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Title: Transport of Spin-Entangled Triplet Excitons Generated by Singlet Fission

Abstract

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 cm(2)s(-1) at 5 K, approaching that for the free singlet excitons, which we attribute to the spin-entangled correlated triplet pair state (1)[TT]. 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.

Authors:
 [1];  [2]; ORCiD logo [3]; ORCiD logo [4]; ORCiD logo [5]
+ Show Author Affiliations
  1. Beijing Normal University (China); Purdue Univ., West Lafayette, IN (United States)
  2. Argonne National Lab. (ANL), Argonne, IL (United States)
  3. Argonne National Lab. (ANL), Argonne, IL (United States); Northwestern Univ., Evanston, IL (United States)
  4. National Renewable Energy Lab. (NREL), Golden, CO (United States)
  5. Purdue Univ., West Lafayette, IN (United States)
Publication Date:
Research Org.:
National Renewable Energy Laboratory (NREL), Golden, CO (United States); Argonne National Laboratory (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences, and Biosciences Division
OSTI Identifier:
1485559
Alternate Identifier(s):
OSTI ID: 1510069
Report Number(s):
NREL/JA-5900-70909
Journal ID: ISSN 1948-7185
Grant/Contract Number:  
AC36-08GO28308; AC02-06CH11357
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Physical Chemistry Letters
Additional Journal Information:
Journal Volume: 9; Journal Issue: 23; Journal ID: ISSN 1948-7185
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; diffusion constant; intermediate state; Shockley-Queisser limits; singlet and triplet state; spintronic applications; temperature dependent; transient absorption; transport of spin

Citation Formats

Wan, Yan, Wiederrecht, Gary P., Schaller, Richard D., Johnson, Justin C., and Huang, Libai. Transport of Spin-Entangled Triplet Excitons Generated by Singlet Fission. United States: N. p., 2018. Web. doi:10.1021/acs.jpclett.8b02944.
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Wan, Yan, Wiederrecht, Gary P., Schaller, Richard D., Johnson, Justin C., & Huang, Libai. Transport of Spin-Entangled Triplet Excitons Generated by Singlet Fission. United States. https://doi.org/10.1021/acs.jpclett.8b02944
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Wan, Yan, Wiederrecht, Gary P., Schaller, Richard D., Johnson, Justin C., and Huang, Libai. Wed . "Transport of Spin-Entangled Triplet Excitons Generated by Singlet Fission". United States. https://doi.org/10.1021/acs.jpclett.8b02944. https://www.osti.gov/servlets/purl/1485559.
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@article{osti_1485559,
title = {Transport of Spin-Entangled Triplet Excitons Generated by Singlet Fission},
author = {Wan, Yan and Wiederrecht, Gary P. and Schaller, Richard D. and Johnson, Justin C. and Huang, Libai},
abstractNote = {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 cm(2)s(-1) at 5 K, approaching that for the free singlet excitons, which we attribute to the spin-entangled correlated triplet pair state (1)[TT]. 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.},
doi = {10.1021/acs.jpclett.8b02944},
journal = {Journal of Physical Chemistry Letters},
number = 23,
volume = 9,
place = {United States},
year = {Wed Nov 07 00:00:00 EST 2018},
month = {Wed Nov 07 00:00:00 EST 2018}
}
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https://doi.org/10.1021/acs.jpclett.8b02944
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    Works referencing / citing this record:

    Time dependent correlations of entangled states with nondegenerate branches and possible experimental realization using singlet fission
    journal, September 2019

    • Bardeen, Christopher J.
    • The Journal of Chemical Physics, Vol. 151, Issue 12
    • DOI: 10.1063/1.5117155

    Coupled double triplet state in singlet fission
    journal, January 2018

    • Kim, Hyungjun; Zimmerman, Paul M.
    • Physical Chemistry Chemical Physics, Vol. 20, Issue 48
    • DOI: 10.1039/c8cp06256k

    Weakly coupled triplet pair states probed by quantum beating in delayed fluorescence in tetracene crystals
    journal, October 2019

    • Wang, Zhiwei; Zhang, Chunfeng; Wang, Rui
    • The Journal of Chemical Physics, Vol. 151, Issue 13
    • DOI: 10.1063/1.5110188

    Routes to singlet exciton fission in rubrene crystals and amorphous films
    journal, September 2019

    • Finton, Drew M.; Wolf, Eric A.; Zoutenbier, Vincent S.
    • AIP Advances, Vol. 9, Issue 9
    • DOI: 10.1063/1.5118942

    Anisotropic Singlet Fission in Single Crystalline Hexacene
    journal, September 2019

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