Ab initio molecular dynamics modelling of organic crystal electro-optical properties

TL;DR

This paper uses ab initio molecular dynamics to model the vibrational and optical properties of organic crystals DAST and DSTMS, linking their phononic behavior to terahertz generation capabilities and validating with experimental data.

Contribution

It introduces a computational approach combining molecular dynamics and Green-Kubo relations to predict optical properties of organic crystals.

Findings

Vibrational modes identified and linked to terahertz generation

Calculated optical properties agree with experimental transmission data

Insights into phononic contributions to electro-optical behavior

Abstract

Molecular dynamics calculations were preformed on organic crystals 4-N,N-dimethylamino-4'-N'-methyl-stilbazolium tosylate (DAST) and 4-N,N-dimethylamino-4'-N'-methylstilbazolium 2,4,6-trimethylbenzenesulfonate (DSTMS). Vibrational modes of the structures were investigated to examine the single unit cell phononic contribution of the organic crystals to their terahertz generating capabilities. Linear optical properties were also calculated from snapshots of the molecular dynamics structures through Green-Kubo relations, and compared with experimental transmission.