Simulating optical linear absorption for mesoscale molecular aggregates: an adaptive hierarchy of pure states approach

Abstract

In this paper, we present a new method for calculating linear absorption spectra for large molecular aggregates, called dyadic adaptive HOPS (DadHOPS). This method combines the adaptive HOPS (adHOPS) framework, which uses locality to improve computational scaling, with the dyadic HOPS method previously developed to calculate linear and non-linear spectroscopic signals. To construct a local representation of dyadic HOPS, we introduce an initial state decomposition which reconstructs the linear absorption spectra from a sum over locally excited initial conditions. We demonstrate the sum over initial conditions can be efficiently Monte Carlo sampled, that the corresponding calculations achieve size-invariant (i.e. $\mathcal{O}(1)$) scaling for sufficiently large aggregates, and that it allows for the trivial inclusion of static disorder in the Hamiltonian. We present calculations on the photosystem I core complex to explore the behavior of the initial state decomposition in complex molecular aggregates, and proof-of-concept DadHOPS calculations on an artificial molecular aggregate inspired by perylene bis-imide.

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Cited by in corpus (8)

• Simulating optical linear absorption for mesoscale molecular aggregates: an adaptive hierarchy of pure states approach
• Dynamics of a strongly coupled quantum heat engine -- computing bath observables from the hierarchy of pure states
• Simulating Non-Markovian Dynamics in Multidimensional Electronic Spectroscopy via Quantum Algorithm
• Spectral signatures of the Markovian to Non-Markovian transition in open quantum systems
• Spectral Densities, Structured Noise and Ensemble Averaging within Open Quantum Dynamics
• nuHOPS: A quantum trajectory method for highly excited environments in non-Markovian open quantum dynamics
• Extracting Coupling-Mode Spectral Densities with Two-Dimensional Electronic Spectroscopy
• Non-Markovian dynamics in nonstationary Gaussian baths: a hierarchy of pure states approach