Rethinking the models of charge transport in polymeric semiconductors
Lead Research Organisation:
University of Liverpool
Department Name: Chemistry
Abstract
The structure-property relation of semiconducting polymers is poorly understood and there is no guidance for the design of new materials. We have noted an important mismatch between the assumption used to model charge transport in polymers (phenomenological theories) and the results of electronic structure calculation of realistic polymers (atomistic theories). The latter show that, as carriers are promoted to higher energy, they access more delocalized states characterized by longer range electron transfer and smaller polaronic effects. No model of transport currently takes this effect into account.
This proposal will build new foundations of the phenomenological theories based on a more detailed knowledge of the electronic properties of few selected systems. Existing results on amorphous low mobility polymers (like PPV) and semicrystalline polymers (line P3HT and PBTTT) will be combined with new simulations of amorphous high mobility polymers (of the DPP class) to achieve a detailed description of representatives from each main class of semiconducting polymers.
A new, more general and more accurate, expression for the rate of change hopping between sites will be introduced. A model Hamiltonian will be built to reproduce the main features of the electronic structure of realistic polymers. In essence, we will build a connection between detailed models of the chemistry of the system and the more simplified models needed to study charge transport.
With the new methodology we will determine the actual number of parameters that affects the mobility in polymeric semiconductors considering the recent experimental observation by Paul Blom's group that the incredible diversity in semiconducting polymers may be actually reducible into a single effective parameter per material. Moreover, the methodology lends itself to making predictions on new chemical structures of high mobility polymers.
This proposal benefits from the collaboration of Paul Blom (Eindhoven), David Haddleton (Warwick). A PhD student already in the group will contribute to some of the tasks.
This proposal will build new foundations of the phenomenological theories based on a more detailed knowledge of the electronic properties of few selected systems. Existing results on amorphous low mobility polymers (like PPV) and semicrystalline polymers (line P3HT and PBTTT) will be combined with new simulations of amorphous high mobility polymers (of the DPP class) to achieve a detailed description of representatives from each main class of semiconducting polymers.
A new, more general and more accurate, expression for the rate of change hopping between sites will be introduced. A model Hamiltonian will be built to reproduce the main features of the electronic structure of realistic polymers. In essence, we will build a connection between detailed models of the chemistry of the system and the more simplified models needed to study charge transport.
With the new methodology we will determine the actual number of parameters that affects the mobility in polymeric semiconductors considering the recent experimental observation by Paul Blom's group that the incredible diversity in semiconducting polymers may be actually reducible into a single effective parameter per material. Moreover, the methodology lends itself to making predictions on new chemical structures of high mobility polymers.
This proposal benefits from the collaboration of Paul Blom (Eindhoven), David Haddleton (Warwick). A PhD student already in the group will contribute to some of the tasks.
Planned Impact
The UK is world leading in organic electronics research, including synthesis, processing and device fabrication. Developing the ability to design radically different high-mobility polymers will ensure that critical intellectual property is retained in the county and the large investments in the area are protected. The risk of losing leadership is particularly high when there are fundamental gaps in understanding that may occasionally reward luck over design.
The very large number of potential applications suggests that organic electronics and its theoretical underpinning will constitute an important share of industrialized economies in the future. Display technology based on organic electronics is already well developed. Biomedical sensors and low cost transistors are emerging in the market and very intense activity if focused on the use of polymers in organic solar cells. Detailed plans have been proposed within this project to engage with the private sector and the Warwick technology transfer office with the objective of maximizing the short term impact of the scientific outcome of this research and to foster new collaborations.
A robust dissemination plan toward the academic community is in place as well as opportunities for training the main researchers carrying out this work. The high profile collaborators will strengthen the international profile of the project.
The very large number of potential applications suggests that organic electronics and its theoretical underpinning will constitute an important share of industrialized economies in the future. Display technology based on organic electronics is already well developed. Biomedical sensors and low cost transistors are emerging in the market and very intense activity if focused on the use of polymers in organic solar cells. Detailed plans have been proposed within this project to engage with the private sector and the Warwick technology transfer office with the objective of maximizing the short term impact of the scientific outcome of this research and to foster new collaborations.
A robust dissemination plan toward the academic community is in place as well as opportunities for training the main researchers carrying out this work. The high profile collaborators will strengthen the international profile of the project.
