Modular path integral for finite-temperature dynamics of extended systems with intramolecular vibrations

Sohang Kundu, Nancy Makri

Research output: Contribution to journalArticlepeer-review

Abstract

The modular decomposition of the path integral is a linear-scaling, numerically exact algorithm for calculating dynamical properties of extended systems composed of multilevel units with local couplings. In a recent article, we generalized the method to wavefunction propagation in aggregates characterized by non-diagonal couplings between adjacent units. Here, we extend the method to the calculation of reduced density matrices in aggregates where each unit includes an arbitrary number of coupled harmonic bath modes, which may describe intramolecular normal mode vibrations, at finite temperature. The effects of harmonic modes are included through influence functional factors, which involve analytical expressions that we derive. Representative applications to spin arrays described by the Heisenberg Hamiltonian with dissipative interactions and to J-aggregates of perylene bisimide, where all coupled normal modes are treated explicitly, are presented.

Original languageEnglish (US)
Article number044124
JournalJournal of Chemical Physics
Volume153
Issue number4
DOIs
StatePublished - Jul 28 2020

ASJC Scopus subject areas

  • Physics and Astronomy(all)
  • Physical and Theoretical Chemistry

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