Photovoltaic Blend Microstructure for High Efficiency Post-Fullerene Solar Cells. To Tilt or Not To Tilt?
Abstract
Achieving efficient polymer solar cells (PSCs) requires a structurally optimal donor-acceptor heterojunction morphology. In this paper, we report the combined experimental and theoretical characterization of a benzodithiophene benzothiadiazole donor polymer series (PBTZF4-R; R = alkyl substituent) blended with the non-fullerene acceptor ITIC-Th, and analyse the effects of substituent dimensions on blend morphology, charge transport, carrier dynamics, and PSC metrics. Varying substituent dimensions has a pronounced effect on the blend morphology with a direct link between domain purity, to some extent domain dimensions, and charge generation and collection. The polymer with the smallest alkyl substituent yields the highest PSC power conversion efficiency (PCE, 11%), reflecting relatively small, high-purity domains, and possibly benefiting from “matched” donor polymer - small molecule acceptor orientations. The distinctive morphologies arising from the substituents are investigated using molecular dynamics (MD) computation which reveals that substituent dimensions dictate a well-defined set of polymer conformations, in turn driving chain aggregation, and ultimately, the various film morphologies and mixing with acceptor small molecules. Finally, a straightforward energetic parameter explains the experimental polymer domain morphological trends, hence PCE, and suggests strategies for substituent selection to optimize PSC materials morphologies.
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- Northwestern Univ., Evanston, IL (United States)
- National Inst. of Standards and Technology (NIST), Gaithersburg, MD (United States)
- Argonne National Lab. (ANL), Argonne, IL (United States)
- Linköping Univ., Norrköping (Sweden)
- Northwestern Univ., Evanston, IL (United States); Flexterra Corporation, Skokie, IL (United States)
- Publication Date:
- Research Org.:
- Energy Frontier Research Centers (EFRC) (United States). Center for Light Energy Activated Redox Processes (LEAP); Argonne National Lab. (ANL), Argonne, IL (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1560046
- Grant/Contract Number:
- AC02-06CH11357; AC02-05CH11231; SC0001059
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Journal of the American Chemical Society
- Additional Journal Information:
- Journal Volume: 141; Journal Issue: 34; 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; domain purity; donor-acceptor heterojunction morphology; high efficiency; molecular dynamics computation; polymer aggregation; post-fullerene solar cells
Citation Formats
Wang, Gang, Swick, Steven M., Matta, Micaela, Mukherjee, Subhrangsu, Strzalka, Joseph W., Logsdon, Jenna Leigh, Fabiano, Simone, Huang, Wei, Aldrich, Thomas J., Yang, Tony, Timalsina, Amod, Powers-Riggs, Natalia, Alzola, Joaquin M., Young, Ryan M., DeLongchamp, Dean M., Wasielewski, Michael R., Kohlstedt, Kevin L., Schatz, George C., Melkonyan, Ferdinand S., Facchetti, Antonio, and Marks, Tobin J. Photovoltaic Blend Microstructure for High Efficiency Post-Fullerene Solar Cells. To Tilt or Not To Tilt?. United States: N. p., 2019.
Web. doi:10.1021/jacs.9b03770.
Wang, Gang, Swick, Steven M., Matta, Micaela, Mukherjee, Subhrangsu, Strzalka, Joseph W., Logsdon, Jenna Leigh, Fabiano, Simone, Huang, Wei, Aldrich, Thomas J., Yang, Tony, Timalsina, Amod, Powers-Riggs, Natalia, Alzola, Joaquin M., Young, Ryan M., DeLongchamp, Dean M., Wasielewski, Michael R., Kohlstedt, Kevin L., Schatz, George C., Melkonyan, Ferdinand S., Facchetti, Antonio, & Marks, Tobin J. Photovoltaic Blend Microstructure for High Efficiency Post-Fullerene Solar Cells. To Tilt or Not To Tilt?. United States. https://doi.org/10.1021/jacs.9b03770
Wang, Gang, Swick, Steven M., Matta, Micaela, Mukherjee, Subhrangsu, Strzalka, Joseph W., Logsdon, Jenna Leigh, Fabiano, Simone, Huang, Wei, Aldrich, Thomas J., Yang, Tony, Timalsina, Amod, Powers-Riggs, Natalia, Alzola, Joaquin M., Young, Ryan M., DeLongchamp, Dean M., Wasielewski, Michael R., Kohlstedt, Kevin L., Schatz, George C., Melkonyan, Ferdinand S., Facchetti, Antonio, and Marks, Tobin J. Mon .
