Emilia Benvenuti
Beyond the 2D Field‐Effect Charge Transport Paradigm in Molecular Thin‐Film Transistors
Benvenuti, Emilia; Portale, Giuseppe; Brucale, Marco; Quiroga, Santiago D.; Baldoni, Matteo; MacKenzie, Roderick C.I.; Mercuri, Francesco; Canola, Sofia; Negri, Fabrizia; Lago, Nicolò; Buonomo, Marco; Pollesel, Andrea; Cester, Andrea; Zambianchi, Massimo; Melucci, Manuela; Muccini, Michele; Toffanin, Stefano
Authors
Giuseppe Portale
Marco Brucale
Santiago D. Quiroga
Matteo Baldoni
Dr Roderick MacKenzie roderick.mackenzie@durham.ac.uk
Associate Professor
Francesco Mercuri
Sofia Canola
Fabrizia Negri
Nicolò Lago
Marco Buonomo
Andrea Pollesel
Andrea Cester
Massimo Zambianchi
Manuela Melucci
Michele Muccini
Stefano Toffanin
Abstract
Organic field-effect transistors (OFETs) are considered almost purely interfacial devices with charge current mainly confined in the first two semiconducting layers in contact with the dielectric with no active role of the film thickness exceeding six to eight monolayers (MLs). By a combined electronic, morphological, structural, and theoretical investigation, it is demonstrated that the charge mobility and source–drain current in 2,20-(2,20-bithiophene-5,50-diyl)bis(5-butyl-5H-thieno[2,3-c]pyrrole-4,6)-dione (NT4N) organic transistors directly correlate with the out-of-plane domain size and crystallite orientation in the vertical direction, well beyond the dielectric interfacial layers. Polycrystalline films with thickness as high as 75 nm (≈30 MLs) and 3D molecular architecture provide the best electrical and optoelectronic OFET characteristics, highlighting that the molecular orientational order in the bulk of the film is the key-enabling factor for optimum device performance. X-ray scattering analysis and multiscale simulations reveal the functional correlation between the thickness-dependent molecular packing, electron mobility, and vertical charge distribution. These results call for a broader view of the fundamental mechanisms that govern field-effect charge transport in OFETs beyond the interfacial 2D paradigm and demonstrate the unexpected role of the out-of-plane domain size and crystallite orientation in polycrystalline films to achieve optimum electronic and optoelectronic properties in organic transistors.
Citation
Benvenuti, E., Portale, G., Brucale, M., Quiroga, S. D., Baldoni, M., MacKenzie, R. C., Mercuri, F., Canola, S., Negri, F., Lago, N., Buonomo, M., Pollesel, A., Cester, A., Zambianchi, M., Melucci, M., Muccini, M., & Toffanin, S. (2023). Beyond the 2D Field‐Effect Charge Transport Paradigm in Molecular Thin‐Film Transistors. Advanced Electronic Materials, 9(1), Article 2200547. https://doi.org/10.1002/aelm.202200547
Journal Article Type | Article |
---|---|
Online Publication Date | Aug 15, 2022 |
Publication Date | 2023-01 |
Deposit Date | Aug 25, 2022 |
Publicly Available Date | Mar 15, 2023 |
Journal | Advanced Electronic Materials |
Electronic ISSN | 2199-160X |
Publisher | Wiley |
Peer Reviewed | Peer Reviewed |
Volume | 9 |
Issue | 1 |
Article Number | 2200547 |
DOI | https://doi.org/10.1002/aelm.202200547 |
Public URL | https://durham-repository.worktribe.com/output/1193617 |
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Copyright Statement
© 2022 The Authors. Advanced Electronic Materials published by Wiley-VCH GmbH
This is an open access article under the terms of the Creative Commons Attribution License, which permits use, distribution and reproduction in any medium, provided the original work is properly cited.
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