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Title: Crystallization Mechanism and Charge Carrier Transport in MAPLE-Deposited Conjugated Polymer Thin Films

Abstract

Although spin casting and chemical surface reactions are the most common methods used for fabricating functional polymer films onto substrates, they are limited with regard to producing films of certain morphological characteristics on different wetting and nonwetting substrates. The matrix-assisted pulsed laser evaporation (MAPLE) technique offers advantages with regard to producing films of different morphologies on different types of substrates. Here, we provide a quantitative characterization, using X-ray diffraction and optical methods, to elucidate the additive growth mechanism of MAPLE-deposited poly(3-hexylthiophene) (P3HT) films on substrates that have undergone different surface treatments, enabling them to possess different wettabilities. We show that MAPLE-deposited films are composed of crystalline phases, wherein the overall P3HT aggregate size and crystallite coherence length increase with deposition time. A complete pole figure constructed from X-ray diffraction measurements reveals that in these MAPLE-deposited films, there exist two distinct crystallite populations: (i) highly oriented crystals that grow from the flat dielectric substrate and (ii) misoriented crystals that preferentially grow on top of the existing polymer layers. The growth of the highly oriented crystals is highly sensitive to the chemistry of the substrate, whereas the effect of substrate chemistry on misoriented crystal growth is weaker. The use of a self-assembledmore » monolayer to treat the substrate greatly enhances the population and crystallite coherence length at the buried interfaces, particularly during the early stage of deposition. Furthermore, the evolution of the in-plane carrier mobilities during the course of deposition is consistent with the development of highly oriented crystals at the buried interface, suggesting that this interface plays a key role toward determining carrier transport in organic thin-film transistors.« less

Authors:
ORCiD logo [1];  [2];  [2];  [3];  [4]; ORCiD logo [5]
  1. Univ. of Michigan, Ann Arbor, MI (United States); The Univ. of Chicago, Chicago, IL (United States)
  2. Argonne National Lab. (ANL), Argonne, IL (United States)
  3. Univ. of Michigan, Ann Arbor, MI (United States)
  4. Univ. of Tennessee, Knoxville, TN (United States)
  5. Univ. of Michigan, Ann Arbor, MI (United States); National Renewable Energy Lab. (NREL), Golden, CO (United States)
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
National Science Foundation (NSF), Directorate for Mathematical and Physical Sciences Division of Materials Research (MPS-DMR); Vietnam Education Foundation; University of Michigan; USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1415483
Grant/Contract Number:  
AC02-06CH11357
Resource Type:
Accepted Manuscript
Journal Name:
ACS Applied Materials and Interfaces
Additional Journal Information:
Journal Volume: 9; Journal Issue: 51; Journal ID: ISSN 1944-8244
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; MAPLE; X-Ray diffraction; conjugated polymers; crystallization; structure-transport relationship

