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Thermal and Thermoelectric Properties of SAM-Based Molecular Junctions

Cite this: ACS Appl. Mater. Interfaces 2022, 14, 20, 22818–22825
Publication Date (Web):December 27, 2021
https://doi.org/10.1021/acsami.1c20840
Copyright © 2021 American Chemical Society

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    Abstract

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    In molecular thermoelectrics, the thermopower of molecular junctions is closely interlinked with their thermal properties; however, the detailed relationship between them remains uncertain. This study systematically investigates the thermal properties of self-assembled monolayer (SAM)-based molecular junctions and relates them to the thermoelectric performance of the junctions. The electrode temperatures for the bare AuTS, AuTS/EGaIn, and AuTS/TPT SAM//Ga2O3/EGaIn samples placed on a hot chuck were measured under different conditions, such as air vs vacuum and the presence and absence of thermal grease, which generates a heat conduction channel from a hot chuck to gold. It was revealed that the SAM was the most efficient thermal resistor, which was responsible for the creation of a temperature differential (ΔT) across the junction; ΔT in an air atmosphere is overestimated to some extent, and air mainly contributes to large dispersions of thermovoltage (ΔV) data. While junction measurements in air were possible at low ΔT (up to 13 K), the new optimal condition, under a vacuum and with thermal grease, allowed us to examine a wide temperature range up to ΔT = 40 K and obtain a more reliable Seebeck coefficient (S, μV/K). The value of S under the new condition was ∼1.4 times higher than that measured in air without thermal grease. Our study shows the potential of liquid-metal-based junctions to reliably investigate heat conduction across nanometer-thick organic films and elaborates on how the thermal properties of molecular junctions affect their thermoelectric performance.

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acsami.1c20840.

    • Summary of thermoelectric measurements over AuTS/TPT//Ga2O3/EGaIn under a vacuum with grease 2; thermoresponse data of bare AuAD substrate (PDF)

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    Cited By

    This article is cited by 8 publications.

    1. Peng He, Abdalghani H. S. Daaoub, Sara Sangtarash, Hatef Sadeghi, Hyo Jae Yoon. Thermopower in Underpotential Deposition-Based Molecular Junctions. Nano Letters 2024, 24 (6) , 1988-1995. https://doi.org/10.1021/acs.nanolett.3c04438
    2. Saurabh Soni, Irina Werner, Michael Aidi, Marco Moors, C. Lungani Mthembu, Michael Zharnikov, Remco W. A. Havenith, Kirill Yu. Monakhov, Ryan C. Chiechi. Influence of Polyoxovanadate and Phthalocyanine on 4f Electron Transfer in Gold-Confined Monolayers Probed with EGaIn Top Contacts. ACS Applied Nano Materials 2023, 6 (24) , 22643-22650. https://doi.org/10.1021/acsanm.3c05021
    3. Jiung Jang, Peng He, Hyo Jae Yoon. Molecular Thermoelectricity in EGaIn-Based Molecular Junctions. Accounts of Chemical Research 2023, 56 (12) , 1613-1622. https://doi.org/10.1021/acs.accounts.3c00168
    4. Sohyun Park, Jiung Jang, Yuya Tanaka, Hyo Jae Yoon. High Seebeck Coefficient Achieved by Multinuclear Organometallic Molecular Junctions. Nano Letters 2022, 22 (23) , 9693-9699. https://doi.org/10.1021/acs.nanolett.2c03974
    5. Sohyun Park, Jeong Woo Jo, Jiung Jang, Tatsuhiko Ohto, Hirokazu Tada, Hyo Jae Yoon. Thermopower in Transition from Tunneling to Hopping. Nano Letters 2022, 22 (18) , 7682-7689. https://doi.org/10.1021/acs.nanolett.2c03083
    6. Sohyun Park, Seohyun Kang, Hyo Jae Yoon. Thermopower of Molecular Junction in Harsh Thermal Environments. Nano Letters 2022, 22 (10) , 3953-3960. https://doi.org/10.1021/acs.nanolett.2c00422
    7. Jinlong He, Lei Tao, Weikang Xian, Tom Arbaugh, Ying Li. Molecular self-assembled monolayers anomalously enhance thermal conductance across polymer–semiconductor interfaces. Nanoscale 2022, 14 (47) , 17681-17693. https://doi.org/10.1039/D2NR04936H
    8. Enyang Liu, Lei Lei, Renguang Ye, Degang Deng, Shiqing Xu. Improved relative temperature sensitivity of over 10% K −1 in fluoride nanocrystals via engineering the interfacial layer. Chemical Communications 2022, 58 (65) , 9076-9079. https://doi.org/10.1039/D2CC02548E

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