Formally exact fluorescence spectroscopy simulations for mesoscale molecular aggregates with N0 scaling

Publikation: Beitrag in FachzeitschriftForschungsartikelBeigetragenBegutachtung

Beitragende

Abstract

We present a size-invariant (i.e., N0) scaling algorithm for simulating fluorescence spectroscopy in large molecular aggregates. We combine
the dyadic adaptive hierarchy of pure states (DadHOPS) equation-of-motion with an operator decomposition scheme and an efficient Monte
Carlo sampling algorithm to enable a formally exact, local description of the fluorescence spectrum in large molecular aggregates. Furthermore,
we demonstrate that the ensemble average inverse participation ratio of DadHOPS wave functions reproduces the delocalization extent
extracted from fluorescence spectroscopy of J-aggregates with strong vibronic transitions. This work provides a computationally efficient
framework for fluorescence simulations, offering a new tool for understanding the optical properties of mesoscale molecular systems.

Details

OriginalspracheEnglisch
Aufsatznummer234111
Seitenumfang17
FachzeitschriftThe Journal of chemical physics
Jahrgang162
Ausgabenummer23
PublikationsstatusVeröffentlicht - 20 Juni 2025
Peer-Review-StatusJa

Externe IDs

Scopus 105008674074

Schlagworte

Schlagwörter

  • fluorescence spectroscopy, Stochastic differential equation, Hierarchy of pure states