Hierarchical equations of motion model for phonon and photon correlations
POSTER
Abstract
The hierarchical equations of motion (HEOM), constructed through Feynman and Vernon path integrals, are used to model the dynamics of quantum systems within a statistical ensemble representing the condensed phase. We show that second-order, two-time correlation functions for phonons and photons emitted from a vibronic molecule in a thermal bath produce signatures relating to exchange with the environment and discuss how these arise from the hierarchical equations of motion. Additionally, we discuss the physical justification for the fundamental steps involved in deriving the HEOM and highlight the profound impact on the system memory effects that changes in the spectral density, or bilinear system-environment coupling, can have.
*Research carried out on the High-Performance Computing Cluster supported by the Research and Specialist Computing Support service at the University of East Anglia. B.S.H. thanks the UEA Faculty of Science for studentship funding.
Publication:B. S. Humphries, D. Green, M. O. Borgh, G. A. Jones, arXiv:2302.01105 (2023) B. S. Humphries, D. Green, and G. A. Jones, The influence of a hamiltonian vibration vs a bath vibration on the 2D electronic spectra of a homodimer, The Journal of Chemical Physics 156, 084103 (2022), https://doi.org/10.1063/5.0077404 D. Green, B. S. Humphries, A. G. Dijkstra, and G. A. Jones, Quantifying non-markovianity in underdamped versus overdamped environments and its effect on spectral lineshape, The Journal of Chemical Physics 151, 174112 (2019), https://doi.org/10.1063/1.5119300.