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By means of highly accurate  ab initio  calculations, we identify two excellent ultracold molecular candidates from group VA hydrides. We find that NH and PH are suitable for the production of ultracold molecules, and the feasibility and advantage of two laser cooling schemes are demonstrated, which involve different spin-orbit states (A  3    Π  2andX  3    Σ  1  −). The internally contracted multireference configuration interaction method is applied in calculations of the six low-lying Λ-S states of NH and PH with the spin-orbit coupling effects included, and excellent agreement is achieved between the computed and experimental spectroscopic data. We find that the locations of crossing point between theA  3   ΠandΣ  −5states of NH and PH are higher than the corresponding  v ′ = 2 vibrational levels of theA  3   Πstate indicating that the crossings with higher electronic states would not affect laser cooling. Meanwhile, the extremely small vibrational branching loss ratios of theA  3    Π  2→a  1    Δ  2transition for NH and PH (NH: 1.81 × 10 –8 ; PH: 1.08 × 10 –6 ) indicate that thea  1    Δ  2intermediate electronic state will not interfere with the laser cooling. Consequently, we construct feasible laser-cooling schemes for NH and PH using three lasers based on theA  3    Π  2→X  3    Σ  1  −transition, which feature highly diagonal vibrational branching ratioR   00(NH: 0.9952; PH: 0.9977), the large number of scattered photons (NH: 1.04×10 5 ; PH: 8.32×10 6 ) and very short radiative lifetimes (NH: 474 ns; PH: 526 ns). Our work suggests that feasible laser-cooling schemes could be established for a molecular system with extra electronic states close to those chosen for laser-cooling.

Excellent Ultracold Molecular Candidates From Group VA Hydrides: Whether Do Nearby Electronic States Interfere?