Search Menu
DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information
Search Scholarly Publications

Title: Understanding Interfacial Alignment in Solution Coated Conjugated Polymer Thin Films

Abstract

Domain alignment in conjugated polymer thin films can significantly enhance charge carrier mobility. However, the alignment mechanism during meniscus-guided solution coating remains unclear. Furthermore, interfacial alignment has been rarely studied despite its direct relevance and critical importance to charge transport. In this study, we uncover a significantly higher degree of alignment at the top interface of solution coated thin films, using a donor–acceptor conjugated polymer, poly(diketopyrrolopyrrole-co-thiopheneco- thieno[3,2-b]thiophene-co-thiophene) (DPP2T-TT), as the model system. At the molecular level, we observe in-plane π–π stacking anisotropy of up to 4.8 near the top interface with the polymer backbone aligned parallel to the coating direction. The bulk of the film is only weakly aligned with the backbone oriented transverse to coating. At the mesoscale, we observe a well-defined fibril-like morphology at the top interface with the fibril long axis pointing toward the coating direction. Significantly smaller fibrils with poor orientational order are found on the bottom interface, weakly aligned orthogonal to the fibrils on the top interface. The high degree of alignment at the top interface leads to a charge transport anisotropy of up to 5.4 compared to an anisotropy close to 1 on the bottom interface. We attribute the formation of distinct interfacial morphologymore » to the skin-layer formation associated with high Peclet number, which promotes crystallization on the top interface while suppressing it in the bulk. As a result, we further infer that the interfacial fibril alignment is driven by the extensional flow on the top interface arisen from increasing solvent evaporation rate closer to the meniscus front.« less

Authors:
 [1];  [2];  [3];  [1];  [1];  [4];  [3]; ORCiD logo [2]; ORCiD logo [1]
+ Show Author Affiliations
  1. Univ. of Illinois Urbana-Champaign, Urbana, IL (United States)
  2. Purdue Univ., West Lafayette, IN (United States)
  3. Univ. of Washington, Seattle, WA (United States)
  4. Argonne National Lab. (ANL), Argonne, IL (United States)
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1376901
Grant/Contract Number:  
AC02-06CH11357
Resource Type:
Accepted Manuscript
Journal Name:
ACS Applied Materials and Interfaces
Additional Journal Information:
Journal Volume: 9; Journal Issue: 33; Journal ID: ISSN 1944-8244
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; morphology; polymer crystallization; alignment; charge transport; conjugated polymer; interfacial; solution printing