Citation Formats

Dong, Ban Xuan, Strzalka, Joseph, Jiang, Zhang, Li, Huanghe, Stein, Gila E., and Green, Peter F.. Crystallization Mechanism and Charge Carrier Transport in MAPLE-Deposited Conjugated Polymer Thin Films. United States: N. p., 2017. Web. https://doi.org/10.1021/acsami.7b13609.
Dong, Ban Xuan, Strzalka, Joseph, Jiang, Zhang, Li, Huanghe, Stein, Gila E., & Green, Peter F.. Crystallization Mechanism and Charge Carrier Transport in MAPLE-Deposited Conjugated Polymer Thin Films. United States. https://doi.org/10.1021/acsami.7b13609
Dong, Ban Xuan, Strzalka, Joseph, Jiang, Zhang, Li, Huanghe, Stein, Gila E., and Green, Peter F.. Thu . "Crystallization Mechanism and Charge Carrier Transport in MAPLE-Deposited Conjugated Polymer Thin Films". United States. https://doi.org/10.1021/acsami.7b13609. https://www.osti.gov/servlets/purl/1415483.
@article{osti_1415483,
title = {Crystallization Mechanism and Charge Carrier Transport in MAPLE-Deposited Conjugated Polymer Thin Films},
author = {Dong, Ban Xuan and Strzalka, Joseph and Jiang, Zhang and Li, Huanghe and Stein, Gila E. and Green, Peter F.},
abstractNote = {Although spin casting and chemical surface reactions are the most common methods used for fabricating functional polymer films onto substrates, they are limited with regard to producing films of certain morphological characteristics on different wetting and nonwetting substrates. The matrix-assisted pulsed laser evaporation (MAPLE) technique offers advantages with regard to producing films of different morphologies on different types of substrates. Here, we provide a quantitative characterization, using X-ray diffraction and optical methods, to elucidate the additive growth mechanism of MAPLE-deposited poly(3-hexylthiophene) (P3HT) films on substrates that have undergone different surface treatments, enabling them to possess different wettabilities. We show that MAPLE-deposited films are composed of crystalline phases, wherein the overall P3HT aggregate size and crystallite coherence length increase with deposition time. A complete pole figure constructed from X-ray diffraction measurements reveals that in these MAPLE-deposited films, there exist two distinct crystallite populations: (i) highly oriented crystals that grow from the flat dielectric substrate and (ii) misoriented crystals that preferentially grow on top of the existing polymer layers. The growth of the highly oriented crystals is highly sensitive to the chemistry of the substrate, whereas the effect of substrate chemistry on misoriented crystal growth is weaker. The use of a self-assembled monolayer to treat the substrate greatly enhances the population and crystallite coherence length at the buried interfaces, particularly during the early stage of deposition. Furthermore, the evolution of the in-plane carrier mobilities during the course of deposition is consistent with the development of highly oriented crystals at the buried interface, suggesting that this interface plays a key role toward determining carrier transport in organic thin-film transistors.},
doi = {10.1021/acsami.7b13609},
journal = {ACS Applied Materials and Interfaces},
number = 51,
volume = 9,
place = {United States},
year = {2017},
month = {11}
}

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Works referenced in this record:

Organic light-emitting diode (OLED) technology: materials, devices and display technologies
journal, January 2006

  • Geffroy, Bernard; le Roy, Philippe; Prat, Christophe
  • Polymer International, Vol. 55, Issue 6
  • DOI: 10.1002/pi.1974

25th Anniversary Article: Organic Field-Effect Transistors: The Path Beyond Amorphous Silicon
journal, January 2014


Conjugated Polymer-Based Organic Solar Cells
journal, April 2007

  • Günes, Serap; Neugebauer, Helmut; Sariciftci, Niyazi Serdar
  • Chemical Reviews, Vol. 107, Issue 4, p. 1324-1338
  • DOI: 10.1021/cr050149z

Small Bandgap Polymers for Organic Solar Cells (Polymer Material Development in the Last 5 Years)
journal, August 2008


Introduction to Organic Thin Film Transistors and Design of n-Channel Organic Semiconductors
journal, August 2004

  • Newman, Christopher R.; Frisbie, C. Daniel; da Silva Filho, Demetrio A.
  • Chemistry of Materials, Vol. 16, Issue 23, p. 4436-4451
  • DOI: 10.1021/cm049391x

Printing Highly Efficient Organic Solar Cells
journal, September 2008

  • Hoth, Claudia N.; Schilinsky, Pavel; Choulis, Stelios A.
  • Nano Letters, Vol. 8, Issue 9
  • DOI: 10.1021/nl801365k

High-Performance Semiconducting Polythiophenes for Organic Thin-Film Transistors
journal, March 2004

  • Ong, Beng S.; Wu, Yiliang; Liu, Ping
  • Journal of the American Chemical Society, Vol. 126, Issue 11, p. 3378-3379
  • DOI: 10.1021/ja039772w

Increased mobility from regioregular poly(3-hexylthiophene) field-effect transistors
journal, May 2003

  • Wang, Guangming; Swensen, James; Moses, Daniel
  • Journal of Applied Physics, Vol. 93, Issue 10
  • DOI: 10.1063/1.1568526

Dependence of persistent photocurrent on gate bias in inkjet printed organic thin-film transistor
journal, March 2010

  • Kim, Chang Hyun; Choi, Min Hee; Lee, Sun Hee
  • Applied Physics Letters, Vol. 96, Issue 12
  • DOI: 10.1063/1.3372619

