Vibrationally-induced electronic population inversion with strong femtosecond pulses

TL;DR

This paper introduces a novel method for electronic population inversion using strong femtosecond pulses mediated by vibrational motion, with potential applications demonstrated in Na2 molecules.

Contribution

The study reveals a new vibrationally-induced inversion mechanism and extends it to multiphoton processes, highlighting the importance of transition dipole moment slope.

Findings

Population inversion achieved with single femtosecond pulse.

Sign of transition dipole slope influences dynamics.

Method applicable to multiphoton processes in molecules.

Abstract

We discover a new mechanism of electronic population inversion using strong femtosecond pulses, where the transfer is mediated by vibrational motion on a light-induced potential. The process can be achieved with a single pulse tuning its frequency to the red of the Franck-Condon window. We show the determinant role that the sign of the slope of the transition dipole moment can play on the dynamics, and extend the method to multiphoton processes with odd number of pulses. As an example, we show how the scheme can be applied to population inversion in Na2.