Citation Formats

Qu, Ge, Zhao, Xikang, Newbloom, Gregory M., Zhang, Fengjiao, Mohammadi, Erfan, Strzalka, Joseph W., Pozzo, Lilo D., Mei, Jianguo, and Diao, Ying. Understanding Interfacial Alignment in Solution Coated Conjugated Polymer Thin Films. United States: N. p., 2017. Web. doi:10.1021/acsami.7b08133.
Copy to clipboard
Qu, Ge, Zhao, Xikang, Newbloom, Gregory M., Zhang, Fengjiao, Mohammadi, Erfan, Strzalka, Joseph W., Pozzo, Lilo D., Mei, Jianguo, & Diao, Ying. Understanding Interfacial Alignment in Solution Coated Conjugated Polymer Thin Films. United States. https://doi.org/10.1021/acsami.7b08133
Copy to clipboard
Qu, Ge, Zhao, Xikang, Newbloom, Gregory M., Zhang, Fengjiao, Mohammadi, Erfan, Strzalka, Joseph W., Pozzo, Lilo D., Mei, Jianguo, and Diao, Ying. Tue . "Understanding Interfacial Alignment in Solution Coated Conjugated Polymer Thin Films". United States. https://doi.org/10.1021/acsami.7b08133. https://www.osti.gov/servlets/purl/1376901.
Copy to clipboard
@article{osti_1376901,
title = {Understanding Interfacial Alignment in Solution Coated Conjugated Polymer Thin Films},
author = {Qu, Ge and Zhao, Xikang and Newbloom, Gregory M. and Zhang, Fengjiao and Mohammadi, Erfan and Strzalka, Joseph W. and Pozzo, Lilo D. and Mei, Jianguo and Diao, Ying},
abstractNote = {Domain alignment in conjugated polymer thin films can significantly enhance charge carrier mobility. However, the alignment mechanism during meniscus-guided solution coating remains unclear. Furthermore, interfacial alignment has been rarely studied despite its direct relevance and critical importance to charge transport. In this study, we uncover a significantly higher degree of alignment at the top interface of solution coated thin films, using a donor–acceptor conjugated polymer, poly(diketopyrrolopyrrole-co-thiopheneco- thieno[3,2-b]thiophene-co-thiophene) (DPP2T-TT), as the model system. At the molecular level, we observe in-plane π–π stacking anisotropy of up to 4.8 near the top interface with the polymer backbone aligned parallel to the coating direction. The bulk of the film is only weakly aligned with the backbone oriented transverse to coating. At the mesoscale, we observe a well-defined fibril-like morphology at the top interface with the fibril long axis pointing toward the coating direction. Significantly smaller fibrils with poor orientational order are found on the bottom interface, weakly aligned orthogonal to the fibrils on the top interface. The high degree of alignment at the top interface leads to a charge transport anisotropy of up to 5.4 compared to an anisotropy close to 1 on the bottom interface. We attribute the formation of distinct interfacial morphology to the skin-layer formation associated with high Peclet number, which promotes crystallization on the top interface while suppressing it in the bulk. As a result, we further infer that the interfacial fibril alignment is driven by the extensional flow on the top interface arisen from increasing solvent evaporation rate closer to the meniscus front.},
doi = {10.1021/acsami.7b08133},
journal = {ACS Applied Materials and Interfaces},
number = 33,
volume = 9,
place = {United States},
year = {Tue Aug 01 00:00:00 EDT 2017},
month = {Tue Aug 01 00:00:00 EDT 2017}
}
Copy to clipboard
Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record
https://doi.org/10.1021/acsami.7b08133
Copyright Statement
Other availability
Search WorldCat Search WorldCat to find libraries that may hold this journal
Citation Metrics:
Cited by: 38 works
Citation information provided by
Web of Science
Save / Share:
Export Metadata
Save to My Library
You must Sign In or Create an Account in order to save documents to your library.

Works referenced in this record:

Engineering semiconducting polymers for efficient charge transport
journal, June 2015

  • Himmelberger, Scott; Salleo, Alberto
  • MRS Communications, Vol. 5, Issue 3
  • DOI: 10.1557/mrc.2015.44

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
  • DOI: 10.1038/nmat3722

Approaching disorder-free transport in high-mobility conjugated polymers
journal, November 2014

  • Venkateshvaran, Deepak; Nikolka, Mark; Sadhanala, Aditya
  • Nature, Vol. 515, Issue 7527
  • DOI: 10.1038/nature13854

Molecular origin of high field-effect mobility in an indacenodithiophene–benzothiadiazole copolymer
journal, July 2013

  • Zhang, Xinran; Bronstein, Hugo; Kronemeijer, Auke J.
  • Nature Communications, Vol. 4, Issue 1
  • DOI: 10.1038/ncomms3238

Temperature-Resolved Local and Macroscopic Charge Carrier Transport in Thin P3HT Layers
journal, June 2010

  • Pingel, Patrick; Zen, Achmad; Abellón, Ruben D.
  • Advanced Functional Materials, Vol. 20, Issue 14
  • DOI: 10.1002/adfm.200902273

The Importance of Bridging Points for Charge Transport in Webs of Conjugated Polymer Nanofibers
journal, January 2012

  • Bolsée, Jean-Christophe; Oosterbaan, Wibren D.; Lutsen, Laurence
  • Advanced Functional Materials, Vol. 23, Issue 7
  • DOI: 10.1002/adfm.201102078

Chain conformations dictate multiscale charge transport phenomena in disordered semiconducting polymers
journal, September 2013

