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Nano Research 2024, 17(5): 4573-4581 https://doi.org/10.1007/s12274-023-6252-3
Research Article | Issue | Published: 02 December 2023

Molecule-based vertical transistor via intermolecular charge transport through π-π stacking

Show Author's Information Cheng Liu1,§,  Cheng Fu1,2,§,  Lingyu Tang1,  Jianghua Wu3,  Zhangyan Mu1,  Yamei Sun1,  Yanghang Pan1,  Bailin Tian1,  Kai Bao4,  Jing Ma1,2( ),  Qiyuan He4( ),  Mengning Ding1( )
Key Laboratory of Mesoscopic Chemistry, School of Chemistry and Chemical Engineering, Nanjing University, Nanjing 210023, China
Jiangsu Key Laboratory of Advanced Organic Materials, School of Chemistry and Chemical Engineering, Nanjing University, Nanjing 210023, China
National Laboratory of Solid State Microstructures, Jiangsu Key Laboratory of Artificial Functional Materials, College of Engineering and Applied Sciences, Collaborative Innovation Center of Advanced Microstructures, Nanjing University, Nanjing 210093, China
Department of Materials Science and Engineering, City University of Hong Kong, Hong Kong 999077, China

§ Cheng Liu and Cheng Fu contributed equally to this work.

Keywords:
electrical transport, electrochemical intercalation, organic semiconductor, tunneling field effect transistor, π-π stacking
Topics:
Semiconductor device manufacture
Cite this article:
Liu C, Fu C, Tang L, et al. Molecule-based vertical transistor via intermolecular charge transport through π-π stacking. Nano Research, 2024, 17(5): 4573-4581. https://doi.org/10.1007/s12274-023-6252-3
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Abstract Full text Electronic supplementary material About this article

The π-π stacking is a well-recognized intermolecular interaction that is responsible for the construction of electron hopping channels in numerous conducting frameworks/aggregates. However, the exact role of π-to-π channels within typical single crystalline organic semiconductors remains unclear as the orientations of these molecules are diverse, and their control usually requires additional side chain groups that misrepresent the intrinsic properties of the original semiconducting molecules. Therefore, the construction of conduction channels with intrinsic π-π stacking in the molecule-based device is crucial for the utilization of their unique transport characteristics and understanding of the transport mechanism. To this end, we present a molecular intercalation strategy that integrates two-dimensional layered materials with functional organic semiconductor molecules for functional molecule-based electronics. Various organic semiconductor molecules can be effectively intercalated into the van der Waals gaps of semi-metallic TaS2 with π-π stacking configuration and controlled intercalant content. Our results show that the vertical charge transport in the stacking direction shows a tunneling-dominated mechanism that strongly depends on the molecular structures. Furthermore, we demonstrated a new type of molecule-based vertical transistor in which TaS2 and π-π stacked organic molecules function as the electrical contact and the active channel, respectively. On/off ratios as high as 447 are achieved under electrostatic modulation in ionic liquid, comparable to the current state-of-the-art molecular transistors. Our study provides an ideal platform for probing intrinsic charge transport across π-π stacked conjugated molecules and also a feasible approach for the construction of high-performance molecule-based electronic devices.


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Electronic supplementary material
About this article

Molecule-based vertical transistor via intermolecular charge transport through π-π stacking

Show Author's information Cheng Liu1,§, Cheng Fu1,2,§, Lingyu Tang1, Jianghua Wu3, Zhangyan Mu1, Yamei Sun1, Yanghang Pan1, Bailin Tian1, Kai Bao4, Jing Ma1,2( ), Qiyuan He4( ), Mengning Ding1( )
Key Laboratory of Mesoscopic Chemistry, School of Chemistry and Chemical Engineering, Nanjing University, Nanjing 210023, China
Jiangsu Key Laboratory of Advanced Organic Materials, School of Chemistry and Chemical Engineering, Nanjing University, Nanjing 210023, China
National Laboratory of Solid State Microstructures, Jiangsu Key Laboratory of Artificial Functional Materials, College of Engineering and Applied Sciences, Collaborative Innovation Center of Advanced Microstructures, Nanjing University, Nanjing 210093, China
Department of Materials Science and Engineering, City University of Hong Kong, Hong Kong 999077, China

§ Cheng Liu and Cheng Fu contributed equally to this work.

Abstract

The π-π stacking is a well-recognized intermolecular interaction that is responsible for the construction of electron hopping channels in numerous conducting frameworks/aggregates. However, the exact role of π-to-π channels within typical single crystalline organic semiconductors remains unclear as the orientations of these molecules are diverse, and their control usually requires additional side chain groups that misrepresent the intrinsic properties of the original semiconducting molecules. Therefore, the construction of conduction channels with intrinsic π-π stacking in the molecule-based device is crucial for the utilization of their unique transport characteristics and understanding of the transport mechanism. To this end, we present a molecular intercalation strategy that integrates two-dimensional layered materials with functional organic semiconductor molecules for functional molecule-based electronics. Various organic semiconductor molecules can be effectively intercalated into the van der Waals gaps of semi-metallic TaS2 with π-π stacking configuration and controlled intercalant content. Our results show that the vertical charge transport in the stacking direction shows a tunneling-dominated mechanism that strongly depends on the molecular structures. Furthermore, we demonstrated a new type of molecule-based vertical transistor in which TaS2 and π-π stacked organic molecules function as the electrical contact and the active channel, respectively. On/off ratios as high as 447 are achieved under electrostatic modulation in ionic liquid, comparable to the current state-of-the-art molecular transistors. Our study provides an ideal platform for probing intrinsic charge transport across π-π stacked conjugated molecules and also a feasible approach for the construction of high-performance molecule-based electronic devices.

Keywords: electrical transport, electrochemical intercalation, organic semiconductor, tunneling field effect transistor, π-π stacking

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Publication history
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Acknowledgements

Publication history

Received: 11 August 2023
Revised: 27 September 2023
Accepted: 07 October 2023
Published: 02 December 2023
Issue date: May 2024

Copyright

© Tsinghua University Press 2023

Acknowledgements

Acknowledgements

M. N. D. acknowledges the support by the National Natural Science Foundation of China (Nos. 22172075 and 92156024), the Fundamental Research Funds for the Central Universities in China (Nos. 0210/14380174 and 14380273), Beijing National Laboratory for Molecular Sciences (No. BNLMS202107), and Thousand Talents Plan of Jiangxi Province (No. jxsq2019102002). J. M. acknowledges the support by the National Natural Science Foundation of China (No. 22033004). Q. Y. H. acknowledges support from Early Career Scheme Project (No. 21302821) and General Research Fund Project (No. 11314322) from the University Grants Committee of Hong Kong.

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