Excitonic transitions in organic semiconductors are associated with large oscillator strength that limits the excited-state lifetime and can in turn impede long-range exciton migration. We present perylene-based emissive H-aggregate nanowires where the lowest energy state is only weakly coupled to the ground state, thus dramatically enhancing lifetime. Exciton migration occurs by thermally activated hopping, leading to luminescence quenching on topological wire defects. An atomic force microscope tip can introduce local topological quenchers by distorting the H-aggregate structure, demonstrating long-range exciton migration at room temperature and offering a potential route to writing fluorescent "nanobarcodes" and excitonic circuits.
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http://dx.doi.org/10.1021/nl1033039 | DOI Listing |
Sci Adv
January 2025
Department of Physics, University of Arizona, Tucson, AZ 85721, USA.
J Am Chem Soc
January 2025
Department of Chemistry and Center for NanoScience (CeNS), University of Munich (LMU), Butenandtstraße 5-13, Munich 81377, Germany.
Covalent organic frameworks (COFs), crystalline and porous conjugated structures, are of great interest for sustainable energy applications. Organic building blocks in COFs with suitable electronic properties can feature strong optical absorption, whereas the extended crystalline network can establish a band structure enabling long-range coherent transport. This peculiar combination of both molecular and solid-state materials properties makes COFs an interesting platform to study and ultimately utilize photoexcited charge carrier diffusion.
View Article and Find Full Text PDFNanophotonics
June 2024
Nanoscience Center and Department of Chemistry, University of Jyväskylä, P.O. Box 35, 40014 Jyväskylä, Finland.
Placing a material inside an optical cavity can enhance transport of excitation energy by hybridizing excitons with confined light modes into polaritons, which have a dispersion that provides these light-matter quasi-particles with low effective masses and very high group velocities. While in experiments, polariton propagation is typically initiated with laser pulses, tuned to be resonant either with the polaritonic branches that are delocalized over many molecules, or with an uncoupled higher-energy electronic excited state that is localized on a single molecule, practical implementations of polariton-mediated exciton transport into devices would require operation under low-intensity incoherent light conditions. Here, we propose to initiate polaritonic exciton transport with a photo-acid, which upon absorption of a photon in a spectral range not strongly reflected by the cavity mirrors, undergoes ultra-fast excited-state proton transfer into a red-shifted excited-state photo-product that can couple collectively with a large number of suitable dye molecules to the modes of the cavity.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
November 2024
State Key Laboratory of Silicon and Advanced Semiconductor Materials, Department of Polymer Science and Engineering, Zhejiang University, Hangzhou, 310058, China.
There are great demands of developing ultra-narrow bandgap electron acceptors for multifunctional electronic devices, particularly semi-transparent organic photovoltaics (OPVs) for building-integrated applications. However, current ultra-narrow bandgap materials applied in OPVs, primarily based on electron-rich cores, exhibit defects of high-lying energy levels and inferior performance. We herein proposed a novel strategy by designing the benzothiazole-fused cyanoindone (BTC) unit with ultra-strong electron-withdrawing ability as the terminal to synthesize the acceptor BTC-2.
View Article and Find Full Text PDFChem Sci
December 2024
Department of Chemistry and The James Franck Institute, The University of Chicago Chicago IL 60637 USA
Recent experiments have realized exciton condensation in bilayer materials such as graphene double layers and the van der Waals heterostructure MoSe-WSe with the potential for nearly frictionless energy transport. Here we computationally observe the microscopic beginnings of exciton condensation in a molecular-scale fragment of MoSe-WSe, using advanced electronic structure methods based on reduced density matrices. We establish a connection between the signature of exciton condensation-the presence of a large eigenvalue in the particle-hole reduced density matrix-and experimental evidence of exciton condensation in the material.
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