  • Noriega, R.; Salleo, A.; Spakowitz, A. J.
  • Proceedings of the National Academy of Sciences, Vol. 110, Issue 41
  • DOI: 10.1073/pnas.1307158110

Charge-Transport Anisotropy Due to Grain Boundaries in Directionally Crystallized Thin Films of Regioregular Poly(3-hexylthiophene)
journal, April 2009

  • Jimison, Leslie H.; Toney, Michael F.; McCulloch, Iain
  • Advanced Materials, Vol. 21, Issue 16
  • DOI: 10.1002/adma.200802722

Large modulation of carrier transport by grain-boundary molecular packing and microstructure in organic thin films
journal, November 2009

  • Rivnay, Jonathan; Jimison, Leslie H.; Northrup, John E.
  • Nature Materials, Vol. 8, Issue 12, p. 952-958
  • DOI: 10.1038/nmat2570

High-Mobility Field-Effect Transistors Fabricated with Macroscopic Aligned Semiconducting Polymers
journal, February 2014

A molecular design principle of lyotropic liquid-crystalline conjugated polymers with directed alignment capability for plastic electronics
journal, March 2013

  • Kim, Bong-Gi; Jeong, Eun Jeong; Chung, Jong Won
  • Nature Materials, Vol. 12, Issue 7
  • DOI: 10.1038/nmat3595

Highly Oriented Polymer Semiconductor Films Compressed at the Surface of Ionic Liquids for High-Performance Polymeric Organic Field-Effect Transistors
journal, August 2014

  • Soeda, Junshi; Matsui, Hiroyuki; Okamoto, Toshihiro
  • Advanced Materials, Vol. 26, Issue 37
  • DOI: 10.1002/adma.201401495

Macroscopic and high-throughput printing of aligned nanostructured polymer semiconductors for MHz large-area electronics
journal, September 2015

  • Bucella, Sadir G.; Luzio, Alessandro; Gann, Eliot
  • Nature Communications, Vol. 6, Issue 1
  • DOI: 10.1038/ncomms9394

Charge-Transport Anisotropy in a Uniaxially Aligned Diketopyrrolopyrrole-Based Copolymer
journal, October 2015

Large Scale Alignment and Charge Transport Anisotropy of pBTTT Films Oriented by High Temperature Rubbing
journal, May 2013

  • Biniek, Laure; Leclerc, Nicolas; Heiser, Thomas
  • Macromolecules, Vol. 46, Issue 10
  • DOI: 10.1021/ma400516d

A nanogroove-guided slot-die coating technique for highly ordered polymer films and high-mobility transistors
journal, January 2016

  • Kyaw, Aung Ko Ko; Lay, Lim Siew; Peng, Goh Wei
  • Chemical Communications, Vol. 52, Issue 2
  • DOI: 10.1039/C5CC05247E

High Mobility Field Effect Transistors Based on Macroscopically Oriented Regioregular Copolymers
journal, February 2012

  • Tseng, Hsin-Rong; Ying, Lei; Hsu, Ben B. Y.
  • Nano Letters, Vol. 12, Issue 12
  • DOI: 10.1021/nl303612z

Controlling the Orientation of Terraced Nanoscale “Ribbons” of a Poly(thiophene) Semiconductor
journal, March 2009

  • DeLongchamp, Dean M.; Kline, R. Joseph; Jung, Youngsuk
  • ACS Nano, Vol. 3, Issue 4
  • DOI: 10.1021/nn800574f

Enhanced Polymer Thin Film Transistor Performance by Carefully Controlling the Solution Self-Assembly and Film Alignment with Slot Die Coating
journal, June 2015

  • Chang, Jingjing; Lin, Zhenhua; Li, Jun
  • Advanced Electronic Materials, Vol. 1, Issue 7
  • DOI: 10.1002/aelm.201500036

Highly oriented crystals at the buried interface in polythiophene thin-film transistors
journal, February 2006

  • Joseph Kline, R.; McGehee, Michael D.; Toney, Michael F.
  • Nature Materials, Vol. 5, Issue 3
  • DOI: 10.1038/nmat1590

Observation of a Distinct Surface Molecular Orientation in Films of a High Mobility Conjugated Polymer
journal, January 2013

