Abstract
Performed through side-chain engineering or by incorporating intramolecular locking units, the directionality and dynamic nature of noncovalent interactions are particularly attractive for the design of novel semiconducting materials in a wide variety of applications. This work investigates the nature and position of hydrogen bonding (intra- versus intermolecular), with the objective of developing a rational approach to the design of new semiconducting materials with improved properties in the solid state. To control the polymer chains' self-assembly, a π-conjugated polymer incorporating a moiety capable of generating intramolecular hydrogen bonding is evaluated against a polymer that allows for intermolecular hydrogen bonding. Characterization through various techniques, optical spectroscopies, grazing incidence wide-angle x-ray scattering, and solution small-angle neutron scattering showed that intramolecular hydrogen bonds resulted in materials with improved crystallinity and higher effective conjugation in the solid state. Additionally, the effect of the noncovalent interaction configuration on the optoelectronic properties was analyzed in organic field-effect transistor fabrication. Devices prepared from the materials with intramolecular hydrogen bonds showed significantly higher performance, with three orders of magnitude higher charge mobility than their counterparts fabricated from polymers with intermolecular hydrogen bonds. These results confirm the importance of chemical design on polymer structures and offer a novel route for the design of high-efficiency semiconducting polymers for next-generation electronics.
| Original language | English |
|---|---|
| Pages (from-to) | 8267-8277 |
| Number of pages | 11 |
| Journal | Chemistry of Materials |
| Volume | 33 |
| Issue number | 21 |
| DOIs | |
| State | Published - Nov 9 2021 |
Funding
The authors thank Prof. Armand Soldera at Universit? de Sherbrooke for use of their allocated computing time. R.B.G. thanks NSERC for financial support through an Undergraduate Student Research Award (USRA). M.U.O. thanks NSERC for support through a postgraduate doctoral scholarship (PGS-D). L.A.G. acknowledges support from the NSF NRT program ?Interface? (award #DGE-1449999) through the University of Southern Mississippi. A portion of this research used resources at the Spallation Neutron Source, a DOE Office of Science User Facility operated by the Oak Ridge National Laboratory. This work was supported by NSERC through a Discovery Grant (RGPIN: 2017-06611). S.R.-G. also acknowledges the Canadian Foundation for Innovation for infrastructure support. Y.-C.C. thanks the Ministry of Science and Technology, Taiwan, for financial support (Project Number 110-2221-E-011-009). Y.F., L.A.G., Z.C., S.Z., and X.G. thank the financial support by the U.S. Department of Energy, Office of Science, Office of Basic Energy Science under award number of DE-SC0019361 for supporting the neutron scattering experiment and data analysis. The authors declare no competing financial interest. The authors thank Prof. Armand Soldera at Universite\u0301 de Sherbrooke for use of their allocated computing time. R.B.G. thanks NSERC for financial support through an Undergraduate Student Research Award (USRA). M.U.O. thanks NSERC for support through a postgraduate doctoral scholarship (PGS-D). L.A.G. acknowledges support from the NSF NRT program \u201CInterface\u201D (award #DGE-1449999) through the University of Southern Mississippi. A portion of this research used resources at the Spallation Neutron Source, a DOE Office of Science User Facility operated by the Oak Ridge National Laboratory.