Computational approaches to efficient generation of the stationary state for incoherent light excitation

TL;DR

This paper introduces three computational methods to efficiently determine the stationary state of molecular systems under incoherent light excitation without requiring full Hamiltonian diagonalization, addressing a key challenge in light-harvesting simulations.

Contribution

The paper presents novel approaches that bypass the need for full Hamiltonian diagonalization to compute stationary states under incoherent light, improving computational efficiency.

Findings

Three efficient algorithms for stationary state calculation

Established link between incoherent perturbations and Kraus operators

Methods applicable to realistic molecular systems

Abstract

Light harvesting processes are often computationally studied from a time-dependent viewpoint, in line with ultrafast coherent spectroscopy experiments. Yet, natural processes take place in the presence of incoherent light, which induces a stationary state. Such stationary states can be described using the eigenbasis of the molecular Hamiltonian, but for realistic systems a full diagonalization is prohibitively expensive. We propose three efficient computational approaches to obtaining the stationary state that circumvent system Hamiltonian diagonalization. The connection between the incoherent perturbations, decoherence, and Kraus operators is established.