DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Tuning the Cross-Linker Crystallinity of a Stretchable Polymer Semiconductor

Journal Article · · Chemistry of Materials

The cross-linking of conjugated polymers has been shown to be an effective strategy to improve its elastic properties to give deformable semiconductors for plastic electronics. Although there have been extensive studies of the structural requirements of the polymer host for good film ductility, no work to date has focused on the relevance of the structural design or chemistry of these cross-linker additives. In this study, urethane groups and tertiary carbon atoms are inserted into the alkyl backbone of perfluorophenyl azide-based cross-linkers to investigate the importance of cross-linker crystallinity with respect to polymer morphology and hence mechanical and electrical properties. Linear cross-linkers with hydrogen bonding from urethane groups readily phase separate and recrystallize in the polymer network to form cross-linked domains that obstruct the strain distribution of the polymer film. Branch cross-linkers with tertiary carbon on the other hand form an evenly cross-linked network in the polymer blend stemming from excellent miscibility and show a 4-fold increase in fracture strain. Furthermore, a stable hole mobility of 0.2 cm2 V–1 s–1 is achieved up to ε = 100%, and a stable hole mobility of 0.1 cm2 V–1 s–1 after 2000 cycles of ε = 25% on fully stretchable organic field-effect transistors.

Research Organization:
Univ. of Southern Mississippi, Hattiesburg, MI (United States); University of Southern Mississippi, Hattiesburg, MS (United States)
Sponsoring Organization:
Air Force Office of Scientific Research (AFOSR); National Science Foundation (NSF); USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division (MSE)
Grant/Contract Number:
SC0019361
OSTI ID:
1599403
Journal Information:
Chemistry of Materials, Journal Name: Chemistry of Materials Journal Issue: 17 Vol. 31; ISSN 0897-4756
Publisher:
American Chemical Society (ACS)Copyright Statement
Country of Publication:
United States
Language:
English

References (47)

Tough, Semiconducting Polyethylene-poly(3-hexylthiophene) Diblock Copolymers journal October 2007
Anisotropic Structure and Charge Transport in Highly Strain-Aligned Regioregular Poly(3-hexylthiophene) journal August 2011
Mechanical Properties of Conjugated Polymers and Polymer-Fullerene Composites as a Function of Molecular Structure journal October 2013
Inducing Elasticity through Oligo-Siloxane Crosslinks for Intrinsically Stretchable Semiconducting Polymers journal August 2016
Effect of Nonconjugated Spacers on Mechanical Properties of Semiconducting Polymers for Stretchable Transistors journal September 2018
Polythiophene Nanofibril Bundles Surface-Embedded in Elastomer: A Route to a Highly Stretchable Active Channel Layer journal January 2015
Melt-Processing of Complementary Semiconducting Polymer Blends for High Performance Organic Transistors journal December 2016
Deformable Organic Nanowire Field-Effect Transistors journal January 2018
Tough and Water-Insensitive Self-Healing Elastomer for Robust Electronic Skin journal February 2018
Stretchable and Transparent Organic Semiconducting Thin Film with Conjugated Polymer Nanowires Embedded in an Elastomeric Matrix journal October 2015
Effects of Molecular Structure and Packing Order on the Stretchability of Semicrystalline Conjugated Poly(Tetrathienoacene-diketopyrrolopyrrole) Polymers journal December 2016
Stretchable Polymer Semiconductors for Plastic Electronics journal January 2018
Improving Miscibility of a Naphthalene Diimide-Bithiophene Copolymer with n-Type Dopants through the Incorporation of “Kinked” Monomers journal March 2018
Effect of Broken Conjugation on the Stretchability of Semiconducting Polymers journal August 2016
Probing the Viscoelastic Property of Pseudo Free-Standing Conjugated Polymeric Thin Films journal May 2018
FTIR analysis of hydrogen bonding in amorphous linear aromatic polyurethanes. I. Influence of temperature journal June 1994
Skin-Inspired Electronics: An Emerging Paradigm journal April 2018
Elastomer–Polymer Semiconductor Blends for High-Performance Stretchable Charge Transport Networks journal February 2016
Mechanical Properties of a Library of Low-Band-Gap Polymers journal March 2016
Mechanical Properties of Polymer–Fullerene Bulk Heterojunction Films: Role of Nanomorphology of Composite Films journal April 2017
Mechanical Properties of Organic Semiconductors for Stretchable, Highly Flexible, and Mechanically Robust Electronics journal March 2017
Electronic Muscles and Skins: A Review of Soft Sensors and Actuators journal August 2017
Tuning Mechanical and Optoelectrical Properties of Poly(3-hexylthiophene) through Systematic Regioregularity Control journal June 2015
Soft Poly(butyl acrylate) Side Chains toward Intrinsically Stretchable Polymeric Semiconductors for Field-Effect Transistor Applications journal June 2017
Amide-Containing Alkyl Chains in Conjugated Polymers: Effect on Self-Assembly and Electronic Properties journal February 2018
Exploiting π–π Stacking for Stretchable Semiconducting Polymers journal March 2018
Nonhalogenated Solvent Processable and Printable High-Performance Polymer Semiconductor Enabled by Isomeric Nonconjugated Flexible Linkers journal June 2018
Comparison of Methods for Determining the Mechanical Properties of Semiconducting Polymer Films for Stretchable Electronics journal March 2017
Biodegradable Polymeric Materials in Degradable Electronic Devices journal February 2018
Perfluorophenyl Azides: New Applications in Surface Functionalization and Nanomaterial Synthesis journal November 2010
Significant Improvement of Semiconducting Performance of the Diketopyrrolopyrrole–Quaterthiophene Conjugated Polymer through Side-Chain Engineering via Hydrogen-Bonding journal December 2015
Correlations between Mechanical and Electrical Properties of Polythiophenes journal November 2010
Intrinsically stretchable and healable semiconducting polymer for organic transistors journal November 2016
The rise of plastic bioelectronics journal December 2016
Skin electronics from scalable fabrication of an intrinsically stretchable transistor array journal February 2018
Molecular origin of high field-effect mobility in an indacenodithiophene–benzothiadiazole copolymer journal July 2013
Flexible, highly efficient all-polymer solar cells journal October 2015
High-performance polymer semiconducting heterostructure devices by nitrene-mediated photocrosslinking of alkyl side chains journal December 2009
Critical assessment of charge mobility extraction in FETs journal December 2017
The meniscus-guided deposition of semiconducting polymers journal February 2018
An ABA triblock copolymer strategy for intrinsically stretchable semiconductors journal January 2015
Environmentally benign fabrication processes for high-performance polymeric semiconductors journal January 2017
Biocompatible and totally disintegrable semiconducting polymer for ultrathin and ultralightweight transient electronics journal May 2017
Highly stretchable polymer semiconductor films through the nanoconfinement effect journal January 2017
Stretchable and ultraflexible organic electronics journal February 2017
Intrinsically stretchable field-effect transistors journal February 2017
Morphological considerations of organic electronic films for flexible and stretchable devices journal February 2017

Cited By (2)

Improved thin film stability of differently formulated, printed, and crosslinked polymer layers against successive solvent printing journal January 2020
Challenge and Solution of Characterizing Glass Transition Temperature for Conjugated Polymers by Differential Scanning Calorimetry journal August 2019