Preferential Charge Generation at Aggregate Sites in Narrow Band Gap Infrared Photoresponsive Polymer Semiconductors

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.

doi:10.1002/adom.201701138

Title: Preferential Charge Generation at Aggregate Sites in Narrow Band Gap Infrared Photoresponsive Polymer Semiconductors

Journal Article · Tue Feb 13 00:00:00 EST 2018 · Advanced Optical Materials

DOI:https://doi.org/10.1002/adom.201701138· OSTI ID:1454810

Sulas, Dana B. ^[1];

^[2]; Huang, Lifeng ^[2]; Xu, Lihua ^[3];

^[4]; Ng, Tse Nga ^[4]; Wong, Bryan M. ^[3]; Schlenker, Cody W. ^[1];

^[2];

^[5]

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)

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.

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Research Organization:: Brookhaven National Laboratory (BNL), Upton, NY (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: SC0012704; DE‐SC0016269

OSTI ID:: 1454810

Alternate ID(s):: OSTI ID: 1420339

Report Number(s):: BNL-205769-2018-JAAM

Journal Information:: Advanced Optical Materials, Vol. 6, Issue 7; ISSN 2195-1071

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 26 works

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