have also observed an intruder which can only be excited in the presence of the magnetic field.
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