A fast method for electronic couplings in embedded multichromophoric systems. (27th July 2022)

• Record Type: Journal Article
• Authors: Cignoni, Edoardo; Cupellini, Lorenzo; Mennucci, Benedetta
• Is Part Of: Journal of physics. Volume 34:Number 30(2022)
• Publication Date: 2022-07-27
• Subjects: polarizable MM embedding -- light harvesting -- electronic couplings -- excitons -- excitation energy transfer; Condensed matter -- Periodicals; Matière condensée -- Périodiques; Vaste stoffen; Vloeistoffen; Natuurkunde; Electronic journals; Computer network resources; 530.4105
• DOI: 10.1088/1361-648X/ac6f3c
• Languages: English
• ISSNs: 0953-8984

Abstract

Abstract: Electronic couplings are key to understanding exciton delocalization and transport in natural and artificial light harvesting processes. We develop a method to compute couplings in multichromophoric aggregates embedded in complex environments without running expensive quantum chemical calculations. We use a transition charge approximation to represent the quantum mechanical transition densities of the chromophores and an atomistic and polarizable classical model to describe the environment atoms. We extend our framework to estimate transition charges directly from the chromophore geometry, i.e., bypassing completely the quantum mechanical calculations using a regression approach. The method allows to rapidly compute accurate couplings for a large number of geometries along molecular dynamics trajectories.