Structural Disorder at the Edges of Rubrene Crystals Enhances Singlet Fission.

Autor:	Volek TS; Department of Chemistry, The University of Texas at Austin, Austin, Texas 78712, United States.; Center for Adopting Flaws as Features, Urbana, Illinois 61801, United States., Armstrong ZT; Center for Adopting Flaws as Features, Urbana, Illinois 61801, United States.; Department of Chemistry, University of Wisconsin Madison, Madison, Wisconsin 53706, United States., Sowa JK; Center for Adopting Flaws as Features, Urbana, Illinois 61801, United States.; Department of Chemistry, Rice University, Houston, Texas 77005, United States., Wilson KS; Department of Chemistry, The University of Texas at Austin, Austin, Texas 78712, United States.; Center for Adopting Flaws as Features, Urbana, Illinois 61801, United States., Bohlmann Kunz M; Center for Adopting Flaws as Features, Urbana, Illinois 61801, United States.; Department of Chemistry, University of Wisconsin Madison, Madison, Wisconsin 53706, United States., Bera K; Department of Chemistry, University of Minnesota, Minneapolis, Minnesota 55455, United States., Koble M; Department of Chemistry, University of Minnesota, Minneapolis, Minnesota 55455, United States., Frontiera RR; Department of Chemistry, University of Minnesota, Minneapolis, Minnesota 55455, United States., Rossky PJ; Center for Adopting Flaws as Features, Urbana, Illinois 61801, United States.; Department of Chemistry, Rice University, Houston, Texas 77005, United States., Zanni MT; Center for Adopting Flaws as Features, Urbana, Illinois 61801, United States.; Department of Chemistry, University of Wisconsin Madison, Madison, Wisconsin 53706, United States., Roberts ST; Department of Chemistry, The University of Texas at Austin, Austin, Texas 78712, United States.; Center for Adopting Flaws as Features, Urbana, Illinois 61801, United States.
Jazyk:	angličtina
Zdroj:	The journal of physical chemistry letters [J Phys Chem Lett] 2023 Dec 21; Vol. 14 (50), pp. 11497-11505. Date of Electronic Publication: 2023 Dec 13.
DOI:	10.1021/acs.jpclett.3c02845
Abstrakt:	Materials that undergo singlet fission are of interest for their use in light-harvesting, photocatalysis, and quantum information science, but their ability to undergo fission can be sensitive to local variations in molecular packing. Herein we employ transient absorption microscopy, molecular dynamics simulations, and electronic structure calculations to interrogate how structures found at the edges of orthorhombic rubrene crystals impact singlet fission. Within a micrometer-scale spatial region at the edges of rubrene crystals, we find that the rate of singlet fission increases nearly 4-fold. This observation is consistent with formation of a region at crystal edges with reduced order that accelerates singlet fission by disrupting the symmetry found in rubrene's orthorhombic crystal structure. Our work demonstrates that structural distortions of singlet fission materials can be used to control fission in time and in space, potentially offering a means of controlling this process in light harvesting and quantum information applications.
Databáze:	MEDLINE
Externí odkaz:	Zobrazit plný text záznamu