Lattice Symmetry-Guided Charge Transport in 2D Supramolecular Polymers Promotes Triplet Formation.

Autor: Emmanuele R; Center for Nanoscale Materials, Argonne National Laboratory, Lemont, IL, 60439, USA., Sai H; Simpson Querrey Institute for BioNanotechnology, Northwestern University, Chicago, IL, 60611, USA., Chen JS; Center for Nanoscale Materials, Argonne National Laboratory, Lemont, IL, 60439, USA.; Simpson Querrey Institute for BioNanotechnology, Northwestern University, Chicago, IL, 60611, USA.; Center for Molecular Quantum Transduction, Northwestern University, Evanston, IL, 60208, USA., Morrow DJ; Center for Nanoscale Materials, Argonne National Laboratory, Lemont, IL, 60439, USA., Đorđević L; Department of Chemistry, Northwestern University, Evanston, IL, 60208, USA., Gosztola DJ; Center for Nanoscale Materials, Argonne National Laboratory, Lemont, IL, 60439, USA., Hla SW; Center for Nanoscale Materials, Argonne National Laboratory, Lemont, IL, 60439, USA.; Nanoscale and Quantum Phenomena Institute and Department of Physics and Astronomy, Ohio University, Athens, OH, 45701, USA., Stupp SI; Simpson Querrey Institute for BioNanotechnology, Northwestern University, Chicago, IL, 60611, USA.; Department of Chemistry, Northwestern University, Evanston, IL, 60208, USA.; Department of Materials Science and Engineering, Northwestern University, Evanston, IL, 60208, USA.; Department of Medicine, Northwestern University, Chicago, IL, 60611, USA., Ma X; Center for Nanoscale Materials, Argonne National Laboratory, Lemont, IL, 60439, USA.; Center for Molecular Quantum Transduction, Northwestern University, Evanston, IL, 60208, USA.; Consortium for Advanced Science and Engineering, University of Chicago, Chicago, IL, 60637, USA.
Jazyk: angličtina
Zdroj: Advanced science (Weinheim, Baden-Wurttemberg, Germany) [Adv Sci (Weinh)] 2024 Aug; Vol. 11 (30), pp. e2402932. Date of Electronic Publication: 2024 Jun 12.
DOI: 10.1002/advs.202402932
Abstrakt: Singlet-to-triplet intersystem crossing (ISC) in organic molecules is intimately connected with their geometries: by modifying the molecular shape, symmetry selection rules pertaining to spin-orbit coupling can be partially relieved, leading to extra matrix elements for increased ISC. As an analog to this molecular design concept, the study finds that the lattice symmetry of supramolecular polymers also defines their triplet formation efficiencies. A supramolecular polymer self-assembled from weakly interacting molecules is considered. Its 2D oblique unit cell effectively renders it as a coplanar array of 1D molecular columns weakly bound to each other. Using momentum-resolved photoluminescence imaging in combination with Monte Carlo simulations, the study found that photogenerated charge carriers in the supramolecular polymer predominantly recombine as spin-uncorrelated carrier pairs through inter-column charge transfer states. This lattice-defined recombination pathway leads to a substantial triplet formation efficiency (≈60%) in the supramolecular polymer. These findings suggest that lattice symmetry of micro-/macroscopic structures relying on intermolecular interactions can be strategized for controlled triplet formation.
(© 2024 UChicago Argonne, LLC and The Author(s). Advanced Science published by Wiley‐VCH GmbH.)
Databáze: MEDLINE
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