Preferential Charge Generation at Aggregate Sites in Narrow Band Gap Infrared Photoresponsive Polymer Semiconductors
Abstract
Abstract Infrared organic photodetector materials are investigated using transient absorption spectroscopy, demonstrating that ultrafast charge generation assisted by polymer aggregation is essential to compensate for the energy gap law, which dictates that excited state lifetimes decrease as the band gap narrows. Short sub‐picosecond singlet exciton lifetimes are measured in a structurally related series of infrared‐absorbing copolymers that consist of alternating cyclopentadithiophene electron‐rich “push” units and strong electron‐deficient “pull” units, including benzothiadiazole, benzoselenadiazole, pyridalselenadiazole, or thiadiazoloquinoxaline. While the ultrafast lifetimes of excitons localized on individual polymer chains suggest that charge carrier generation will be inefficient, high detectivity for polymer:PC 71 BM infrared photodetectors is measured in the 0.6 < λ < 1.5 µm range. The photophysical processes leading to charge generation are investigated by performing a global analysis on transient absorption data of blended polymer:PC 71 BM films. In these blends, charge carriers form primarily at polymer aggregate sites on the ultrafast time scale (within our instrument response), leaving quickly decaying single‐chain excitons unquenched. The results have important implications for the further development of organic infrared optoelectronic devices, where targeting processes such as excited state delocalization over aggregates may be necessary to mitigate losses to ultrafast exciton decay as materials withmore »
- Authors:
-
- Univ. of Washington, Seattle, WA (United States)
- Univ. of Southern Mississippi, Hattiesburg, MS (United States)
- Univ. of California, Riverside, CA (United States)
- Univ. of California San Diego, La Jolla, CA (United States)
- Brookhaven National Lab. (BNL), Upton, NY (United States)
- Publication Date:
- Research Org.:
- Brookhaven National Laboratory (BNL), Upton, NY (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1454810
- Alternate Identifier(s):
- OSTI ID: 1420339
- Report Number(s):
- BNL-205769-2018-JAAM
Journal ID: ISSN 2195-1071
- Grant/Contract Number:
- SC0012704; DE‐SC0016269
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Advanced Optical Materials
- Additional Journal Information:
- Journal Volume: 6; Journal Issue: 7; Journal ID: ISSN 2195-1071
- Publisher:
- Wiley
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 36 MATERIALS SCIENCE; organic electronics; ultrafast spectroscopy; delocalization; push-pull; bulk heterojunction
Citation Formats
Sulas, Dana B., London, Alexander E., Huang, Lifeng, Xu, Lihua, Wu, Zhenghui, Ng, Tse Nga, Wong, Bryan M., Schlenker, Cody W., Azoulay, Jason D., and Sfeir, Matthew Y. Preferential Charge Generation at Aggregate Sites in Narrow Band Gap Infrared Photoresponsive Polymer Semiconductors. United States: N. p., 2018.
Web. doi:10.1002/adom.201701138.
Sulas, Dana B., London, Alexander E., Huang, Lifeng, Xu, Lihua, Wu, Zhenghui, Ng, Tse Nga, Wong, Bryan M., Schlenker, Cody W., Azoulay, Jason D., & Sfeir, Matthew Y. Preferential Charge Generation at Aggregate Sites in Narrow Band Gap Infrared Photoresponsive Polymer Semiconductors. United States. https://doi.org/10.1002/adom.201701138
Sulas, Dana B., London, Alexander E., Huang, Lifeng, Xu, Lihua, Wu, Zhenghui, Ng, Tse Nga, Wong, Bryan M., Schlenker, Cody W., Azoulay, Jason D., and Sfeir, Matthew Y. Tue .
"Preferential Charge Generation at Aggregate Sites in Narrow Band Gap Infrared Photoresponsive Polymer Semiconductors". United States. https://doi.org/10.1002/adom.201701138. https://www.osti.gov/servlets/purl/1454810.
@article{osti_1454810,
title = {Preferential Charge Generation at Aggregate Sites in Narrow Band Gap Infrared Photoresponsive Polymer Semiconductors},
author = {Sulas, Dana B. and London, Alexander E. and Huang, Lifeng and Xu, Lihua and Wu, Zhenghui and Ng, Tse Nga and Wong, Bryan M. and Schlenker, Cody W. and Azoulay, Jason D. and Sfeir, Matthew Y.},
abstractNote = {Abstract Infrared organic photodetector materials are investigated using transient absorption spectroscopy, demonstrating that ultrafast charge generation assisted by polymer aggregation is essential to compensate for the energy gap law, which dictates that excited state lifetimes decrease as the band gap narrows. Short sub‐picosecond singlet exciton lifetimes are measured in a structurally related series of infrared‐absorbing copolymers that consist of alternating cyclopentadithiophene electron‐rich “push” units and strong electron‐deficient “pull” units, including benzothiadiazole, benzoselenadiazole, pyridalselenadiazole, or thiadiazoloquinoxaline. While the ultrafast lifetimes of excitons localized on individual polymer chains suggest that charge carrier generation will be inefficient, high detectivity for polymer:PC 71 BM infrared photodetectors is measured in the 0.6 < λ < 1.5 µm range. The photophysical processes leading to charge generation are investigated by performing a global analysis on transient absorption data of blended polymer:PC 71 BM films. In these blends, charge carriers form primarily at polymer aggregate sites on the ultrafast time scale (within our instrument response), leaving quickly decaying single‐chain excitons unquenched. The results have important implications for the further development of organic infrared optoelectronic devices, where targeting processes such as excited state delocalization over aggregates may be necessary to mitigate losses to ultrafast exciton decay as materials with even lower band gaps are developed.},
doi = {10.1002/adom.201701138},
journal = {Advanced Optical Materials},
number = 7,
volume = 6,
place = {United States},
year = {Tue Feb 13 00:00:00 EST 2018},
month = {Tue Feb 13 00:00:00 EST 2018}
}
Web of Science
Figures / Tables:
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