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Title: Observation of Two Triplet-Pair Intermediates in Singlet Exciton Fission

Authors:
 [1];  [1];  [2];  [3];  [4];  [3];  [4];  [2];  [3];  [1]
  1. Department of Chemistry, Princeton University, Princeton, New Jersey 08544, United States
  2. Department of Chemistry, University of Toronto, Toronto, Ontario M5S 3H6, Canada
  3. Department of Chemistry, University of Kentucky, Lexington, Kentucky 40506, United States
  4. Department of Chemistry, The Pennsylvania State University, University Park, Pennsylvania 16802, United States
Publication Date:
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1414335
Grant/Contract Number:
SC0008120
Resource Type:
Journal Article: Published Article
Journal Name:
Journal of Physical Chemistry Letters
Additional Journal Information:
Journal Volume: 7; Journal Issue: 13; Related Information: CHORUS Timestamp: 2017-12-20 15:28:19; Journal ID: ISSN 1948-7185
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English

Citation Formats

Pensack, Ryan D., Ostroumov, Evgeny E., Tilley, Andrew J., Mazza, Samuel, Grieco, Christopher, Thorley, Karl J., Asbury, John B., Seferos, Dwight S., Anthony, John E., and Scholes, Gregory D.. Observation of Two Triplet-Pair Intermediates in Singlet Exciton Fission. United States: N. p., 2016. Web. doi:10.1021/acs.jpclett.6b00947.
Pensack, Ryan D., Ostroumov, Evgeny E., Tilley, Andrew J., Mazza, Samuel, Grieco, Christopher, Thorley, Karl J., Asbury, John B., Seferos, Dwight S., Anthony, John E., & Scholes, Gregory D.. Observation of Two Triplet-Pair Intermediates in Singlet Exciton Fission. United States. doi:10.1021/acs.jpclett.6b00947.
Pensack, Ryan D., Ostroumov, Evgeny E., Tilley, Andrew J., Mazza, Samuel, Grieco, Christopher, Thorley, Karl J., Asbury, John B., Seferos, Dwight S., Anthony, John E., and Scholes, Gregory D.. 2016. "Observation of Two Triplet-Pair Intermediates in Singlet Exciton Fission". United States. doi:10.1021/acs.jpclett.6b00947.
@article{osti_1414335,
title = {Observation of Two Triplet-Pair Intermediates in Singlet Exciton Fission},
author = {Pensack, Ryan D. and Ostroumov, Evgeny E. and Tilley, Andrew J. and Mazza, Samuel and Grieco, Christopher and Thorley, Karl J. and Asbury, John B. and Seferos, Dwight S. and Anthony, John E. and Scholes, Gregory D.},
abstractNote = {},
doi = {10.1021/acs.jpclett.6b00947},
journal = {Journal of Physical Chemistry Letters},
number = 13,
volume = 7,
place = {United States},
year = 2016,
month = 6
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record at 10.1021/acs.jpclett.6b00947

Citation Metrics:
Cited by: 29works
Citation information provided by
Web of Science

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  • By direct imaging of singlet and triplet populations with ultrafast microscopy, it is shown that the triplet diffusion length and singlet fission yield can be simultaneously optimized for tetracene and its derivatives, making them ideal structures for application in bilayer solar cells.
  • Singlet fission, the conversion of a singlet exciton (S 1) to two triplets (2 × T 1), may increase the solar energy conversion efficiency beyond the Shockley-Queisser limit. This process is believed to involve the correlated triplet pair state 1(TT). Despite extensive research, the nature of the 1(TT) state and its spectroscopic signature remain actively debated. We use an end-connected pentacene dimer (BP0) as a model system and show evidence for a tightly bound 1(TT) state. It is characterized in the near-infrared (IR) region (~1.0 eV) by a distinct excited-state absorption (ESA) spectral feature, which closely resembles that of themore » S 1 state; both show vibronic progressions of the aromatic ring breathing mode. We assign these near-IR spectra to 1(TT)→S n and S 1→S n' transitions; S n and S n' likely come from the antisymmetric and symmetric linear combinations, respectively, of the S 2 state localized on each pentacene unit in the dimer molecule. The 1(TT)→S n transition is an indicator of the intertriplet electronic coupling strength, because inserting a phenylene spacer or twisting the dihedral angle between the two pentacene chromophores decreases the intertriplet electronic coupling and diminishes this ESA peak. In addition to spectroscopic signature, the tightly bound 1(TT) state also shows chemical reactivity that is distinctively different from that of an individual T 1 state. Using an electron-accepting iron oxide molecular cluster [Fe 8O 4] linked to the pentacene or pentacene dimer (BP0), we show that electron transfer to the cluster occurs efficiently from an individual T 1 in pentacene but not from the tightly bound 1(TT) state. Thus, reducing intertriplet electronic coupling in 1(TT) via molecular design might be necessary for the efficient harvesting of triplets from intramolecular singlet fission.« less