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Title: Aggregation control in natural brush-printed conjugated polymer films and implications for enhancing charge transport

Abstract

Shear-printing is an enticing processing technique in organic electronics for microstructure/charge transport modification and large-area film fabrication. Nevertheless, the mechanism by which shear-printing can enhance charge transport is not well-understood. In this study, a printing approach using natural brushes is adopted as an informative tool to realize direct aggregation control of conjugated polymers and to investigate the interplay between printing parameters, macromolecule backbone alignment and aggregation, and charge transport anisotropy in a conjugated polymer series differing in architecture and electronic structure. This series includes ( i) semicrystalline hole-transporting P3HT, ( ii) semicrystalline electron-transporting N2200, ( iii) low-crystallinity hole-transporting PBDTT-FTTE, and ( iv) low-crystallinity conducting PEDOT:PSS. The (semi-)conducting films are characterized by a battery of morphology and microstructure analysis techniques and by charge transport measurements. We report that remarkably enhanced mobilities/conductivities, as high as 5.7×/3.9×, are achieved by controlled growth of nanofibril aggregates and by backbone alignment, with the adjustedR 2( R 2 adj) correlation between aggregation and charge transport as high as 95%. Yet, while shear-induced aggregation is important for enhancing charge transport, backbone alignment alone does not guarantee charge transport anisotropy. The correlations between efficient charge transport and aggregation are clearly shown, while mobility and degree of orientation aremore » not always well-correlated. These observations offer insights into macroscopic charge transport mechanisms in conjugated polymers and suggest guidelines for optimization.« less

Authors:
 [1];  [1];  [1];  [2];  [3];  [1];  [1];  [1];  [4];  [1];  [1];  [3];  [1];  [1];  [5];  [1]
  1. Northwestern Univ., Evanston, IL (United States)
  2. Northwestern Univ., Evanston, IL (United States); Flexterra, Inc., Skokie, IL (United States); Linköping Univ. (Sweden)
  3. Northwestern Univ., Evanston, IL (United States); Argonne National Lab. (ANL), Argonne, IL (United States)
  4. Flexterra, Inc., Skokie, IL (United States)
  5. Northwestern Univ., Evanston, IL (United States); Flexterra, Inc., Skokie, IL (United States)
Publication Date:
Research Org.:
Northwestern Univ., Evanston, IL (United States). Energy Frontier Research Center (EFRC) Argonne-Northwestern Solar Energy Research Center (ANSER)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); Swedish Research Council (SRC); US Air Force Office of Scientific Research (AFOSR); National Science Foundation (NSF)
OSTI Identifier:
1470379
Grant/Contract Number:  
[SC0001059]
Resource Type:
Accepted Manuscript
Journal Name:
Proceedings of the National Academy of Sciences of the United States of America
Additional Journal Information:
[ Journal Volume: 114; Journal Issue: 47; Related Information: ANSER partners with Northwestern University (lead); Argonne National Laboratory; University of Chicago; University of Illinois, Urbana-Champaign; Yale University]; Journal ID: ISSN 0027-8424
Publisher:
National Academy of Sciences
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; natural brush-printing; shear effects; polymer alignment; polymer aggregation; polymer charge; transport

Citation Formats

Wang, Gang, Huang, Wei, Eastham, Nicholas D., Fabiano, Simone, Manley, Eric F., Zeng, Li, Wang, Binghao, Zhang, Xinan, Chen, Zhihua, Li, Ran, Chang, Robert P. H., Chen, Lin X., Bedzyk, Michael J., Melkonyan, Ferdinand S., Facchetti, Antonio, and Marks, Tobin J. Aggregation control in natural brush-printed conjugated polymer films and implications for enhancing charge transport. United States: N. p., 2017. Web. doi:10.1073/pnas.1713634114.
Wang, Gang, Huang, Wei, Eastham, Nicholas D., Fabiano, Simone, Manley, Eric F., Zeng, Li, Wang, Binghao, Zhang, Xinan, Chen, Zhihua, Li, Ran, Chang, Robert P. H., Chen, Lin X., Bedzyk, Michael J., Melkonyan, Ferdinand S., Facchetti, Antonio, & Marks, Tobin J. Aggregation control in natural brush-printed conjugated polymer films and implications for enhancing charge transport. United States. doi:10.1073/pnas.1713634114.
Wang, Gang, Huang, Wei, Eastham, Nicholas D., Fabiano, Simone, Manley, Eric F., Zeng, Li, Wang, Binghao, Zhang, Xinan, Chen, Zhihua, Li, Ran, Chang, Robert P. H., Chen, Lin X., Bedzyk, Michael J., Melkonyan, Ferdinand S., Facchetti, Antonio, and Marks, Tobin J. Mon . "Aggregation control in natural brush-printed conjugated polymer films and implications for enhancing charge transport". United States. doi:10.1073/pnas.1713634114. https://www.osti.gov/servlets/purl/1470379.
@article{osti_1470379,
title = {Aggregation control in natural brush-printed conjugated polymer films and implications for enhancing charge transport},
author = {Wang, Gang and Huang, Wei and Eastham, Nicholas D. and Fabiano, Simone and Manley, Eric F. and Zeng, Li and Wang, Binghao and Zhang, Xinan and Chen, Zhihua and Li, Ran and Chang, Robert P. H. and Chen, Lin X. and Bedzyk, Michael J. and Melkonyan, Ferdinand S. and Facchetti, Antonio and Marks, Tobin J.},
abstractNote = {Shear-printing is an enticing processing technique in organic electronics for microstructure/charge transport modification and large-area film fabrication. Nevertheless, the mechanism by which shear-printing can enhance charge transport is not well-understood. In this study, a printing approach using natural brushes is adopted as an informative tool to realize direct aggregation control of conjugated polymers and to investigate the interplay between printing parameters, macromolecule backbone alignment and aggregation, and charge transport anisotropy in a conjugated polymer series differing in architecture and electronic structure. This series includes (i) semicrystalline hole-transporting P3HT, (ii) semicrystalline electron-transporting N2200, (iii) low-crystallinity hole-transporting PBDTT-FTTE, and (iv) low-crystallinity conducting PEDOT:PSS. The (semi-)conducting films are characterized by a battery of morphology and microstructure analysis techniques and by charge transport measurements. We report that remarkably enhanced mobilities/conductivities, as high as 5.7×/3.9×, are achieved by controlled growth of nanofibril aggregates and by backbone alignment, with the adjustedR2(R2adj) correlation between aggregation and charge transport as high as 95%. Yet, while shear-induced aggregation is important for enhancing charge transport, backbone alignment alone does not guarantee charge transport anisotropy. The correlations between efficient charge transport and aggregation are clearly shown, while mobility and degree of orientation are not always well-correlated. These observations offer insights into macroscopic charge transport mechanisms in conjugated polymers and suggest guidelines for optimization.},
doi = {10.1073/pnas.1713634114},
journal = {Proceedings of the National Academy of Sciences of the United States of America},
number = [47],
volume = [114],
place = {United States},
year = {2017},
month = {11}
}

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