Observation of resonant monopole-dipole energy transfer between Rydberg atoms and polar molecules

Abstract

Resonant energy transfer (RET), between equal parity 1s65s$^3\mathrm{S}_1$ and 1s66s$^3\mathrm{S}_1$ Rydberg levels in helium has been observed in low-temperature ($\sim80$ mK) collisions with ammonia molecules which undergo inversion transitions in their X$^1$A$_1$ ground electronic state. This hybrid Rydberg-atom-polar-molecule RET represents a monopole-dipole energy exchange reaction that necessarily requires spatial overlap of the Rydberg-electron and molecular wavefunctions. Calculations, that account explicitly for the charge-dipole interaction between the Rydberg electron and the molecule, provide a quantitative explanation of the observations. Total parity is conserved in the reaction through the mixing of collisional angular momentum in the atom-molecule complex. This work opens opportunities to expand the toolbox for quantum science with charge-dipole-mediated energy exchange in hybrid neutral-atom-polar-molecule platforms.