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Optically accessible long-lived electronic biexcitons at room temperature in strongly coupled H- aggregates

Siddhartha Sohoni, Indranil Ghosh, Geoffrey T. Nash, Claire A. Jones, Lawson T. Lloyd, Beiye C. Li, Karen L. Ji, Zitong Wang, Wenbin Lin and Gregory S. Engel ()
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Siddhartha Sohoni: The University of Chicago
Indranil Ghosh: The University of Chicago
Geoffrey T. Nash: The University of Chicago
Claire A. Jones: The University of Chicago
Lawson T. Lloyd: The University of Chicago
Beiye C. Li: The University of Chicago
Karen L. Ji: The University of Chicago
Zitong Wang: The University of Chicago
Wenbin Lin: The University of Chicago
Gregory S. Engel: The University of Chicago

Nature Communications, 2024, vol. 15, issue 1, 1-9

Abstract: Abstract Photon absorption is the first process in light harvesting. Upon absorption, the photon redistributes electrons in the materials to create a Coulombically bound electron-hole pair called an exciton. The exciton subsequently separates into free charges to conclude light harvesting. When two excitons are in each other’s proximity, they can interact and undergo a two-particle process called exciton-exciton annihilation. In this process, one electron-hole pair spontaneously recombines: its energy is lost and cannot be harnessed for applications. In this work, we demonstrate the creation of two long-lived excitons on the same chromophore site (biexcitons) at room temperature in a strongly coupled H-aggregated zinc phthalocyanine material. We show that exciton-exciton annihilation is suppressed in these H- aggregated chromophores at fluences many orders of magnitudes higher than solar light. When we chemically connect the same aggregated chromophores to allow exciton diffusion, we observe that exciton-exciton annihilation is switched on. Our findings demonstrate a chemical strategy, to toggle on and off the exciton-exciton annihilation process that limits the dynamic range of photovoltaic devices.

Date: 2024
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DOI: 10.1038/s41467-024-52341-2

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