Theory of electronic-state coherences produced in combined laser-field—collisional reactions

Abstract

A method for producing electronic-state coherences using either collisionally-aided radiative excitation (or "optical collision") or laser-induced collisional energy transfer (or "radiative collision") is proposed. Two atoms, $A$ and ${A}^{\ensuremath{'}}$, collide in the presence of two pulsed-laser fields having frequencies $\ensuremath{\Omega}$ and ${\ensuremath{\Omega}}_{1}$. It is shown that by choosing ${\ensuremath{\Omega}}_{1}\ifmmode\pm\else\textpm\fi{}\ensuremath{\Omega}$ such that an energy-conserving transition can occur in the composite $A{A}^{\ensuremath{'}}$ system, one can create an electronic-state coherence in the $A$ or ${A}^{\ensuremath{'}}$ atoms. The coherence can be produced between states of the same or of opposite parity; if it is between states of opposite parity, coherent emission at frequency ${\ensuremath{\Omega}}_{1}\ifmmode\pm\else\textpm\fi{}\ensuremath{\Omega}$ may be generated. The relationship of this work to theories of "pressure-induced extra resonances" in four-wave mixing is discussed.