| Autor: |
Bradbury, Nadine C., Chuang, Chern, Deshmukh, Arundhati P., Rabani, Eran, Baer, Roi, Caram, Justin R., Neuhauser, Daniel |
| Zdroj: |
The Journal of Physical Chemistry - Part A; December 2020, Vol. 124 Issue: 49 p10111-10120, 10p |
| Abstrakt: |
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 Ndye 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. |
| Databáze: |
Supplemental Index |
| Externí odkaz: |
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