High-Resolution Inkjet Printing of All-Polymer Transistor Circuits
journal, December 2000


High performance airbrushed organic thin film transistors
journal, March 2010

  • Chan, Calvin K.; Richter, Lee J.; Dinardo, Brad
  • Applied Physics Letters, Vol. 96, Issue 13
  • DOI: 10.1063/1.3360230

Efficient Solvent-Assisted Post-Treatment for Molecular Rearrangement of Sprayed Polymer Field-Effect Transistors
journal, December 2011

  • Park, Hye-Yun; Yang, Hoichang; Choi, Si-Kyung
  • ACS Applied Materials & Interfaces, Vol. 4, Issue 1
  • DOI: 10.1021/am201274s

Growth of organic thin films by the matrix assisted pulsed laser evaporation (MAPLE) technique
journal, November 1999


Laser Deposition of Polymer and Biomaterial Films
journal, February 2003

  • Chrisey, D. B.; Piqué, A.; McGill, R. A.
  • Chemical Reviews, Vol. 103, Issue 2
  • DOI: 10.1021/cr010428w

MAPLE Deposition of Macromolecules
journal, February 2013

  • Shepard, Kimberly B.; Priestley, Rodney D.
  • Macromolecular Chemistry and Physics, Vol. 214, Issue 8
  • DOI: 10.1002/macp.201200621

Patchy Janus particles with tunable roughness and composition via vapor-assisted deposition of macromolecules
journal, March 2015

  • Shepard, Kimberly B.; Christie, Dane A.; Sosa, Chris L.
  • Applied Physics Letters, Vol. 106, Issue 9
  • DOI: 10.1063/1.4913913

Growth of polymer–metal nanocomposites by pulsed laser deposition
journal, December 2008


Tabletop Resonant Infrared Matrix-Assisted Pulsed Laser Evaporation of Light-Emitting Organic Thin Films
journal, January 2008

  • Pate, Ryan; Lantz, Kevin R.; Stiff-Roberts, Adrienne D.
  • IEEE Journal of Selected Topics in Quantum Electronics, Vol. 14, Issue 4
  • DOI: 10.1109/jstqe.2008.915625

Bulk heterojunction PCPDTBT:PC 71 BM organic solar cells deposited by emulsion-based, resonant infrared matrix-assisted pulsed laser evaporation
journal, June 2014

  • McCormick, Ryan D.; Nyikayaramba, Gift; Stiff-Roberts, Adrienne D.
  • Applied Physics Letters, Vol. 104, Issue 22
  • DOI: 10.1063/1.4881058

Emulsion-Based RIR-MAPLE Deposition of Conjugated Polymers: Primary Solvent Effect and Its Implications on Organic Solar Cell Performance
journal, July 2016

  • Ge, Wangyao; Li, Nan K.; McCormick, Ryan D.
  • ACS Applied Materials & Interfaces, Vol. 8, Issue 30
  • DOI: 10.1021/acsami.6b05596

Influence of morphological disorder on in- and out-of-plane charge transport in conjugated polymer films
journal, November 2015

  • Li, Anton; Dong, Ban Xuan; Green, Peter F.
  • MRS Communications, Vol. 5, Issue 4
  • DOI: 10.1557/mrc.2015.72

Growth of polyalkylthiophene films by matrix assisted pulsed laser evaporation
journal, March 2004


Effects of Emulsion-Based Resonant Infrared Matrix Assisted Pulsed Laser Evaporation (RIR-MAPLE) on the Molecular Weight of Polymers
journal, February 2012

  • McCormick, Ryan D.; Lenhardt, Jeremy; Stiff-Roberts, Adrienne D.
  • Polymers, Vol. 4, Issue 1
  • DOI: 10.3390/polym4010341

White multi-layered polymer light emitting diode through matrix assisted pulsed laser evaporation
journal, January 2016

  • Mariano, F.; Caricato, A. P.; Accorsi, G.
  • Journal of Materials Chemistry C, Vol. 4, Issue 32
  • DOI: 10.1039/c6tc01826b

Hybrid nanocomposite thin films deposited by emulsion-based resonant infrared matrix-assisted pulsed laser evaporation for photovoltaic applications
journal, July 2015


