skip to main content
OSTI.GOV title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Inducing Molecular Aggregation of Polymer Semiconductors in a Secondary Insulating Polymer Matrix to Enhance Charge Transport

Journal Article · · Chemistry of Materials

Polymer semiconductors (PSCs) are a desirable class of materials for next-generation electronics. However, the conformational complexity associated with macromolecules, as well as the presence of unique inter- and intrachain interactions, make it challenging to control the morphology of PSCs. Previously, it has been reported that beyond a certain molecular weight, thin-film charge carrier mobility typically drops due to reduced crystallinity and increased entanglement. In this work, the use of an insulating secondary matrix polymer, polystyrene-block-poly(ethylene-ran-butylene)-block-polystyrene (SEBS), is shown to induce molecular ordering of PSCs across multiple length scales. Aggregation-induced molecular ordering in SEBS/PSC hybrid films is strongly correlated to the molecular weight of the semiconducting component. The higher the molecular weight of PSC used to blend with SEBS, the greater the observed improvement in polymer aggregation and orientation. This leads to a 5-fold increase of charge carrier mobility, from 0.3 to 1.5 cm2 V–1 s–1 (P-97k), in field-effect transistors (FETs) with only 30 wt % of the semiconducting polymer in SEBS. Moreover, mobility can be further elevated to 2 cm2 V–1 s–1 using an extensional flow-driven solution shearing deposition method. The findings here on using a secondary polymer matrix to dramatically improve the molecular organization and charge transport of a high-molecular-weight PSC are a useful morphological control strategy. It can also be carried out using nonhalogenated solvents, such as $$p$$-xylene, which are more environmentally benign and industrially relevant than commonly used chlorinated solvents.

Research Organization:
SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States). Stanford Synchrotron Radiation Lightsource (SSRL); Stanford Univ., CA (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES); Ministry of Science and Technology of Taiwan; National Science Foundation (NSF)
Grant/Contract Number:
AC02-76SF00515; SC0016523; MOST 106-2917-I-564-023; ECCS-1542152
OSTI ID:
1605283
Alternate ID(s):
OSTI ID: 1782829; OSTI ID: 1985486
Journal Information:
Chemistry of Materials, Vol. 32, Issue 2; ISSN 0897-4756
Publisher:
American Chemical Society (ACS)Copyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 30 works
Citation information provided by
Web of Science

References (35)

Materials and Applications for Large Area Electronics: Solution-Based Approaches journal January 2010
25th Anniversary Article: Organic Field-Effect Transistors: The Path Beyond Amorphous Silicon journal January 2014
Mechanical Properties of Organic Semiconductors for Stretchable, Highly Flexible, and Mechanically Robust Electronics journal March 2017
Organic Semiconductor/Polymer Blend Films for Organic Field‐Effect Transistors journal June 2019
Morphology and field-effect transistor characteristics of semicrystalline poly(3-hexylthiophene) and poly(stearyl acrylate) blend nanowires journal January 2012
Optically transparent semiconducting polymer nanonetwork for flexible and transparent electronics journal November 2016
Robust and Stretchable Polymer Semiconducting Networks: From Film Microstructure to Macroscopic Device Performance journal December 2018
Multi-scale ordering in highly stretchable polymer semiconducting films journal April 2019
Highly stretchable polymer semiconductor films through the nanoconfinement effect journal January 2017
Effective Use of Electrically Insulating Units in Organic Semiconductor Thin Films for High-Performance Organic Transistors journal December 2016
Enhancing Crystalline Structural Orders of Polymer Semiconductors for Efficient Charge Transport via Polymer-Matrix-Mediated Molecular Self-Assembly journal May 2016
Solution-Processed Donor-Acceptor Polymer Nanowire Network Semiconductors For High-Performance Field-Effect Transistors journal April 2016
The impact of molecular weight on microstructure and charge transport in semicrystalline polymer semiconductors–poly(3-hexylthiophene), a model study journal December 2013
A general relationship between disorder, aggregation and charge transport in conjugated polymers journal August 2013
Importance of Critical Molecular Weight of Semicrystalline n-Type Polymers for Mechanically Robust, Efficient Electroactive Thin Films journal April 2019
Entanglements in marginal solutions: a means of tuning pre-aggregation of conjugated polymers with positive implications for charge transport journal January 2015
Synthesis and Properties of Soluble Fused Thiophene Diketopyrrolopyrrole-Based Polymers with Tunable Molecular Weight journal November 2018
Controlling the Field-Effect Mobility of Regioregular Polythiophene by Changing the Molecular Weight journal September 2003
Influence of Semiconductor Thickness and Molecular Weight on the Charge Transport of a Naphthalenediimide-Based Copolymer in Thin-Film Transistors journal March 2015
All-Polymer Solar Cell Performance Optimized via Systematic Molecular Weight Tuning of Both Donor and Acceptor Polymers journal January 2016
Charge Transport in Organic Semiconductors journal April 2007
Exploring the origin of high optical absorption in conjugated polymers journal May 2016
Two-dimensional charge transport in self-organized, high-mobility conjugated polymers journal October 1999
Observation of a Distinct Surface Molecular Orientation in Films of a High Mobility Conjugated Polymer journal January 2013
Annealing-Free High-Mobility Diketopyrrolopyrrole−Quaterthiophene Copolymer for Solution-Processed Organic Thin Film Transistors journal February 2011
Enhanced Solid-State Order and Field-Effect Hole Mobility through Control of Nanoscale Polymer Aggregation journal December 2013
Role of Borderline Solvents to Induce Pronounced Extended-Chain Lamellar Order in π-Stackable Polymers journal December 2011
Anomalous Charge Transport in Conjugated Polymers Reveals Underlying Mechanisms of Trapping and Percolation journal November 2016
Uniaxial Alignment of Conjugated Polymer Films for High-Performance Organic Field-Effect Transistors journal March 2018
High Mobility Organic Field-Effect Transistors from Majority Insulator Blends journal February 2016
Nonhalogenated Solvent Processable and Printable High-Performance Polymer Semiconductor Enabled by Isomeric Nonconjugated Flexible Linkers journal June 2018
Scalable Synthesis of Fused Thiophene-Diketopyrrolopyrrole Semiconducting Polymers Processed from Nonchlorinated Solvents into High Performance Thin Film Transistors journal February 2013
Green-solvent-processable organic solar cells journal November 2016
Crystalline Ultrasmooth Self-Assembled Monolayers of Alkylsilanes for Organic Field-Effect Transistors journal July 2009
Contact-induced crystallinity for high-performance soluble acene-based transistors and circuits journal February 2008