  • Schuettfort, Torben; Thomsen, Lars; McNeill, Christopher R.
  • Journal of the American Chemical Society, Vol. 135, Issue 3
  • DOI: 10.1021/ja310240q

Effects of Confinement on Microstructure and Charge Transport in High Performance Semicrystalline Polymer Semiconductors
journal, November 2012

  • Himmelberger, Scott; Dacuña, Javier; Rivnay, Jonathan
  • Advanced Functional Materials, Vol. 23, Issue 16
  • DOI: 10.1002/adfm.201202408

Microstructure of Polycrystalline PBTTT Films: Domain Mapping and Structure Formation
journal, January 2012

  • Schuettfort, Torben; Watts, Benjamin; Thomsen, Lars
  • ACS Nano, Vol. 6, Issue 2
  • DOI: 10.1021/nn2051295

NEXAFS Spectroscopy Reveals the Molecular Orientation in Blade-Coated Pyridal[2,1,3]thiadiazole-Containing Conjugated Polymer Thin Films
journal, September 2015

Tuning charge transport in solution-sheared organic semiconductors using lattice strain
journal, December 2011

  • Giri, Gaurav; Verploegen, Eric; Mannsfeld, Stefan C. B.
  • Nature, Vol. 480, Issue 7378, p. 504-508
  • DOI: 10.1038/nature10683

High‐Performance Organic Thin‐Film Transistors through Solution‐Sheared Deposition of Small‐Molecule Organic Semiconductors
journal, July 2008

  • Becerril, Héctor A.; Roberts, Mark E.; Liu, Zihong
  • Advanced Materials, Vol. 20, Issue 13, p. 2588-2594
  • DOI: 10.1002/adma.200703120

Capillary flow as the cause of ring stains from dried liquid drops
journal, October 1997

  • Deegan, Robert D.; Bakajin, Olgica; Dupont, Todd F.
  • Nature, Vol. 389, Issue 6653, p. 827-829
  • DOI: 10.1038/39827

Charge separation in localized and delocalized electronic states in polymeric semiconductors
journal, April 1998

  • Köhler, A.; dos Santos, D. A.; Beljonne, D.
  • Nature, Vol. 392, Issue 6679
  • DOI: 10.1038/31901

Optical constants of highly stretch-oriented poly( p -phenylene-vinylene): A joint experimental and theoretical study
journal, October 2000

Exploring the origin of high optical absorption in conjugated polymers
journal, May 2016

  • Vezie, Michelle S.; Few, Sheridan; Meager, Iain
  • Nature Materials, Vol. 15, Issue 7
  • DOI: 10.1038/nmat4645

Morphological Origin of Charge Transport Anisotropy in Aligned Polythiophene Thin Films
journal, February 2014

  • O'Connor, Brendan T.; Reid, Obadiah G.; Zhang, Xinran
  • Advanced Functional Materials, Vol. 24, Issue 22
  • DOI: 10.1002/adfm.201303351

Anisotropic Structure and Charge Transport in Highly Strain-Aligned Regioregular Poly(3-hexylthiophene)
journal, August 2011

  • O'Connor, Brendan; Kline, R. Joseph; Conrad, Brad R.
  • Advanced Functional Materials, Vol. 21, Issue 19
  • DOI: 10.1002/adfm.201100904

Quantitative Determination of Organic Semiconductor Microstructure from the Molecular to Device Scale
journal, June 2012

  • Rivnay, Jonathan; Mannsfeld, Stefan C. B.; Miller, Chad E.
  • Chemical Reviews, Vol. 112, Issue 10
  • DOI: 10.1021/cr3001109

Molecular Characterization of Organic Electronic Films
journal, August 2010

  • DeLongchamp, Dean M.; Kline, R. Joseph; Fischer, Daniel A.
  • Advanced Materials, Vol. 23, Issue 3
  • DOI: 10.1002/adma.201001760

Reversible Soft-Contact Lamination and Delamination for Non-Invasive Fabrication and Characterization of Bulk-Heterojunction and Bilayer Organic Solar Cells
journal, August 2010