Molecular organization in MAPLE-deposited conjugated polymer thin films and the implications for carrier transport characteristics
journal, September 2016

  • Dong, Ban Xuan; Li, Anton; Strzalka, Joseph
  • Journal of Polymer Science Part B: Polymer Physics, Vol. 55, Issue 1
  • DOI: 10.1002/polb.24237

Band bending in conjugated polymer films: role of morphology and implications for bulk charge transport characteristics
journal, January 2017

  • Wenderott, J. K.; Dong, Ban Xuan; Green, Peter F.
  • Journal of Materials Chemistry C, Vol. 5, Issue 30
  • DOI: 10.1039/c7tc02302b

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

Radiation damage in polymer films from grazing-incidence X-ray scattering measurements
journal, February 2016

  • Vaselabadi, Saeed Ahmadi; Shakarisaz, David; Ruchhoeft, Paul
  • Journal of Polymer Science Part B: Polymer Physics, Vol. 54, Issue 11
  • DOI: 10.1002/polb.24006

Quantification of Thin Film Crystallographic Orientation Using X-ray Diffraction with an Area Detector
journal, June 2010

  • Baker, Jessy L.; Jimison, Leslie H.; Mannsfeld, Stefan
  • Langmuir, Vol. 26, Issue 11
  • DOI: 10.1021/la904840q

Vertical confinement and interface effects on the microstructure and charge transport of P3HT thin films
journal, February 2013

  • Jimison, Leslie H.; Himmelberger, Scott; Duong, Duc T.
  • Journal of Polymer Science Part B: Polymer Physics, Vol. 51, Issue 7
  • DOI: 10.1002/polb.23265

Nanoscale Orientation Effects on Carrier Transport in a Low-Band-Gap Polymer
journal, July 2014

  • Dong, Ban Xuan; Huang, Bingyuan; Tan, Aaron
  • The Journal of Physical Chemistry C, Vol. 118, Issue 31
  • DOI: 10.1021/jp506374m

Modeling disorder in polymer aggregates: The optical spectroscopy of regioregular poly(3-hexylthiophene) thin films
journal, June 2005

  • Spano, Frank C.
  • The Journal of Chemical Physics, Vol. 122, Issue 23
  • DOI: 10.1063/1.1914768

H- and J-Aggregate Behavior in Polymeric Semiconductors
journal, April 2014


Molecular dynamics simulation study of the ejection and transport of polymer molecules in matrix-assisted pulsed laser evaporation
journal, October 2007

  • Leveugle, Elodie; Zhigilei, Leonid V.
  • Journal of Applied Physics, Vol. 102, Issue 7
  • DOI: 10.1063/1.2783898

Origins of nanostructure in amorphous polymer coatings via matrix assisted pulsed laser evaporation
journal, September 2013

  • Shepard, Kimberly B.; Arnold, Craig B.; Priestley, Rodney D.
  • Applied Physics Letters, Vol. 103, Issue 12
  • DOI: 10.1063/1.4821366

Role of Intermolecular Coupling in the Photophysics of Disordered Organic Semiconductors: Aggregate Emission in Regioregular Polythiophene
journal, May 2007


Excitonic versus electronic couplings in molecular assemblies: The importance of non-nearest neighbor interactions
journal, January 2009

  • Gierschner, Johannes; Huang, Ya-Shih; Van Averbeke, Bernard
  • The Journal of Chemical Physics, Vol. 130, Issue 4
  • DOI: 10.1063/1.3065267

Two-dimensional charge transport in self-organized, high-mobility conjugated polymers
journal, October 1999

  • Sirringhaus, H.; Brown, P. J.; Friend, R. H.
  • Nature, Vol. 401, Issue 6754, p. 685-688
  • DOI: 10.1038/44359

Depth-resolved molecular structure and orientation of polymer thin films by synchrotron X-ray diffraction
journal, March 2011


Thickness Dependence of the Crystalline Structure and Hole Mobility in Thin Films of Low Molecular Weight Poly(3-hexylthiophene)
journal, September 2008

  • Joshi, Siddharth; Grigorian, Souren; Pietsch, Ullrich
  • Macromolecules, Vol. 41, Issue 18
  • DOI: 10.1021/ma702802x

