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Spectroscopic Properties and Spin-Orbit Coupling of Electronic Excited States of GeCl.

The electronic structure and spectroscopic properties of GeCl+ are studied by high-level ab initio calculations by considering spin-orbit coupling (SOC). The potential energy curves (PECs) and spectroscopic constants of 12 Λ-S states and 23 Ω states are calculated using the multi-reference configuration interaction plus Davidson correction method (MRCI + Q), which are in good agreement with the experiment. Based on the calculated SO matrix and the PECs of the Ω states, the interaction between the d3Π state and other states caused by the SOC and the double-potential well structure caused by the avoided crossing rule and the properties of transitions d3Π0+-X1Σ+0+, d3Π1-X1Σ+0+, and a3Σ+1-X1Σ+0+ are studied. Our results indicate that the previously observed spectra of GeCl+ in the 290-325 nm range should be assigned as the a3Σ+1-X1Σ+0+ transition. Moreover, the predissociation behavior of the d3Π state between the vibrational levels v' = 1 and v' = 10 is discussed, and the radiative lifetimes of transitions d3Π0+-X1Σ+0+ and d3Π1-X1Σ+0+ are evaluated on the order of microseconds, while a3Σ+1-X1Σ+0+ is on the order of milliseconds. We estimate that the strongest bands of a3Σ+1-X1Σ+0+ are the 0-16, 0-17, and 0-18 bands. This study will promote our understanding of the detailed electronic structure and spectra of the GeCl+ radical cation.