  • Kim, Jong Bok; Lee, Stephanie; Toney, Michael F.
  • Chemistry of Materials, Vol. 22, Issue 17
  • DOI: 10.1021/cm101692a

Lamination Method for the Study of Interfaces in Polymeric Thin Film Transistors
journal, November 2004

  • Chabinyc, Michael L.; Salleo, Alberto; Wu, Yiliang
  • Journal of the American Chemical Society, Vol. 126, Issue 43
  • DOI: 10.1021/ja044884o

Microfluidic Crystal Engineering of π-Conjugated Polymers
journal, July 2015

Charge Transport in Organic Semiconductors
journal, April 2007

  • Coropceanu, Veaceslav; Cornil, Jérôme; da Silva Filho, Demetrio A.
  • Chemical Reviews, Vol. 107, Issue 4
  • DOI: 10.1021/cr050140x

Mobility overestimation due to gated contacts in organic field-effect transistors
journal, March 2016

  • Bittle, Emily G.; Basham, James I.; Jackson, Thomas N.
  • Nature Communications, Vol. 7, Issue 1
  • DOI: 10.1038/ncomms10908

On the Extraction of Charge Carrier Mobility in High-Mobility Organic Transistors
journal, November 2015

  • Uemura, Takafumi; Rolin, Cedric; Ke, Tung-Huei
  • Advanced Materials, Vol. 28, Issue 1
  • DOI: 10.1002/adma.201503133

Anisotropy of Charge Transport in a Uniaxially Aligned and Chain-Extended, High-Mobility, Conjugated Polymer Semiconductor
journal, January 2011

  • Lee, Mi Jung; Gupta, Dhritiman; Zhao, Ni
  • Advanced Functional Materials, Vol. 21, Issue 5
  • DOI: 10.1002/adfm.201001781

Control of mesoscale and nanoscale ordering of organic semiconductors at the gate dielectric/semiconductor interface for organic transistors
journal, January 2010

  • Lee, Wi Hyoung; Cho, Jeong Ho; Cho, Kilwon
  • Journal of Materials Chemistry, Vol. 20, Issue 13
  • DOI: 10.1039/b924415h

Drying of a Solution in a Meniscus: A Model Coupling the Liquid and the Gas Phases
journal, September 2010

Numerical simulation of complex fluid drying in a Hele-Shaw cell
journal, March 2013

  • Hsueh, Ching; Doumenc, Frédéric; Guerrier, Béatrice
  • The European Physical Journal Special Topics, Vol. 219, Issue 1
  • DOI: 10.1140/epjst/e2013-01780-8

Modeling Flow Coating of Colloidal Dispersions in the Evaporative Regime: Prediction of Deposit Thickness
journal, December 2016

Low-flow limit in slot coating of dilute solutions of high molecular weight polymer
journal, April 2004

  • Romero, O. J.; Suszynski, W. J.; Scriven, L. E.
  • Journal of Non-Newtonian Fluid Mechanics, Vol. 118, Issue 2-3
  • DOI: 10.1016/j.jnnfm.2004.03.004

Anisotropic particles align perpendicular to the flow direction in narrow microchannels
journal, April 2013

  • Trebbin, M.; Steinhauser, D.; Perlich, J.
  • Proceedings of the National Academy of Sciences, Vol. 110, Issue 17
  • DOI: 10.1073/pnas.1219340110

Rotation and alignment of rods in two-dimensional chaotic flow
journal, April 2011

  • Parsa, Shima; Guasto, Jeffrey S.; Kishore, Monica
  • Physics of Fluids, Vol. 23, Issue 4
  • DOI: 10.1063/1.3570526

Alignment of Dispersions of Plate-Like Colloidal Particles of Ni(OH) 2 Induced by Elongational Flow
journal, April 2011

  • Qazi, S. Junaid S.; Rennie, Adrian R.; Tucker, Ian
  • The Journal of Physical Chemistry B, Vol. 115, Issue 13
  • DOI: 10.1021/jp108805m

