Formally Exact Simulations of Mesoscale Exciton Diffusion in a Light-Harvesting 2 Antenna Nanoarray.

Autor:	Varvelo L; Department of Chemistry, Southern Methodist University, P.O. Box 750314, Dallas, Texas 75275, United States., Lynd JK; Department of Chemistry, Southern Methodist University, P.O. Box 750314, Dallas, Texas 75275, United States., Citty B; Department of Chemistry, Southern Methodist University, P.O. Box 750314, Dallas, Texas 75275, United States., Kühn O; Institute of Physics, University of Rostock, Albert-Einstein-Strasse 23-24, 18059 Rostock, Germany., Raccah DIGB; Department of Chemistry, Southern Methodist University, P.O. Box 750314, Dallas, Texas 75275, United States.
Jazyk:	angličtina
Zdroj:	The journal of physical chemistry letters [J Phys Chem Lett] 2023 Mar 30; Vol. 14 (12), pp. 3077-3083. Date of Electronic Publication: 2023 Mar 22.
DOI:	10.1021/acs.jpclett.3c00086
Abstrakt:	The photosynthetic apparatus of plants and bacteria combine atomically precise pigment-protein complexes with dynamic membrane architectures to control energy transfer on the 10-100 nm length scales. Recently, synthetic materials have integrated photosynthetic antenna proteins to enhance exciton transport, though the influence of artificial packing on the excited-state dynamics in these biohybrid materials is not fully understood. Here, we use the adaptive hierarchy of pure states (adHOPS) to perform a formally exact simulation of excitation energy transfer within artificial aggregates of light-harvesting complex 2 (LH2) with a range of packing densities. We find that LH2 aggregates support a remarkable exciton diffusion length ranging from 100 nm at a biological packing density to 300 nm at the densest packing previously suggested in an artificial aggregate. The unprecedented scale of these formally exact calculations also underscores the efficiency with which adHOPS simulates excited-state processes in molecular materials.
Databáze:	MEDLINE
Externí odkaz:	Zobrazit plný text záznamu