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A study of the intensity-borrowing mechanisms important to optical cyclingtransitions in laser-coolable polyatomic molecules arising from non-adiabaticcoupling, contributions beyond the Franck-Condon approximation, and Fermiresonances is reported. It has been shown to be necessary to includenon-adiabatic coupling to obtain computational accuracy that is sufficient tobe useful for laser cooling of molecules. The predicted vibronic branchingratios using perturbation theory based on the non-adiabatic mechanisms havebeen demonstrated to agree well with those obtained from variational discretevariable representation calculations for representative molecules includingCaOH, SrOH, and YbOH. The electron-correlation and basis-set effects on thecalculated transition properties, including the vibronic coupling constants,the spin-orbit coupling matrix elements, and the transition dipole moments, andon the calculated branching ratios have been thoroughly studied. The vibronicbranching ratios predicted using the present methodologies demonstrate thatRaOH is a promising radioactive molecule candidate for laser cooling.

Intensity-borrowing mechanisms pertinent to laser cooling of linear polyatomic molecules