"Photovoltaic Blend Microstructure for High Efficiency Post-Fullerene Solar Cells. To Tilt or Not To Tilt?". United States. https://doi.org/10.1021/jacs.9b03770. https://www.osti.gov/servlets/purl/1560046.
@article{osti_1560046,
title = {Photovoltaic Blend Microstructure for High Efficiency Post-Fullerene Solar Cells. To Tilt or Not To Tilt?},
author = {Wang, Gang and Swick, Steven M. and Matta, Micaela and Mukherjee, Subhrangsu and Strzalka, Joseph W. and Logsdon, Jenna Leigh and Fabiano, Simone and Huang, Wei and Aldrich, Thomas J. and Yang, Tony and Timalsina, Amod and Powers-Riggs, Natalia and Alzola, Joaquin M. and Young, Ryan M. and DeLongchamp, Dean M. and Wasielewski, Michael R. and Kohlstedt, Kevin L. and Schatz, George C. and Melkonyan, Ferdinand S. and Facchetti, Antonio and Marks, Tobin J.},
abstractNote = {Achieving efficient polymer solar cells (PSCs) requires a structurally optimal donor-acceptor heterojunction morphology. In this paper, we report the combined experimental and theoretical characterization of a benzodithiophene benzothiadiazole donor polymer series (PBTZF4-R; R = alkyl substituent) blended with the non-fullerene acceptor ITIC-Th, and analyse the effects of substituent dimensions on blend morphology, charge transport, carrier dynamics, and PSC metrics. Varying substituent dimensions has a pronounced effect on the blend morphology with a direct link between domain purity, to some extent domain dimensions, and charge generation and collection. The polymer with the smallest alkyl substituent yields the highest PSC power conversion efficiency (PCE, 11%), reflecting relatively small, high-purity domains, and possibly benefiting from “matched” donor polymer - small molecule acceptor orientations. The distinctive morphologies arising from the substituents are investigated using molecular dynamics (MD) computation which reveals that substituent dimensions dictate a well-defined set of polymer conformations, in turn driving chain aggregation, and ultimately, the various film morphologies and mixing with acceptor small molecules. Finally, a straightforward energetic parameter explains the experimental polymer domain morphological trends, hence PCE, and suggests strategies for substituent selection to optimize PSC materials morphologies.},
doi = {10.1021/jacs.9b03770},
journal = {Journal of the American Chemical Society},
number = 34,
volume = 141,
place = {United States},
year = {2019},
month = {8}
}
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Cited by: 32 works
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Figures / Tables:
Figure 1: Donor and acceptor materials and their physicochemical properties. a) P‐EH, P‐BO, P‐HD, P‐OD and ITIC‐Th molecular structures; b) Film optical absorption spectra of P‐EH, P‐BO, P‐HD, P‐OD, and ITIC‐Th. Neat films of the polymer were spin‐coated from PhCl solutions (5 mg mL‐1) and neat ITIC‐Th films were spin‐coatedmore »
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Works referenced in this record:
Recent Advances in Bulk Heterojunction Polymer Solar Cells
journal, August 2015
- Lu, Luyao; Zheng, Tianyue; Wu, Qinghe
- Chemical Reviews, Vol. 115, Issue 23
Organic solar cells based on non-fullerene acceptors
journal, January 2018
- Hou, Jianhui; Inganäs, Olle; Friend, Richard H.
- Nature Materials, Vol. 17, Issue 2
Non-fullerene acceptors for organic solar cells
journal, February 2018
- Yan, Cenqi; Barlow, Stephen; Wang, Zhaohui
- Nature Reviews Materials, Vol. 3, Issue 3
Bulk Heterojunction Solar Cells: Morphology and Performance Relationships
journal, May 2014
- Huang, Ye; Kramer, Edward J.; Heeger, Alan J.
- Chemical Reviews, Vol. 114, Issue 14
Additives for morphology control in high-efficiency organic solar cells
journal, September 2013
- Liao, Hsueh-Chung; Ho, Chun-Chih; Chang, Chun-Yu
- Materials Today, Vol. 16, Issue 9
Universal Correlation between Fibril Width and Quantum Efficiency in Diketopyrrolopyrrole-Based Polymer Solar Cells
journal, December 2013
- Li, Weiwei; Hendriks, Koen H.; Furlan, Alice
- Journal of the American Chemical Society, Vol. 135, Issue 50
Effect of the Fibrillar Microstructure on the Efficiency of High Molecular Weight Diketopyrrolopyrrole-Based Polymer Solar Cells
journal, November 2013
- Li, Weiwei; Hendriks, Koen H.; Furlan, Alice
- Advanced Materials, Vol. 26, Issue 10
Importance of Domain Purity and Molecular Packing in Efficient Solution-Processed Small-Molecule Solar Cells
journal, December 2014
- Mukherjee, Subhrangsu; Proctor, Christopher M.; Tumbleston, John R.
