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Structural and Dynamic Disorder, Not Ionic Trapping, Controls Charge Transport in Highly Doped Conducting Polymers

Ian E. JacobsOptoelectronics Group, Cavendish Laboratory, University of Cambridge, J J Thomson Avenue, Cambridge CB3 0HE, U.KGabriele D’AvinoGrenoble Alpes University, CNRS, Grenoble INP, Institut Néel, 25 rue des Martyrs, 38042 Grenoble, FranceVincent LemaurLaboratory for Chemistry of Novel Materials, University of Mons, Mons B-7000, BelgiumYue LinOptoelectronics Group, Cavendish Laboratory, University of Cambridge, J J Thomson Avenue, Cambridge CB3 0HE, U.KYuxuan HuangOptoelectronics Group, Cavendish Laboratory, University of Cambridge, J J Thomson Avenue, Cambridge CB3 0HE, U.KChen ChenOptoelectronics Group, Cavendish Laboratory, University of Cambridge, J J Thomson Avenue, Cambridge CB3 0HE, U.KThomas F. HarrelsonMolecular Foundry, Lawrence Berkeley National Laboratory, One Cyclotron Road Building 67, Berkeley, California 94720, United StatesWilliam A. WoodOptoelectronics Group, Cavendish Laboratory, University of Cambridge, J J Thomson Avenue, Cambridge CB3 0HE, U.KLeszek J. SpalekOptoelectronics Group, Cavendish Laboratory, University of Cambridge, J J Thomson Avenue, Cambridge CB3 0HE, U.KTarig MustafaDepartment of Chemistry, University of Cambridge, Lensfield Road, Cambridge CB2 1EW, U.KChristopher A. O’KeefeDepartment of Chemistry, University of Cambridge, Lensfield Road, Cambridge CB2 1EW, U.KXinglong RenOptoelectronics Group, Cavendish Laboratory, University of Cambridge, J J Thomson Avenue, Cambridge CB3 0HE, U.KDimitrios SimatosDepartment of Chemistry, University of Cambridge, Lensfield Road, Cambridge CB2 1EW, U.KDion TjheOptoelectronics Group, Cavendish Laboratory, University of Cambridge, J J Thomson Avenue, Cambridge CB3 0HE, U.KMartin StatzOptoelectronics Group, Cavendish Laboratory, University of Cambridge, J J Thomson Avenue, Cambridge CB3 0HE, U.KJoseph StrzalkaX-Ray Science Division, Argonne National Laboratory, Lemont, Illinois 60439, United StatesJin‐Kyun LeeDepartment of Polymer Science & Engineering, Inha University, Incheon 402-751, South KoreaIain McCullochDepartment of Chemistry, University of Oxford, Oxford OX1 3TA, U.KS. FratiniGrenoble Alpes University, CNRS, Grenoble INP, Institut Néel, 25 rue des Martyrs, 38042 Grenoble, FranceDavid BeljonneLaboratory for Chemistry of Novel Materials, University of Mons, Mons B-7000, BelgiumHenning SirringhausOptoelectronics Group, Cavendish Laboratory, University of Cambridge, J J Thomson Avenue, Cambridge CB3 0HE, U.K

2022en

ABI

Annotatsiya

Doped organic semiconductors are critical to emerging device applications, including thermoelectrics, bioelectronics, and neuromorphic computing devices. It is commonly assumed that low conductivities in these materials result primarily from charge trapping by the Coulomb potentials of the dopant counterions. Here, we present a combined experimental and theoretical study rebutting this belief. Using a newly developed doping technique based on ion exchange, we prepare highly doped films with several counterions of varying size and shape and characterize their carrier density, electrical conductivity, and paracrystalline disorder. In this uniquely large data set composed of several classes of high-mobility conjugated polymers, each doped with at least five different ions, we find electrical conductivity to be strongly correlated with paracrystalline disorder but poorly correlated with ionic size, suggesting that Coulomb traps do not limit transport. A general model for interacting electrons in highly doped polymers is proposed and carefully parametrized against atomistic calculations, enabling the calculation of electrical conductivity within the framework of transient localization theory. Theoretical calculations are in excellent agreement with experimental data, providing insights into the disorder-limited nature of charge transport and suggesting new strategies to further improve conductivities.

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DOI: 10.1021/jacs.1c10651

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