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Article Dans Une Revue Journal of Chemical Physics Année : 2022

Reassessing the potential of TlCl for laser cooling experiments via four-component correlated electronic structure calculations

Résumé

The TlCl molecule has previously been investigated theoretically and proposed as promising candidates for laser cooling searches [X. Yuan et. al. J. Chem. Phys., 149, 094306, 2018]. From these results, the cooling process, which would proceed by transitions between a3Π+0 and X1Σ+0 states, had as potential bottleneck the long lifetime (6.04 µs) of the excited state a3Π+0, that would prohibit experimentally control the slowing region. Here, we revisit this system by employing four-component Multireference Configuration Interaction (MRCI) calculations and investigate the effect of such approaches on the calculated transition moments between a3Π+0 and a3Π1 excited states of TlCl as well as TlF, the latter serving as a benchmark between theory and experiment. Wherever possible, MRCI results have been cross-validated by, and turned out to be consistent with, four-component equation of motion coupled-cluster (EOM-CC) and polarization propagator (PP) calculations. We find that the results of TlF are very closed to experiment values, while for TlCl the lifetime of the a3Π+0 state is now estimated to be 175 ns, which is much shorter than previous calculations indicated, thus yielding a different, more favorable cooling dynamics. By solving the rate-equation numerically, we provide evidence that TlCl could have cooling properties similar to those of TlF. Our investigations also point to the potential benefits of enhancing the stimulated radiation in optical cycle to improve cooling efficiency.
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Dates et versions

hal-03618206 , version 1 (24-03-2022)
hal-03618206 , version 2 (29-07-2022)

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Xiang Yuan, André Severo Pereira Gomes. Reassessing the potential of TlCl for laser cooling experiments via four-component correlated electronic structure calculations. Journal of Chemical Physics, 2022, 157, pp.074313. ⟨10.1063/5.0092620⟩. ⟨hal-03618206v2⟩
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