Stochastically Realized Observables for Excitonic Molecular Aggregates

Nadine C. Bradbury*, Chern Chuang, Arundhati P. Deshmukh, Eran Rabani, Roi Baer, Justin R. Caram*, Daniel Neuhauser

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

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We show that a stochastic approach enables calculations of the optical properties of large 2-dimensional and nanotubular excitonic molecular aggregates. Previous studies of such systems relied on numerically diagonalizing the dense and disordered Frenkel Hamiltonian, which scales approximately as O(N3) for N dye molecules. Our approach scales much more efficiently as O(Nlog(N)), enabling quick study of systems with a million of coupled molecules on the micrometer size scale. We calculate several important experimental observables, including the optical absorption spectrum and density of states, and develop a stochastic formalism for the participation ratio. Quantitative agreement with traditional matrix diagonalization methods is demonstrated for both small- and intermediate-size systems. The stochastic methodology enables the study of the effects of spatial-correlation in site energies on the optical signatures of large 2D aggregates. Our results demonstrate that stochastic methods present a path forward for screening structural parameters and validating experiments and theoretical predictions in large excitonic aggregates.

Original languageAmerican English
Pages (from-to)10111-10120
Number of pages10
JournalJournal of Physical Chemistry A
Issue number49
StatePublished - 10 Dec 2020

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