2007/10/12 by S. M. Vlaming, V. A. Malyshev, J. Knoester
Physics and Astronomy · #Semiconductor Quantum Structures and Devices #Spectroscopy and Quantum Chemical Studies #Strong Light-Matter Interactions #cond-mat.dis-nn #cond-mat.mtrl-sci
paper · pdf · doi:10.1063/1.2784556
published as J. Chem. Phys. 127, 154719 (2007) · 9 pages, 6 figures, to appear in Journal of Chemical Physics
arxiv created 2007/10/12 · openalex publication_date 2007/10/18 · arxiv updated 2009/12/01 · openalex created_date 2016/06/24 · openalex updated_date 2026/08/01
We theoretically study the efficiency of energy harvesting in linear exciton chains with an energy bias, where the initial excitation is taking place at the high-energy end of the chain and the energy is harvested (trapped) at the other end. The efficiency is characterized by means of the average time for the exciton to be trapped after the initial excitation. The exciton transport is treated as the intraband energy relaxation over the states obtained by numerically diagonalizing the Frenkel Hamiltonian that corresponds to the biased chain. The relevant intraband scattering rates are obtained from a linear exciton-phonon interaction. Numerical solution of the Pauli master equation that describes the relaxation and trapping processes reveals a complicated interplay of factors that determine the overall harvesting efficiency. Specifically, if the trapping step is slower than or comparable to the intraband relaxation, this efficiency shows a nonmonotonic dependence on the bias: it first increases when introducing a bias, reaches a maximum at an optimal bias value, and then decreases again because of dynamic (Bloch) localization of the exciton states. Effects of on-site (diagonal) disorder, leading to Anderson localization, are addressed as well.