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

X-ray Scattering Study of Thin Films of Poly(2,5-bis(3-alkylthiophen-2-yl)thieno[3,2- b ]thiophene)
journal, March 2007

  • Chabinyc, Michael L.; Toney, Michael F.; Kline, R. Joseph
  • Journal of the American Chemical Society, Vol. 129, Issue 11
  • DOI: 10.1021/ja0670714

Layering Transitions in Thin Films of Spherical-Domain Block Copolymers
journal, April 2007

  • Stein, Gila E.; Kramer, Edward J.; Li, Xuefa
  • Macromolecules, Vol. 40, Issue 7
  • DOI: 10.1021/ma0625509

Molecular Order in High-Efficiency Polymer/Fullerene Bulk Heterojunction Solar Cells
journal, September 2011

  • Hammond, Matthew R.; Kline, R. Joseph; Herzing, Andrew A.
  • ACS Nano, Vol. 5, Issue 10
  • DOI: 10.1021/nn202951e

Surface induced orientation and vertically layered morphology in thin films of poly(3-hexylthiophene) crystallized from the melt
journal, April 2017

  • Balko, Jens; Portale, Guiseppe; Lohwasser, Ruth H.
  • Journal of Materials Research, Vol. 32, Issue 10
  • DOI: 10.1557/jmr.2017.107

Scherrer grain-size analysis adapted to grazing-incidence scattering with area detectors
journal, October 2009


Quantitative analysis of lattice disorder and crystallite size in organic semiconductor thin films
journal, July 2011


Phase Diagram of P3HT/PCBM Blends and Its Implication for the Stability of Morphology
journal, February 2009

  • Zhao, Jun; Swinnen, Ann; Van Assche, Guy
  • The Journal of Physical Chemistry B, Vol. 113, Issue 6, p. 1587-1591
  • DOI: 10.1021/jp804151a

Solar Cells: Morphological Degradation in Low Bandgap Polymer Solar Cells - An In Operando Study (Adv. Energy Mater. 19/2016)
journal, October 2016

  • Schaffer, Christoph J.; Palumbiny, Claudia M.; Niedermeier, Martin A.
  • Advanced Energy Materials, Vol. 6, Issue 19
  • DOI: 10.1002/aenm.201670115

Additive Growth and Crystallization of Polymer Films
journal, March 2016


Polymer thin-film transistors with chemically modified dielectric interfaces
journal, December 2002

  • Salleo, A.; Chabinyc, M. L.; Yang, M. S.
  • Applied Physics Letters, Vol. 81, Issue 23
  • DOI: 10.1063/1.1527691

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

Enhancing Carrier Mobilities in Organic Thin-Film Transistors Through Morphological Changes at the Semiconductor/Dielectric Interface Using Supercritical Carbon Dioxide Processing
journal, November 2016

  • Dong, Ban Xuan; Amonoo, Jojo A.; Purdum, Geoffrey E.
  • ACS Applied Materials & Interfaces, Vol. 8, Issue 45
  • DOI: 10.1021/acsami.6b08248

Mechanism of Crystallization and Implications for Charge Transport in Poly(3-ethylhexylthiophene) Thin Films
journal, April 2014

  • Duong, Duc T.; Ho, Victor; Shang, Zhengrong
  • Advanced Functional Materials, Vol. 24, Issue 28
  • DOI: 10.1002/adfm.201304247

    Works referencing / citing this record:

    Self-Assembly Behavior of an Oligothiophene-Based Conjugated Liquid Crystal and Its Implication for Ionic Conductivity Characteristics
    journal, November 2018

    • Liu, Ziwei; Dong, Ban Xuan; Misra, Mayank
    • Advanced Functional Materials, Vol. 29, Issue 2
    • DOI: 10.1002/adfm.201805220

    Molecular weight dependent structure and charge transport in MAPLE-deposited poly(3-hexylthiophene) thin films
    journal, February 2018

    • Dong, Ban Xuan; Smith, Mitchell; Strzalka, Joseph
    • Journal of Polymer Science Part B: Polymer Physics, Vol. 56, Issue 8
    • DOI: 10.1002/polb.24588