- Advanced Materials, Vol. 27, Issue 6
Isolating and quantifying the impact of domain purity on the performance of bulk heterojunction solar cells
journal, January 2017
- Huang, Wenchao; Gann, Eliot; Chandrasekaran, Naresh
- Energy & Environmental Science, Vol. 10, Issue 8
The effect of side-chain substitution and hot processing on diketopyrrolopyrrole-based polymers for organic solar cells
journal, January 2017
- Heintges, Gaël H. L.; Leenaers, Pieter J.; Janssen, René A. J.
- Journal of Materials Chemistry A, Vol. 5, Issue 26
Closely packed, low reorganization energy π-extended postfullerene acceptors for efficient polymer solar cells
journal, August 2018
- Swick, Steven M.; Zhu, Weigang; Matta, Micaela
- Proceedings of the National Academy of Sciences, Vol. 115, Issue 36
Enhancing Indacenodithiophene Acceptor Crystallinity via Substituent Manipulation Increases Organic Solar Cell Efficiency
journal, November 2017
- Aldrich, Thomas J.; Swick, Steven M.; Melkonyan, Ferdinand S.
- Chemistry of Materials, Vol. 29, Issue 24
Quantitative relations between interaction parameter, miscibility and function in organic solar cells
journal, February 2018
- Ye, Long; Hu, Huawei; Ghasemi, Masoud
- Nature Materials, Vol. 17, Issue 3
Solvent Additives: Key Morphology-Directing Agents for Solution-Processed Organic Solar Cells
journal, June 2018
- McDowell, Caitlin; Abdelsamie, Maged; Toney, Michael F.
- Advanced Materials, Vol. 30, Issue 33
Fine-tuning of the chemical structure of photoactive materials for highly efficient organic photovoltaics
journal, October 2018
- Fan, Baobing; Du, Xiaoyan; Liu, Feng
- Nature Energy, Vol. 3, Issue 12
Side-chain engineering of high-efficiency conjugated polymer photovoltaic materials
journal, November 2014
- Zhang, Zhi-Guo; Li, Yongfang
- Science China Chemistry, Vol. 58, Issue 2
Alkyl Chain Engineering of Solution-Processable Star-Shaped Molecules for High-Performance Organic Solar Cells
journal, October 2013
- Min, Jie; Luponosov, Yuriy N.; Gerl, Andreas
- Advanced Energy Materials, Vol. 4, Issue 5
Side-Chain Engineering of Isoindigo-Containing Conjugated Polymers Using Polystyrene for High-Performance Bulk Heterojunction Solar Cells
journal, December 2013
- Fang, Lei; Zhou, Yan; Yao, Yu-Xing
- Chemistry of Materials, Vol. 25, Issue 24
Side Chain Engineering in Solution-Processable Conjugated Polymers
journal, September 2013
- Mei, Jianguo; Bao, Zhenan
- Chemistry of Materials, Vol. 26, Issue 1
Effect of Side-Chain Engineering of Bithienylbenzodithiophene- alt -fluorobenzotriazole-Based Copolymers on the Thermal Stability and Photovoltaic Performance of Polymer Solar Cells
journal, July 2018
- Huang, He; Bin, Haijun; Peng, Zhengxing
- Macromolecules, Vol. 51, Issue 15
Subtle Side-Chain Engineering of Random Terpolymers for High-Performance Organic Solar Cells
journal, May 2018
- Huo, Lijun; Xue, Xiaonan; Liu, Tao
- Chemistry of Materials, Vol. 30, Issue 10
Aggregation and Solubility of a Model Conjugated Donor–Acceptor Polymer
journal, July 2018
- Reid, Daniel R.; Jackson, Nicholas E.; Bourque, Alexander J.
- The Journal of Physical Chemistry Letters, Vol. 9, Issue 16
The effect of alkylthio side chains in oligothiophene-based donor materials for organic solar cells
journal, January 2018
- Zou, Yan; Wu, Yue; Yang, Hang
- Molecular Systems Design & Engineering, Vol. 3, Issue 1
Rational design of conjugated side chains for high-performance all-polymer solar cells
journal, January 2018
- Huang, Wei; Li, Meilin; Lin, Fengyuan
- Molecular Systems Design & Engineering, Vol. 3, Issue 1
New donor polymer with tetrafluorinated blocks for enhanced performance in perylenediimide-based solar cells
journal, January 2017
- Timalsina, Amod; Hartnett, Patrick E.; Melkonyan, Ferdinand S.
