Transport of Spin-Entangled Triplet Excitons Generated by Singlet Fission

Wan, Yan; Wiederrecht, Gary P.; Schaller, Richard D.; Johnson, Justin C.; Huang, Libai

doi:10.1021/acs.jpclett.8b02944

Transport of Spin-Entangled Triplet Excitons Generated by Singlet Fission

Journal Article · Wed Nov 07 04:00:00 EST 2018 · Journal of Physical Chemistry Letters

DOI:https://doi.org/10.1021/acs.jpclett.8b02944· OSTI ID:1485559

Wan, Yan ^[1]; Wiederrecht, Gary P. ^[2]; ^[3]; ^[4]; ^[5]

Beijing Normal University (China); Purdue Univ., West Lafayette, IN (United States)
Argonne National Lab. (ANL), Argonne, IL (United States)
Argonne National Lab. (ANL), Argonne, IL (United States); Northwestern Univ., Evanston, IL (United States)
National Renewable Energy Lab. (NREL), Golden, CO (United States)
Purdue Univ., West Lafayette, IN (United States)

We present that singlet fission provides a promising route for overcoming the Shockley-Queisser limit in solar cells using organic materials. Despite singlet fission dynamics having been extensively investigated, the transport of the various intermediates in relation to the singlet and triplet states is largely unknown. Here we employ temperature-dependent ultrafast transient absorption microscopy to image the transport of singlet fission intermediates in single crystals of tetracene. These measurements suggest a mobile singlet fission intermediate state at low temperatures, with a diffusion constant of 36 cm²s^-1 at 5 K, approaching that for the free singlet excitons, which we attribute to the spin-entangled correlated triplet pair state ¹[TT]. In conclusion, these results indicate that ¹[TT] could transport with a similar mechanism as the bright singlet excitons, which has important implications in designing materials for singlet fission and spintronic applications.

View Accepted Manuscript (DOE)

Research Organization:: National Renewable Energy Laboratory (NREL), Golden, CO (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Chemical Sciences, Geosciences & Biosciences Division

Grant/Contract Number:: AC36-08GO28308; AC02-06CH11357

OSTI ID:: 1485559

Alternate ID(s):: OSTI ID: 1510069

Report Number(s):: NREL/JA--5900-70909

Journal Information:: Journal of Physical Chemistry Letters, Journal Name: Journal of Physical Chemistry Letters Journal Issue: 23 Vol. 9; ISSN 1948-7185

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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Coupled double triplet state in singlet fission Kim, Hyungjun; Zimmerman, Paul M. Physical Chemistry Chemical Physics, Vol. 20, Issue 48 https://doi.org/10.1039/c8cp06256k	journal	January 2018
Topology of quantum coherence networks in singlet fission: mapping exciton states into real space and the dislocation induced three dimensional manifolds Tao, Guohua Physical Chemistry Chemical Physics, Vol. 22, Issue 3 https://doi.org/10.1039/c9cp05102c	journal	January 2020
Nonadiabatic simulation of singlet fission dynamics in tetracene clusters: The topology of quantum coherence in a global view Tao, Guohua The Journal of Chemical Physics, Vol. 151, Issue 5 https://doi.org/10.1063/1.5100196	journal	August 2019
Weakly coupled triplet pair states probed by quantum beating in delayed fluorescence in tetracene crystals Wang, Zhiwei; Zhang, Chunfeng; Wang, Rui The Journal of Chemical Physics, Vol. 151, Issue 13 https://doi.org/10.1063/1.5110188	journal	October 2019
Time dependent correlations of entangled states with nondegenerate branches and possible experimental realization using singlet fission Bardeen, Christopher J. The Journal of Chemical Physics, Vol. 151, Issue 12 https://doi.org/10.1063/1.5117155	journal	September 2019
Routes to singlet exciton fission in rubrene crystals and amorphous films Finton, Drew M.; Wolf, Eric A.; Zoutenbier, Vincent S. AIP Advances, Vol. 9, Issue 9 https://doi.org/10.1063/1.5118942	journal	September 2019

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Shockley-Queisser limits
diffusion constant
intermediate state
singlet and triplet state
spintronic applications
temperature dependent
transient absorption
transport of spin

Transport of Spin-Entangled Triplet Excitons Generated by Singlet Fission

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