Polaron Delocalization and Transport in Doped Graphene Nanoribbon Thin Films

Hermosilla-Palacios, M. Alejandra; Lindenthal, Sebastian; Earley, Justin D.; Aubry, Taylor J.; DeLuca, David; Al Khunaizi, Hashim; Spokoyny, Alexander M.; Zaumseil, Jana; Ferguson, Andrew J.; Blackburn, Jeffrey L.

doi:10.1021/acsnano.5c03888

Title: Polaron Delocalization and Transport in Doped Graphene Nanoribbon Thin Films

Journal Article · Mon Jul 07 00:00:00 UTC 2025 · ACS Nano

DOI: https://doi.org/10.1021/acsnano.5c03888 · OSTI ID:2573963

^[1]; Lindenthal, Sebastian ^[2];

^[1];

^[1]; DeLuca, David ^[3]; Al Khunaizi, Hashim ^[3];

^[3];

^[2];

^[1];

^[1]

National Renewable Energy Laboratory (NREL), Golden, CO (United States)
Heidelberg University (Germany)
University of California, Los Angeles, CA (United States)

Graphene nanoribbons (GNRs) are quantum-confined π-conjugated monolayer semiconductors with attractive properties for optoelectronic applications. However, the ground- and excited-state properties of charge carriers in GNRs are still poorly understood, particularly with regards to the coupling between charges and the GNR lattice and the degree to which this coupling impacts local and macroscopic charge transport. To address this issue, we systematically correlate carrier density-dependent charge transport with spectroscopic modulations in chemically doped thin films of armchair graphene nanoribbons (9-aGNRs). This study combines Fourier transform infrared (FTIR) and ultraviolet−visible−near-infrared (UV−vis−NIR) spectroscopy with both local and macroscopic conductivity measurements to arrive at a full and self-consistent picture of transport in doped GNR thin films. Using three different molecular p-type dopants (i.e., oxidants), we demonstrate that hole polarons are the dominant quasi-particle determining charge transport in GNRs and that the degree of polaron delocalization depends sensitively on the dopant and the hole density. For all three dopants, the local conductivity probed by microwave spectroscopy substantially exceeds the long-range conductivity obtained by four-point probe measurements. Interestingly, the dopant size substantially influences charge transport at high hole densities. We ascribe this effect to different propensities for forming bipolarons with lower mobilities than polarons. Comparison of GNR transport and spectral properties to other prototypical π-conjugated semiconductors (e.g., semiconducting polymers or carbon nanotubes) benchmark the charge transport properties of GNR thin films for optoelectronic devices and applications.

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Research Organization:: National Renewable Energy Laboratory (NREL), Golden, CO (United States)

Sponsoring Organization:: European Research Council (ERC); National Institute of General Medical Sciences (NIGMS); USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division (CSGB)

Grant/Contract Number:: AC36-08GO28308

OSTI ID:: 2573963

Report Number(s):: NREL/JA--5900-93393

Journal Information:: ACS Nano, Journal Name: ACS Nano Journal Issue: 28 Vol. 19; ISSN 1936-086X; ISSN 1936-0851

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS
carrier delocalization
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Title: Polaron Delocalization and Transport in Doped Graphene Nanoribbon Thin Films

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