Probing resonant energy transfer in collisions of ammonia with Rydberg helium atoms by microwave spectroscopy

Abstract

We present the results of experiments demonstrating the spectroscopic detection of F\"{o}rster resonance energy transfer from NH$_3$ in the $X\,^1A_1$ ground electronic state to helium atoms in 1s$n$s\,$^3$S$_1$ Rydberg levels, where $n=37$ and $n=40$. For these values of $n$ the 1s$n$s\,$^3$S$_1\rightarrow$1s$n$p\,$^3$P$_J$ transitions in helium lie close to resonance with the ground-state inversion transitions in NH$_3$, and can be tuned through resonance using electric fields of less than 10~V/cm. In the experiments, energy transfer was detected by direct state-selective electric field ionization of the $^3$S$_1$ and $^3$P$_J$ Rydberg levels, and by monitoring the population of the $^3$D$_J$ levels following pulsed microwave transfer from the $^3$P$_J$ levels. Detection by microwave spectroscopic methods represents a highly state selective, low-background approach to probing the collisional energy transfer process and the environment in which the atom-molecule interactions occur. The experimentally observed electric-field dependence of the resonant energy transfer process, probed both by direct electric field ionization and by microwave transfer, agrees well with the results of calculations preformed using a simple theoretical model of the energy transfer process. For measurements performed in zero electric field with atoms prepared in the 1s40s\,$^3$S$_1$ level the transition from a regime in which a single energy transfer channel can be isolated for detection to one in which multiple collision channels begin to play a role has been identified as the NH$_3$ density was increased.Comment: 10 pages, 8 figure