Unified parameter for localization in isotope-selective rotational excitation of diatomic molecules using a train of optical pulses

TL;DR

This paper introduces a simple, unified parameter combining pulse intensity, interval, and molecular energy levels to predict rotational population localization in diatomic molecules subjected to resonant optical pulse trains.

Contribution

It presents a novel unified parameter for characterizing rotational population propagation, including centrifugal distortion effects, validated through analytical derivation and numerical simulations.

Findings

Unified parameter accurately predicts probability localization boundaries.

Parameter accounts for centrifugal distortion effects.

Validation confirms the parameter's effectiveness in isotope-selective excitation.

Abstract

We obtained a simple theoretical unified parameter for the characterization of rotational population propagation of diatomic molecules in a periodic train of resonant optical pulses. The parameter comprises the peak intensity and interval between the pulses, and the level energies of the initial and final rotational states of the molecule. Using the unified parameter, we can predict the upper and lower boundaries of probability localization on the rotational level network, including the effect of centrifugal distortion. The unified parameter was tentatively derived from an analytical expression obtained by performing rotating-wave approximation and spectral decomposition of the time-dependent Schr\"{o}dinger equation under an assumption of time-order invariance. The validity of the parameter was confirmed by comparison with numerical simulations for isotope-selective rotational excitation of KCl molecules.