- Journal of Materials Chemistry A, Vol. 5, Issue 11
All-Polymer Solar Cell Performance Optimized via Systematic Molecular Weight Tuning of Both Donor and Acceptor Polymers
journal, January 2016
- Zhou, Nanjia; Dudnik, Alexander S.; Li, Ting I. N. G.
- Journal of the American Chemical Society, Vol. 138, Issue 4
Effect of Alkyl Side Chains of Conjugated Polymer Donors on the Device Performance of Non-Fullerene Solar Cells
journal, August 2016
- Xia, Dongdong; Wu, Yang; Wang, Qiang
- Macromolecules, Vol. 49, Issue 17
Charge-Carrier Mobility Requirements for Bulk Heterojunction Solar Cells with High Fill Factor and External Quantum Efficiency >90%
journal, June 2015
- Bartelt, Jonathan A.; Lam, David; Burke, Timothy M.
- Advanced Energy Materials, Vol. 5, Issue 15
Device model for the operation of polymer/fullerene bulk heterojunction solar cells
journal, August 2005
- Koster, L. J. A.; Smits, E. C. P.; Mihailetchi, V. D.
- Physical Review B, Vol. 72, Issue 8
Recombination via tail states in polythiophene:fullerene solar cells
journal, March 2011
- Kirchartz, Thomas; Pieters, Bart E.; Kirkpatrick, James
- Physical Review B, Vol. 83, Issue 11
Improved Scaling of Molecular Network Calculations: The Emergence of Molecular Domains
journal, January 2017
- Gagorik, Adam G.; Savoie, Brett; Jackson, Nick
- The Journal of Physical Chemistry Letters, Vol. 8, Issue 2
Side Chain Engineering on Medium Bandgap Copolymers to Suppress Triplet Formation for High-Efficiency Polymer Solar Cells
journal, August 2017
- Xue, Lingwei; Yang, Yankang; Xu, Jianqiu
- Advanced Materials, Vol. 29, Issue 40
Highly efficient charge-carrier generation and collection in polymer/polymer blend solar cells with a power conversion efficiency of 5.7%
journal, January 2014
- Mori, Daisuke; Benten, Hiroaki; Okada, Izumi
- Energy & Environmental Science, Vol. 7, Issue 9
Hole-Transfer Dependence on Blend Morphology and Energy Level Alignment in Polymer: ITIC Photovoltaic Materials
journal, December 2017
- Eastham, Nicholas D.; Logsdon, Jenna L.; Manley, Eric F.
- Advanced Materials, Vol. 30, Issue 3
Molecular Characterization of Organic Electronic Films
journal, August 2010
- DeLongchamp, Dean M.; Kline, R. Joseph; Fischer, Daniel A.
- Advanced Materials, Vol. 23, Issue 3
Modulating the Molecular Packing and Nanophase Blending via a Random Terpolymerization Strategy toward 11% Efficiency Nonfullerene Polymer Solar Cells
journal, July 2017
- Chen, Shanshan; Cho, Hye Jin; Lee, Jungho
- Advanced Energy Materials, Vol. 7, Issue 21
Single-Junction Binary-Blend Nonfullerene Polymer Solar Cells with 12.1% Efficiency
journal, March 2017
- Zhao, Fuwen; Dai, Shuixing; Wu, Yang
- Advanced Materials, Vol. 29, Issue 18
Controlling Molecular Orientation of Naphthalenediimide-Based Polymer Acceptors for High Performance All-Polymer Solar Cells
journal, June 2016
- Jung, Jihye; Lee, Wonho; Lee, Changyeon
- Advanced Energy Materials, Vol. 6, Issue 15
High-Performance Electron Acceptor with Thienyl Side Chains for Organic Photovoltaics
journal, March 2016
- Lin, Yuze; Zhao, Fuwen; He, Qiao
- Journal of the American Chemical Society, Vol. 138, Issue 14
Efficient inverted polymer solar cells employing favourable molecular orientation
journal, May 2015
- Vohra, Varun; Kawashima, Kazuaki; Kakara, Takeshi
- Nature Photonics, Vol. 9, Issue 6
Correlated Donor/Acceptor Crystal Orientation Controls Photocurrent Generation in All-Polymer Solar Cells
journal, April 2014
- Schubert, Marcel; Collins, Brian A.; Mangold, Hannah
- Advanced Functional Materials, Vol. 24, Issue 26
A general relationship between disorder, aggregation and charge transport in conjugated polymers
journal, August 2013
- Noriega, Rodrigo; Rivnay, Jonathan; Vandewal, Koen
- Nature Materials, Vol. 12, Issue 11
Absolute Measurement of Domain Composition and Nanoscale Size Distribution Explains Performance in PTB7:PC 71 BM Solar Cells
journal, October 2012
- Collins, Brian A.; Li, Zhe; Tumbleston, John R.
