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Title: Long-Lived Correlated Triplet Pairs in a π-Stacked Crystalline Pentacene Derivative

Abstract

Singlet fission is the spin-conserving process by which a singlet exciton splits into two triplet excitons. Singlet fission occurs via a correlated triplet pair intermediate, but direct evidence of this state has been scant, and in films of TIPS-pentacene, a small molecule organic semiconductor, even the rate of fission has been unclear. We use polarization-resolved transient absorption microscopy on individual crystalline domains of TIPS-pentacene to establish the fission rate and demonstrate that the initially created triplets remain bound for a surprisingly long time, hundreds of picoseconds, before separating. Furthermore, using a broadband probe, we show that it is possible to determine absorbance spectra of individual excited species in a crystalline solid. We find that triplet interactions perturb the absorbance, and provide evidence that triplet interaction and binding could be caused by the π-stacked geometry. Elucidating the relationship between the lattice structure and the electronic structure and dynamics has important implications for the creation of photovoltaic devices that aim to boost efficiency via singlet fission.

Authors:
 [1];  [1];  [2];  [3]; ORCiD logo [4]
  1. Univ. of California, Berkeley, CA (United States). Dept. of Physics
  2. Univ. of California, Berkeley, CA (United States). Dept. of Physics; Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Molecular Foundry
  3. Univ. of California, Berkeley, CA (United States). Dept. of Physics; Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Molecular Foundry; Kavli Energy NanoSciences Institute, Berkeley, CA (United States)
  4. Univ. of California, Berkeley, CA (United States). Dept. of Physics, and Dept. of Chemistry; Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Molecular Biophysics and Integrated Bioimaging, and Materials Sciences Divisions; Kavli Energy NanoSciences Institute, Berkeley, CA United States
Publication Date:
Research Org.:
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). National Energy Research Scientific Computing Center (NERSC); Univ. of California, Oakland, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1543721
Grant/Contract Number:  
AC02-05CH11231
Resource Type:
Accepted Manuscript
Journal Name:
Journal of the American Chemical Society
Additional Journal Information:
Journal Volume: 140; Journal Issue: 6; Journal ID: ISSN 0002-7863
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Chemistry

Citation Formats

Folie, Brendan D., Haber, Jonah B., Refaely-Abramson, Sivan, Neaton, Jeffrey B., and Ginsberg, Naomi S. Long-Lived Correlated Triplet Pairs in a π-Stacked Crystalline Pentacene Derivative. United States: N. p., 2018. Web. doi:10.1021/jacs.7b12662.
Folie, Brendan D., Haber, Jonah B., Refaely-Abramson, Sivan, Neaton, Jeffrey B., & Ginsberg, Naomi S. Long-Lived Correlated Triplet Pairs in a π-Stacked Crystalline Pentacene Derivative. United States. https://doi.org/10.1021/jacs.7b12662
Folie, Brendan D., Haber, Jonah B., Refaely-Abramson, Sivan, Neaton, Jeffrey B., and Ginsberg, Naomi S. Fri . "Long-Lived Correlated Triplet Pairs in a π-Stacked Crystalline Pentacene Derivative". United States. https://doi.org/10.1021/jacs.7b12662. https://www.osti.gov/servlets/purl/1543721.
@article{osti_1543721,
title = {Long-Lived Correlated Triplet Pairs in a π-Stacked Crystalline Pentacene Derivative},
author = {Folie, Brendan D. and Haber, Jonah B. and Refaely-Abramson, Sivan and Neaton, Jeffrey B. and Ginsberg, Naomi S.},
abstractNote = {Singlet fission is the spin-conserving process by which a singlet exciton splits into two triplet excitons. Singlet fission occurs via a correlated triplet pair intermediate, but direct evidence of this state has been scant, and in films of TIPS-pentacene, a small molecule organic semiconductor, even the rate of fission has been unclear. We use polarization-resolved transient absorption microscopy on individual crystalline domains of TIPS-pentacene to establish the fission rate and demonstrate that the initially created triplets remain bound for a surprisingly long time, hundreds of picoseconds, before separating. Furthermore, using a broadband probe, we show that it is possible to determine absorbance spectra of individual excited species in a crystalline solid. We find that triplet interactions perturb the absorbance, and provide evidence that triplet interaction and binding could be caused by the π-stacked geometry. Elucidating the relationship between the lattice structure and the electronic structure and dynamics has important implications for the creation of photovoltaic devices that aim to boost efficiency via singlet fission.},
doi = {10.1021/jacs.7b12662},
journal = {Journal of the American Chemical Society},
number = 6,
volume = 140,
place = {United States},
year = {2018},
month = {2}
}

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