High Seebeck Coefficient Achieved by Multinuclear Organometallic Molecular Junctions

Sohyun Park; Jiung Jang; Yuya Tanaka; Hyo Jae Yoon

doi:10.1021/acs.nanolett.2c03974

High Seebeck Coefficient Achieved by Multinuclear Organometallic Molecular Junctions

Sohyun Park, Jiung Jang, Yuya Tanaka, Hyo Jae Yoon

Department of Chemistry

Research output: Contribution to journal › Article › peer-review

6 Citations (Scopus)

Abstract

This paper describes the thermoelectric properties of molecular junctions incorporating multinuclear ruthenium alkynyl complexes that comprise Ru(dppe)₂[dppe = 1,2-bis(diphenylphosphino)ethane] fragments and diethylnyl aromatic bridging ligands with thioether anchors. Using the liquid metal technique, the Seebeck coefficient was examined as a function of metal nuclearity, oxidation state, and substituent on the organic ligand backbone. High Seebeck coefficients up to 73 μV/K and appreciable thermal stability with thermovoltage up to ∼3.3 mV at a heating temperature of 423 K were observed. An unusually high proximity of the highest occupied molecular orbital (HOMO) energy level to the Fermi level was revealed to give the remarkable thermoelectric performance as suggested by combined experiments and calculations. This work offers important insights into the development of molecular-scale devices for efficient thermoregulation and heat-to-electricity conversion.

Original language	English
Pages (from-to)	9693-9699
Number of pages	7
Journal	Nano Letters
Volume	22
Issue number	23
DOIs	https://doi.org/10.1021/acs.nanolett.2c03974
Publication status	Published - 2022 Dec 14

Bibliographical note

Funding Information:
This research was supported by the NRF of Korea (NRF-2019R1A2C2011003, NRF-2019R1A6A1A11044070, NRF-2021M3F3A2A03017999, and NRF-2019K2A9A2A08000151). S.P. acknowledges the support of the POSCO TJ Park Doctoral Fellowship. The authors are grateful for the NMR facility in the Institute for Basic Science (IBS) Center for Molecular Spectroscopy and Dynamics. Y.T. acknowledge a research grant from JSPS KAKENHI (21K05211) and The Murata Science Foundation. The computations were performed by using the computer in the Research Center for Computational Science, Okazaki, Japan (21-IMS-C071, 22-IMS-C071).

Publisher Copyright:
© 2022 American Chemical Society. All rights reserved.

Keywords

metal alkynyl
molecular junction
organometallic
Seebeck coefficient
thermopower

ASJC Scopus subject areas

Bioengineering
Chemistry(all)
Materials Science(all)
Condensed Matter Physics
Mechanical Engineering

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10.1021/acs.nanolett.2c03974

Cite this

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title = "High Seebeck Coefficient Achieved by Multinuclear Organometallic Molecular Junctions",

abstract = "This paper describes the thermoelectric properties of molecular junctions incorporating multinuclear ruthenium alkynyl complexes that comprise Ru(dppe)2[dppe = 1,2-bis(diphenylphosphino)ethane] fragments and diethylnyl aromatic bridging ligands with thioether anchors. Using the liquid metal technique, the Seebeck coefficient was examined as a function of metal nuclearity, oxidation state, and substituent on the organic ligand backbone. High Seebeck coefficients up to 73 μV/K and appreciable thermal stability with thermovoltage up to ∼3.3 mV at a heating temperature of 423 K were observed. An unusually high proximity of the highest occupied molecular orbital (HOMO) energy level to the Fermi level was revealed to give the remarkable thermoelectric performance as suggested by combined experiments and calculations. This work offers important insights into the development of molecular-scale devices for efficient thermoregulation and heat-to-electricity conversion.",

keywords = "metal alkynyl, molecular junction, organometallic, Seebeck coefficient, thermopower",

author = "Sohyun Park and Jiung Jang and Yuya Tanaka and Yoon, {Hyo Jae}",

note = "Funding Information: This research was supported by the NRF of Korea (NRF-2019R1A2C2011003, NRF-2019R1A6A1A11044070, NRF-2021M3F3A2A03017999, and NRF-2019K2A9A2A08000151). S.P. acknowledges the support of the POSCO TJ Park Doctoral Fellowship. The authors are grateful for the NMR facility in the Institute for Basic Science (IBS) Center for Molecular Spectroscopy and Dynamics. Y.T. acknowledge a research grant from JSPS KAKENHI (21K05211) and The Murata Science Foundation. The computations were performed by using the computer in the Research Center for Computational Science, Okazaki, Japan (21-IMS-C071, 22-IMS-C071). Publisher Copyright: {\textcopyright} 2022 American Chemical Society. All rights reserved.",

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doi = "10.1021/acs.nanolett.2c03974",

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AU - Park, Sohyun

AU - Jang, Jiung

AU - Tanaka, Yuya

AU - Yoon, Hyo Jae

N1 - Funding Information: This research was supported by the NRF of Korea (NRF-2019R1A2C2011003, NRF-2019R1A6A1A11044070, NRF-2021M3F3A2A03017999, and NRF-2019K2A9A2A08000151). S.P. acknowledges the support of the POSCO TJ Park Doctoral Fellowship. The authors are grateful for the NMR facility in the Institute for Basic Science (IBS) Center for Molecular Spectroscopy and Dynamics. Y.T. acknowledge a research grant from JSPS KAKENHI (21K05211) and The Murata Science Foundation. The computations were performed by using the computer in the Research Center for Computational Science, Okazaki, Japan (21-IMS-C071, 22-IMS-C071). Publisher Copyright: © 2022 American Chemical Society. All rights reserved.

PY - 2022/12/14

Y1 - 2022/12/14

N2 - This paper describes the thermoelectric properties of molecular junctions incorporating multinuclear ruthenium alkynyl complexes that comprise Ru(dppe)2[dppe = 1,2-bis(diphenylphosphino)ethane] fragments and diethylnyl aromatic bridging ligands with thioether anchors. Using the liquid metal technique, the Seebeck coefficient was examined as a function of metal nuclearity, oxidation state, and substituent on the organic ligand backbone. High Seebeck coefficients up to 73 μV/K and appreciable thermal stability with thermovoltage up to ∼3.3 mV at a heating temperature of 423 K were observed. An unusually high proximity of the highest occupied molecular orbital (HOMO) energy level to the Fermi level was revealed to give the remarkable thermoelectric performance as suggested by combined experiments and calculations. This work offers important insights into the development of molecular-scale devices for efficient thermoregulation and heat-to-electricity conversion.

AB - This paper describes the thermoelectric properties of molecular junctions incorporating multinuclear ruthenium alkynyl complexes that comprise Ru(dppe)2[dppe = 1,2-bis(diphenylphosphino)ethane] fragments and diethylnyl aromatic bridging ligands with thioether anchors. Using the liquid metal technique, the Seebeck coefficient was examined as a function of metal nuclearity, oxidation state, and substituent on the organic ligand backbone. High Seebeck coefficients up to 73 μV/K and appreciable thermal stability with thermovoltage up to ∼3.3 mV at a heating temperature of 423 K were observed. An unusually high proximity of the highest occupied molecular orbital (HOMO) energy level to the Fermi level was revealed to give the remarkable thermoelectric performance as suggested by combined experiments and calculations. This work offers important insights into the development of molecular-scale devices for efficient thermoregulation and heat-to-electricity conversion.

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KW - organometallic

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ER -

High Seebeck Coefficient Achieved by Multinuclear Organometallic Molecular Junctions

Abstract

Bibliographical note

Keywords

ASJC Scopus subject areas

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