Organisations
Publications
Claridge K
(2019)
Developing Consistent Molecular Dynamics Force Fields for Biological Chromophores via Force Matching.
in The journal of physical chemistry. B
Claridge K
(2019)
On the arrangement of chromophores in light harvesting complexes: chance versus design.
in Faraday discussions
Dantanarayana V
(2020)
Predictive Model of Charge Mobilities in Organic Semiconductor Small Molecules with Force-Matched Potentials.
in Journal of chemical theory and computation
Elliott JD
(2020)
A QM/MD Coupling Method to Model the Ion-Induced Polarization of Graphene.
in Journal of chemical theory and computation
Fornari RP
(2017)
How Many Parameters Actually Affect the Mobility of Conjugated Polymers?
in Physical review letters
Fornari RP
(2017)
Importance and Nature of Short-Range Excitonic Interactions in Light Harvesting Complexes and Organic Semiconductors.
in Journal of chemical theory and computation
Fratini S
(2017)
A map of high-mobility molecular semiconductors.
in Nature materials
Geng Y
(2017)
Effect of Infrared Pulse Excitation on the Bound Charge-Transfer State of Photovoltaic Interfaces.
in The journal of physical chemistry letters
Harrelson T
(2019)
Direct probe of the nuclear modes limiting charge mobility in molecular semiconductors
in Materials Horizons
Kuzmich A
(2017)
Trends in the electronic and geometric structure of non-fullerene based acceptors for organic solar cells
in Energy & Environmental Science
Landi A
(2021)
Quantitative Prediction of the Electro-Mechanical Response in Organic Crystals.
in Advanced materials (Deerfield Beach, Fla.)
Landi A
(2018)
Rapid Evaluation of Dynamic Electronic Disorder in Molecular Semiconductors
in The Journal of Physical Chemistry C
Landi A
(2019)
Explaining different experimental hole mobilities: influence of polymorphism on dynamic disorder in pentacene
in Journal of Materials Chemistry C
Li P
(2018)
Systematic Study of the Effect of Auxiliary Acceptors in D-A'-p-A Sensitizers Used on Dye-Sensitized Solar Cells
in The Journal of Physical Chemistry C
Manurung R
(2021)
Rapid Method for Calculating the Conformationally Averaged Electronic Structure of Conjugated Polymers
in The Journal of Physical Chemistry B
Matta M
(2020)
Relation between Local Structure, Electric Dipole, and Charge Carrier Dynamics in DHICA Melanin: A Model for Biocompatible Semiconductors.
in The journal of physical chemistry letters
Moser M
(2020)
Ethylene Glycol-Based Side Chain Length Engineering in Polythiophenes and its Impact on Organic Electrochemical Transistor Performance
in Chemistry of Materials
Nematiaram T
(2020)
Strategies to reduce the dynamic disorder in molecular semiconductors
in Materials Horizons
Nematiaram T
(2020)
Modeling charge transport in high-mobility molecular semiconductors: Balancing electronic structure and quantum dynamics methods with the help of experiments.
in The Journal of chemical physics
Nematiaram T
(2019)
Practical Computation of the Charge Mobility in Molecular Semiconductors Using Transient Localization Theory
in The Journal of Physical Chemistry C
Omar ÖH
(2022)
Organic materials repurposing, a data set for theoretical predictions of new applications for existing compounds.
in Scientific data
Padula D
(2019)
Singlet fission molecules among known compounds: finding a few needles in a haystack
in Energy & Environmental Science
Padula D
(2019)
Combining electronic and structural features in machine learning models to predict organic solar cells properties
in Materials Horizons
Padula D
(2019)
Concurrent Optimization of Organic Donor-Acceptor Pairs through Machine Learning
in Advanced Energy Materials
Reisjalali M
(2021)
Local structuring of diketopyrrolopyrrole (DPP)-based oligomers from molecular dynamics simulations.
in Physical chemistry chemical physics : PCCP
Description | We developed a universal theory of transport in polymeric materials that explan a very broad range of observation put forward by the group of Prof. Blom (these have been published in PRL 2017). |
Exploitation Route | The theory was used to propose new high performance polymeric materials. |
Sectors | Chemicals,Electronics,Energy |
Description | A Theory of Organic Bioelectronics |
Amount | € 2,257,300 (EUR) |
Organisation | European Research Council (ERC) |
Sector | Public |
Country | Belgium |
Start | 10/2021 |
End | 09/2026 |