Quintet multiexciton dynamics in singlet fission

Tayebjee, Murad J.  Y.; Sanders, Samuel N.; Kumarasamy, Elango; Campos, Luis M.; Sfeir, Matthew Y.; McCamey, Dane R.

doi:10.1038/NPHYS3909

Title: Quintet multiexciton dynamics in singlet fission

Journal Article · Mon Oct 17 00:00:00 EDT 2016 · Nature Physics

DOI:https://doi.org/10.1038/NPHYS3909· OSTI ID:1394748

^[1]; Sanders, Samuel N. ^[2]; Kumarasamy, Elango ^[2]; Campos, Luis M. ^[2];

^[3]; McCamey, Dane R. ^[4]

Univ. of New South Wales, Sydney, NSW (Australia). School of Photovoltaic and Renewable Energy Engineering
Columbia Univ., New York, NY (United States). Dept. of Chemistry
Brookhaven National Lab. (BNL), Upton, NY (United States). Center for Functional Nanomaterials
Univ. of New South Wales, Sydney, NSW (Australia). School of Physics

Singlet fission, in which two triplet excitons are generated from a single absorbed photon, is a key third-generation solar cell concept. Conservation of angular momentum requires that singlet fission populates correlated multiexciton states, which can subsequently dissociate to generate free triplets. However, little is known about electronic and spin correlations in these systems since, due to its typically short lifetime, the multiexciton state is challenging to isolate and study. Here, we use bridged pentacene dimers, which undergo intramolecular singlet fission while isolated in solution and in solid matrices, as a unimolecular model system that can trap long-lived multiexciton states. We also combine transient absorption and time-resolved electron spin resonance spectroscopies to show that spin correlations in the multiexciton state persist for hundreds of nanoseconds. Furthermore, we confirm long-standing predictions that singlet fission produces triplet pair states of quintet character. Finally, we compare two different pentacene–bridge–pentacene chromophores, systematically tuning the coupling between the pentacenes to understand how differences in molecular structure affect the population and dissociation of multiexciton quintet states.

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Research Organization:: Brookhaven National Laboratory (BNL), Upton, NY (United States). Center for Functional Nanomaterials (CFN)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: SC0012704

OSTI ID:: 1394748

Report Number(s):: BNL-114013-2017-JA; KC0403020; TRN: US1702595

Journal Information:: Nature Physics, Vol. 13, Issue 2; ISSN 1745-2473

Publisher:: Nature Publishing Group (NPG)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 197 works

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
chemical physics
electronic properties and materials
molecular electronics