- Advanced Energy Materials, Vol. 3, Issue 1
Conformational Order in Aggregates of Conjugated Polymers
journal, May 2015
- Jackson, Nicholas E.; Kohlstedt, Kevin L.; Savoie, Brett M.
- Journal of the American Chemical Society, Vol. 137, Issue 19
Controlling Chain Conformation in Conjugated Polymers Using Defect Inclusion Strategies
journal, July 2011
- Bounos, Giannis; Ghosh, Subhadip; Lee, Albert K.
- Journal of the American Chemical Society, Vol. 133, Issue 26
Impact of the Nature of the Side-Chains on the Polymer-Fullerene Packing in the Mixed Regions of Bulk Heterojunction Solar Cells
journal, June 2016
- Wang, Tonghui; Ravva, Mahesh Kumar; Brédas, Jean-Luc
- Advanced Functional Materials, Vol. 26, Issue 32
Collapse of stiff conjugated polymers with chemical defects into ordered, cylindrical conformations
journal, June 2000
- Hu, Dehong; Yu, Ji; Wong, Kim
- Nature, Vol. 405, Issue 6790
Systematic Coarse-Graining of the Dynamics of Self-Attractive Semiflexible Polymers
journal, February 2014
- Kong, Miqiu; Saha Dalal, Indranil; Li, Guangxian
- Macromolecules, Vol. 47, Issue 4
Polymer semiconductor crystals
journal, May 2010
- Lim, Jung Ah; Liu, Feng; Ferdous, Sunzida
- Materials Today, Vol. 13, Issue 5
Enhanced Solid-State Order and Field-Effect Hole Mobility through Control of Nanoscale Polymer Aggregation
journal, December 2013
- Chen, Mark S.; Lee, Olivia P.; Niskala, Jeremy R.
- Journal of the American Chemical Society, Vol. 135, Issue 51
Simulation Study of the Effect of the Side-Chain Structure on the Initial Nucleation Process of Polythiophene Derivatives
journal, January 2017
- Ito, Taiki; Shimomura, Takeshi; Miura, Toshiaki
- The Journal of Physical Chemistry B, Vol. 121, Issue 5
Linear Side Chains in Benzo[1,2- b :4,5- b ′]dithiophene–Thieno[3,4- c ]pyrrole-4,6-dione Polymers Direct Self-Assembly and Solar Cell Performance
journal, March 2013
- Cabanetos, Clément; El Labban, Abdulrahman; Bartelt, Jonathan A.
- Journal of the American Chemical Society, Vol. 135, Issue 12
3,4-Disubstituted Polyalkylthiophenes for High-Performance Thin-Film Transistors and Photovoltaics
journal, October 2011
- Ko, Sangwon; Verploegen, Eric; Hong, Sanghyun
- Journal of the American Chemical Society, Vol. 133, Issue 42
Predicting Flory-Huggins from Simulations
journal, July 2017
- Zhang, Wenlin; Gomez, Enrique D.; Milner, Scott T.
- Physical Review Letters, Vol. 119, Issue 1
Chain conformations and phase behavior of conjugated polymers
journal, January 2017
- Kuei, Brooke; Gomez, Enrique D.
- Soft Matter, Vol. 13, Issue 1
Measuring Temperature-Dependent Miscibility for Polymer Solar Cell Blends: An Easily Accessible Optical Method Reveals Complex Behavior
journal, May 2018
- Peng, Zhengxing; Jiao, Xuechen; Ye, Long
- Chemistry of Materials, Vol. 30, Issue 12
Intrinsic non-radiative voltage losses in fullerene-based organic solar cells
journal, April 2017
- Benduhn, Johannes; Tvingstedt, Kristofer; Piersimoni, Fortunato
- Nature Energy, Vol. 2, Issue 6
Bulk Heterojunction Morphologies with Atomistic Resolution from Coarse-Grain Solvent Evaporation Simulations
journal, March 2017
- Alessandri, Riccardo; Uusitalo, Jaakko J.; de Vries, Alex H.
- Journal of the American Chemical Society, Vol. 139, Issue 10
Works referencing / citing this record:
High-efficiency ternary nonfullerene polymer solar cells with increased phase purity and reduced nonradiative energy loss
journal, January 2020
- Zhang, Cai'e; Jiang, Pengcheng; Zhou, Xiaobo
- Journal of Materials Chemistry A, Vol. 8, Issue 4
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