TY - JOUR
T1 - Transport of Spin-Entangled Triplet Excitons Generated by Singlet Fission
AU - Wan, Yan
AU - Wiederrecht, Gary P.
AU - Schaller, Richard D.
AU - Johnson, Justin C.
AU - Huang, Libai
N1 - Funding Information:
L.H. and Y.W. acknowledge support from US National Science Foundation through grant NSF-CHE-1555005. J.C.J. acknowledges the Solar Photochemistry Program supported by the U.S. Department of Energy, Office of Basic Energy Sciences, Division of Chemical Sciences, Biosciences, and Geosciences under Contract No. DE-AC36-08GO28308 with NREL. Use of the Center for Nanoscale Materials, an Office of Science user facility, was supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, under Contract No. DE-AC02-06CH11357. The views expressed in the article do not necessarily represent the views of the DOE or the U.S. Government. The U.S. Government retains and the publisher, by accepting the article for publication, acknowledges that the U.S. Government retains a nonexclusive, paid-up, irrevocable, worldwide license to publish or reproduce the published form of this work, or allow others to do so, for U.S. Government purposes.
Publisher Copyright:
Copyright © 2018 American Chemical Society.
PY - 2018/12/6
Y1 - 2018/12/6
N2 - 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.
AB - 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.
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U2 - 10.1021/acs.jpclett.8b02944
DO - 10.1021/acs.jpclett.8b02944
M3 - Article
C2 - 30403874
AN - SCOPUS:85056825776
SN - 1948-7185
VL - 9
SP - 6731
EP - 6738
JO - Journal of Physical Chemistry Letters
JF - Journal of Physical Chemistry Letters
IS - 23
ER -