On the prospects of optical cycling in diatomic cations: Effects of transition metals, spin-orbit couplings, and multiple bonds

20 June 2022, Version 2
This content is a preprint and has not undergone peer review at the time of posting.

Abstract

Molecules with optical cycling centers (OCCs) are highly desirable in the context of fundamental studies as well as applications (e.g., quantum computing) because they can be effectively cooled to very low temperatures by repeated absorption and emission (hence, cycling). Charged species offer additional advantages for experimental control and manipulation. We present a systematic computational study of a series of diatomic radical-cations made of a d-block metal and a p-block ligand, that are isoelectronic (in their valence shell) to the successfully laser-cooled neutral molecules. Using high-level electronic structure methods, we characterize state and transition properties of low-lying electronic states and compute Franck-Condon factors. The computed branching ratios and radiative lifetimes reveal that the electronic transitions analogous to those successfully used in the laser cooling of neutral molecules are less than optimal in the cations. We propose alternative transitions suitable for optical cycling and highlight trends that could assist future designs of OCCs in charged or neutral molecules.

Keywords

optical cycling
d-block metals
laser cooling
diatomic cations
spin-orbit couplings
multiple bonds

Supplementary materials

Title
Description
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Title
SI
Description
Supplementary Materials
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Title
Potential energy curves
Description
Potential energy curves
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Title
SOC-corrected PESs
Description
Spin-orbit corrected potential energy surfaces
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