Laser cooling of BH and GaF: insights from an ab initio study.

The feasibility of laser cooling BH and GaF is investigated using ab initio quantum chemistry. The ground state X (1)Σ(+) and first two excited states (3)Π and (1)Π of BH and GaF are calculated using the multireference configuration interaction (MRCI) level of theory. For GaF, the spin-orbit coupling effect is also taken into account in the electronic structure calculations at the MRCI level. Calculated spectroscopic constants for BH and GaF show good agreement with available theoretical and experimental results. The highly diagonal Franck-Condon factors (BH: f00 = 0.9992, f11 = 0.9908, f22 = 0.9235; GaF: f00 = 0.997, f11 = 0.989, f22 = 0.958) for the (1)Π (v' = 0-2) → X (1)Σ(+) (v = 0-2) transitions in BH and GaF are determined, which are found to be in good agreement with the theoretical and experimental data. Radiative lifetime calculations of the (1)Π (v' = 0-2) state (BH: 131, 151, and 187 ns; GaF: 2.26, 2.36, and 2.48 ns) are found to be short enough for rapid laser cooling. The proposed laser cooling schemes that drive the (1)Π (v' = 0) → X (1)Σ(+) (v = 0) transition use just one laser wavelength λ00 (BH: 436 nm, GaF: 209 nm). Though the cooling wavelength of GaF is deep in the UVC, a frequency quadrupled Ti:sapphire laser (189-235 nm) could be capable of generating useful quantities of light at this wavelength. The present results indicate that BH and GaF are two good choices of molecules for laser cooling.