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Stochastically Realized Observables for Excitonic Molecular Aggregates.

  • Author(s): Bradbury, Nadine C
  • Chuang, Chern
  • Deshmukh, Arundhati P
  • Rabani, Eran
  • Baer, Roi
  • Caram, Justin R
  • Neuhauser, Daniel
  • et al.
Abstract

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.

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