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Title: Extreme electron polaron spatial delocalization in π-conjugated materials

Abstract

The electron polaron, a spin-1/2 excitation, is the fundamental negative charge carrier in π-conjugated organic materials. Large polaron spatial dimensions result from weak electron-lattice coupling and thus identify materials with unusually low barriers for the charge transfer reactions that are central to electronic device applications. In this paper, we demonstrate electron polarons in π-conjugated multiporphyrin arrays that feature vast areal delocalization. This finding is evidenced by concurrent optical and electron spin resonance measurements, coupled with electronic structure calculations that suggest atypically small reorganization energies for one-electron reduction of these materials. Finally, because the electron polaron dimension can be linked to key performance metrics in organic photovoltaics, light-emitting diodes, and a host of other devices, these findings identify conjugated materials with exceptional optical, electronic, and spintronic properties.

Authors:
 [1];  [2];  [1]
+ Show Author Affiliations
  1. Department of Chemistry, Duke University, Durham, NC 27708,
  2. Department of Physics, Saint Joseph’s University, Philadelphia, PA 19131
Publication Date:
Research Org.:
Duke Univ., Durham, NC (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1235120
Alternate Identifier(s):
OSTI ID: 1347987
Grant/Contract Number:  
SC0001517
Resource Type:
Published Article
Journal Name:
Proceedings of the National Academy of Sciences of the United States of America
Additional Journal Information:
Journal Name: Proceedings of the National Academy of Sciences of the United States of America Journal Volume: 112 Journal Issue: 45; Journal ID: ISSN 0027-8424
Publisher:
Proceedings of the National Academy of Sciences
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; electron; polaron; delocalized; organic; conjugated

Citation Formats

Rawson, Jeff, Angiolillo, Paul J., and Therien, Michael J. Extreme electron polaron spatial delocalization in π-conjugated materials. United States: N. p., 2015. Web. doi:10.1073/pnas.1512318112.
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Rawson, Jeff, Angiolillo, Paul J., & Therien, Michael J. Extreme electron polaron spatial delocalization in π-conjugated materials. United States. https://doi.org/10.1073/pnas.1512318112
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Rawson, Jeff, Angiolillo, Paul J., and Therien, Michael J. Wed . "Extreme electron polaron spatial delocalization in π-conjugated materials". United States. https://doi.org/10.1073/pnas.1512318112.
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@article{osti_1235120,
title = {Extreme electron polaron spatial delocalization in π-conjugated materials},
author = {Rawson, Jeff and Angiolillo, Paul J. and Therien, Michael J.},
abstractNote = {The electron polaron, a spin-1/2 excitation, is the fundamental negative charge carrier in π-conjugated organic materials. Large polaron spatial dimensions result from weak electron-lattice coupling and thus identify materials with unusually low barriers for the charge transfer reactions that are central to electronic device applications. In this paper, we demonstrate electron polarons in π-conjugated multiporphyrin arrays that feature vast areal delocalization. This finding is evidenced by concurrent optical and electron spin resonance measurements, coupled with electronic structure calculations that suggest atypically small reorganization energies for one-electron reduction of these materials. Finally, because the electron polaron dimension can be linked to key performance metrics in organic photovoltaics, light-emitting diodes, and a host of other devices, these findings identify conjugated materials with exceptional optical, electronic, and spintronic properties.},
doi = {10.1073/pnas.1512318112},
journal = {Proceedings of the National Academy of Sciences of the United States of America},
number = 45,
volume = 112,
place = {United States},
year = {Wed Oct 28 00:00:00 EDT 2015},
month = {Wed Oct 28 00:00:00 EDT 2015}
}
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https://doi.org/10.1073/pnas.1512318112
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