Orientation and Alignment dynamics of polar molecule driven by shaped laser pulses

Spectrochim Acta A Mol Biomol Spectrosc. 2021 Jul 15:256:119663. doi: 10.1016/j.saa.2021.119663. Epub 2021 Mar 11.

Abstract

We review the theoretical status of intense laser induced orientation and alignment-a field of study which lies at the interface of intense laser physics and chemical dynamics and having potential applications such as high harmonic generation, nano-scale processing and control of chemical reactions. The evolution of the rotational wave packet and its dynamics leading to orientation and alignment is the topic of the present discussion. The major part of this article primarily presents an overview of recent theoretical progress in controlling the orientation and alignment dynamics of a molecule by means of shaped laser pulses. The various theoretical approaches that lead to orientation and alignment such as static electrostatic field in combination with laser field(s), combination of orienting and aligning field, combination of aligning fields, combination of orienting fields, application of train of pulses etc. are discussed. It is observed that the train of pulses is quite an efficient tool for increasing the orientation or alignment of a molecule without causing the molecule to ionize. The orientation and alignment both can occur in adiabatic and non-adiabatic conditions with the rotational period of the molecule taken under consideration. The discussion is mostly limited to non-adiabatic rotational excitation (NAREX) i.e. cases in which the pulse duration is shorter than the rotational period of the molecule. We have emphasised on the so called half-cycle pulse (HCP) and square pulse (SQP). The effect of ramped pulses and of collision on the various laser parameters is also studied. We summarize the current discussion by presenting a consistent theoretical approach for describing the action of such pulses on movement of molecules. The impact of a particular pulse shape on the post-pulse dynamics is also calculated and analysed. In addition to this, the roles played by various laser parameters including the laser frequency, the pulse duration and the system temperature etc. are illustrated and discussed. The concept of alignment is extended from one-dimensional alignment to three-dimensional alignment with the proper choice of molecule and the polarised light. We conclude the article by discussing the potential applications of intense laser orientation and alignment.

Keywords: Alignment; Collision; HCP; NAREX; Orientation; Pulse shape; SQP.

Publication types

  • Review