Transverse Alignment of Fibers in a Periodically Sheared Suspension: An Absorbing Phase Transition with a Slowly Varying Control Parameter
journal, December 2011

  • Franceschini, Alexandre; Filippidi, Emmanouela; Guazzelli, Elisabeth
  • Physical Review Letters, Vol. 107, Issue 25
  • DOI: 10.1103/PhysRevLett.107.250603

Shear Induced Alignment of Low Aspect Ratio Gold Nanorods in Newtonian Fluids
journal, September 2015

  • Xie, Donglin; Lista, Marco; Qiao, Greg G.
  • The Journal of Physical Chemistry Letters, Vol. 6, Issue 19
  • DOI: 10.1021/acs.jpclett.5b01641

Evaluating Rigid and Semiflexible Fiber Orientation Evolution Models in Simple Flows
journal, October 2016

  • Lambert, Gregory M.; Baird, Donald G.
  • Journal of Manufacturing Science and Engineering, Vol. 139, Issue 3
  • DOI: 10.1115/1.4034664

High-Performance Ambipolar Diketopyrrolopyrrole-Thieno[3,2- b ]thiophene Copolymer Field-Effect Transistors with Balanced Hole and Electron Mobilities
journal, October 2011

  • Chen, Zhuoying; Lee, Mi Jung; Shahid Ashraf, Raja
  • Advanced Materials, Vol. 24, Issue 5
  • DOI: 10.1002/adma.201102786

The 30 m Small-Angle Neutron Scattering Instruments at the National Institute of Standards and Technology
journal, June 1998

  • Glinka, C. J.; Barker, J. G.; Hammouda, B.
  • Journal of Applied Crystallography, Vol. 31, Issue 3, p. 430-445
  • DOI: 10.1107/S0021889897017020

Reduction and analysis of SANS and USANS data using IGOR Pro
journal, November 2006

The dedicated high-resolution grazing-incidence X-ray scattering beamline 8-ID-E at the Advanced Photon Source
journal, June 2012

  • Jiang, Zhang; Li, Xuefa; Strzalka, Joseph
  • Journal of Synchrotron Radiation, Vol. 19, Issue 4
  • DOI: 10.1107/S0909049512022017

Solution-processed, high-performance n-channel organic microwire transistors
journal, March 2009

  • Oh, J. H.; Lee, H. W.; Mannsfeld, S.
  • Proceedings of the National Academy of Sciences, Vol. 106, Issue 15
  • DOI: 10.1073/pnas.0811923106
    Sort by:
    [ × clear filter / sort ]

    Works referencing / citing this record:

    Increased charge carrier mobility and molecular packing of a solution sheared diketopyrrolopyrrole-based donor–acceptor copolymer by alkyl side chain modification
    journal, January 2019

    • Hambsch, Mike; Erdmann, Tim; Chew, Annabel R.
    • Journal of Materials Chemistry C, Vol. 7, Issue 12
    • DOI: 10.1039/c8tc06255b

    Enhancing Molecular Alignment and Charge Transport of Solution-Sheared Semiconducting Polymer Films by the Electrical-Blade Effect
    journal, May 2018

    • Molina-Lopez, Francisco; Wu, Hung-Chin; Wang, Ging-Ji Nathan
    • Advanced Electronic Materials, Vol. 4, Issue 7
    • DOI: 10.1002/aelm.201800110

    Design rules for dynamic-template-directed crystallization of conjugated polymers
    journal, January 2020

    • Mohammadi, Erfan; Qu, Ge; Kafle, Prapti
    • Molecular Systems Design & Engineering, Vol. 5, Issue 1
    • DOI: 10.1039/c9me00042a

    Quantitative Image Analysis of Fractal‐Like Thin Films of Organic Semiconductors
    journal, August 2019

    • Zhu, Weikun; Mohammadi, Erfan; Diao, Ying
    • Journal of Polymer Science Part B: Polymer Physics, Vol. 57, Issue 23
    • DOI: 10.1002/polb.24875
      Sort by:
      [ × clear filter / sort ]

      Similar Records in DOE PAGES and OSTI.GOV collections: