Beyond the 2D Field‐Effect Charge Transport Paradigm in Molecular Thin‐Film Transistors
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 combine...
| Main Authors: | , , , , , , , , , , , , , , , , |
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| Format: | Article |
| Language: | English |
| Published: |
Wiley-VCH
2023-01-01
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| Series: | Advanced Electronic Materials |
| Subjects: | |
| Online Access: | https://doi.org/10.1002/aelm.202200547 |
| _version_ | 1827893400613945344 |
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| author | Emilia Benvenuti Giuseppe Portale Marco Brucale Santiago D. Quiroga Matteo Baldoni Roderick C. I. MacKenzie Francesco Mercuri Sofia Canola Fabrizia Negri Nicolò Lago Marco Buonomo Andrea Pollesel Andrea Cester Massimo Zambianchi Manuela Melucci Michele Muccini Stefano Toffanin |
| author_facet | Emilia Benvenuti Giuseppe Portale Marco Brucale Santiago D. Quiroga Matteo Baldoni Roderick C. I. MacKenzie Francesco Mercuri Sofia Canola Fabrizia Negri Nicolò Lago Marco Buonomo Andrea Pollesel Andrea Cester Massimo Zambianchi Manuela Melucci Michele Muccini Stefano Toffanin |
| author_sort | Emilia Benvenuti |
| collection | DOAJ |
| description | 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. |
| first_indexed | 2024-03-12T21:52:36Z |
| format | Article |
| id | doaj.art-d3ba214447104bbb8ee043ca4764f43b |
| institution | Directory Open Access Journal |
| issn | 2199-160X |
| language | English |
| last_indexed | 2024-03-12T21:52:36Z |
| publishDate | 2023-01-01 |
| publisher | Wiley-VCH |
| record_format | Article |
| series | Advanced Electronic Materials |
| spelling | doaj.art-d3ba214447104bbb8ee043ca4764f43b2023-07-26T01:35:51ZengWiley-VCHAdvanced Electronic Materials2199-160X2023-01-0191n/an/a10.1002/aelm.202200547Beyond the 2D Field‐Effect Charge Transport Paradigm in Molecular Thin‐Film TransistorsEmilia Benvenuti0Giuseppe Portale1Marco Brucale2Santiago D. Quiroga3Matteo Baldoni4Roderick C. I. MacKenzie5Francesco Mercuri6Sofia Canola7Fabrizia Negri8Nicolò Lago9Marco Buonomo10Andrea Pollesel11Andrea Cester12Massimo Zambianchi13Manuela Melucci14Michele Muccini15Stefano Toffanin16Istituto per lo Studio dei Materiali Nanostrutturati Consiglio Nazionale delle Ricerche (CNR‐ISMN) Via Gobetti 101 Bologna 40129 ItalyZernike Institute for Advanced Materials Micromechanics University of Groningen Nijenborgh 4 Groningen 9747AG The NetherlandsIstituto per lo Studio dei Materiali Nanostrutturati Consiglio Nazionale delle Ricerche (CNR‐ISMN) Via Gobetti 101 Bologna 40129 ItalyIstituto per lo Studio dei Materiali Nanostrutturati Consiglio Nazionale delle Ricerche (CNR‐ISMN) Via Gobetti 101 Bologna 40129 ItalyIstituto per lo Studio dei Materiali Nanostrutturati Consiglio Nazionale delle Ricerche (CNR‐ISMN) Via Gobetti 101 Bologna 40129 ItalyDepartment of Engineering Durham University Lower Mount Joy South Road Durham DH1 3LE UKIstituto per lo Studio dei Materiali Nanostrutturati Consiglio Nazionale delle Ricerche (CNR‐ISMN) Via Gobetti 101 Bologna 40129 ItalyDipartimento di Chimica “Giacomo Ciamician,” Università di Bologna Italy and INSTM UdR Bologna Via F. Selmi 2 Bologna 40126 ItalyDipartimento di Chimica “Giacomo Ciamician,” Università di Bologna Italy and INSTM UdR Bologna Via F. Selmi 2 Bologna 40126 ItalyDipartimento di Ingegneria dell'Informazione Università di Padova Via Gradenigo 6B Padova 35131 ItalyDipartimento di Ingegneria dell'Informazione Università di Padova Via Gradenigo 6B Padova 35131 ItalyDipartimento di Ingegneria dell'Informazione Università di Padova Via Gradenigo 6B Padova 35131 ItalyDipartimento di Ingegneria dell'Informazione Università di Padova Via Gradenigo 6B Padova 35131 ItalyIstituto per la Sintesi Organica e la Fotoreattività Consiglio Nazionale delle Ricerche (CNR‐ISOF) Via Gobetti 101 Bologna 40129 ItalyIstituto per la Sintesi Organica e la Fotoreattività Consiglio Nazionale delle Ricerche (CNR‐ISOF) Via Gobetti 101 Bologna 40129 ItalyIstituto per lo Studio dei Materiali Nanostrutturati Consiglio Nazionale delle Ricerche (CNR‐ISMN) Via Gobetti 101 Bologna 40129 ItalyIstituto per lo Studio dei Materiali Nanostrutturati Consiglio Nazionale delle Ricerche (CNR‐ISMN) Via Gobetti 101 Bologna 40129 ItalyAbstract 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.https://doi.org/10.1002/aelm.202200547charge transportcrystallite orientationoligothiophenesorganic field‐effect transistorsout‐of‐plane crystalline domains |
| spellingShingle | Emilia Benvenuti Giuseppe Portale Marco Brucale Santiago D. Quiroga Matteo Baldoni Roderick C. I. MacKenzie Francesco Mercuri Sofia Canola Fabrizia Negri Nicolò Lago Marco Buonomo Andrea Pollesel Andrea Cester Massimo Zambianchi Manuela Melucci Michele Muccini Stefano Toffanin Beyond the 2D Field‐Effect Charge Transport Paradigm in Molecular Thin‐Film Transistors Advanced Electronic Materials charge transport crystallite orientation oligothiophenes organic field‐effect transistors out‐of‐plane crystalline domains |
| title | Beyond the 2D Field‐Effect Charge Transport Paradigm in Molecular Thin‐Film Transistors |
| title_full | Beyond the 2D Field‐Effect Charge Transport Paradigm in Molecular Thin‐Film Transistors |
| title_fullStr | Beyond the 2D Field‐Effect Charge Transport Paradigm in Molecular Thin‐Film Transistors |
| title_full_unstemmed | Beyond the 2D Field‐Effect Charge Transport Paradigm in Molecular Thin‐Film Transistors |
| title_short | Beyond the 2D Field‐Effect Charge Transport Paradigm in Molecular Thin‐Film Transistors |
| title_sort | beyond the 2d field effect charge transport paradigm in molecular thin film transistors |
| topic | charge transport crystallite orientation oligothiophenes organic field‐effect transistors out‐of‐plane crystalline domains |
| url | https://doi.org/10.1002/aelm.202200547 |
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