Optical excitation and stabilization of ultracold field-linked tetratomic molecules

Abstract

We propose a coherent optical population transfer of weakly bound field-linked (FL) tetratomic molecules (tetramers) to deeper FL bound states using stimulated Raman adiabatic passage. We consider static-electric-field shielded polar alkali-metal diatomic molecules and corresponding FL tetramers in their $\textrm{X}^1\Sigma^+$+$\textrm{X}^1\Sigma^+$ ground electronic state. We show that the excited metastable $\textrm{X}^1\Sigma^+$+$\textrm{b}^3\Pi$ electronic manifold supports FL tetramers in a broader range of electric fields with collisional shielding extended to zero field. We calculate the Franck-Condon factors between the ground and excited FL tetramers and show that they are highly tunable with the electric field. We also predict photoassociation of ground-state shielded molecules to the excited FL states in free-bound optical transitions. We propose proof-of-principle experiments to implement stimulated Raman adiabatic passage and photoassociation using FL tetramers, paving the way for the formation of deeply bound ultracold polyatomic molecules.