We recently showed how optical absorption, density of states, and participation ratios are calculable for giant molecular aggregates of dye monomers (millions of dyes) with a stochastic approach. (Bradbury et al., J. Phys. Chem. A,  2020, 124, 49, 10111–10120).  Leveraging the stochastic resolution of the identity, the method scales very smoothly with the size of the system, O(N log(N)), and does away with costly repetitive numerical diagonalizations of the Hamiltonian. Given the very few requirements on the dye Hamiltonian, this stochastic framework leads to orders-of-magnitude increase in capabilities of screening for modeling parameters and for inclusion of traditionally expensive effects such as vibrational states. <br/><br/>The left of the figure shows the real computer time for a density of states and absorption calculation on a 2D planar aggregate, the right shows example spectra for varying levels of diagonal normally-distributed disorder.

Stochastically realized observables for excitonic molecular aggregates

ACS Spring Meeting 2021

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