Simulating mesoscale quantum dynamics with an adaptive hierarchy of pure states
Year: 2020
Type: preprint
Abstract: The rational design of molecular materials to control photophysical processes requires engineering excited-state carrier dynamics across the 10 nm to 1 $\mu$m length scale. While diffusion occurs over long length scales, the excitons only delocalize on short lengthscales due to the coupling between electronic and vibrational degrees-of-freedom. Here, we demonstrate that the locality of the excitons enables an adaptive Hierarchy of Pure States (adHOPS) method that is formally exact, embarrassingly parallel, and has size-invariant scaling. The size-invariant scaling of adHOPS allows for non-perturbative simulations of molecular aggregates with an arbitrary number of pigments in physically relevant parameter regimes. We provide proof-of-concept calculations on aggregates containing up to 1000 molecules and we expect that adHOPS will enable non-perturbative simulations of mesoscale quantum dynamics in molecular materials.
Source: arXiv (Cornell University)
Language: English
Subfield: Atomic and Molecular Physics, and Optics
Field: Physics and Astronomy
Domain: Physical Sciences
Open Access status: green
OpenAlex ID: W3049304373