Quantum Interference and Contact Effects in the Thermoelectric Performance of Anthracene-Based Molecules

Joseph Hamill; Ali Ismael; Alaa Al-Jobory; Troy L R Bennett; Maryam Alshahrani; Xintai  Wang; Maxwell Akers-Douglas; Luke Alexander Wilkinson; Benjamin J Robinson; Nicholas Long; Colin  Lambert; Tim Albrecht

doi:10.1021/acs.jpcc.3c00069

Quantum Interference and Contact Effects in the Thermoelectric Performance of Anthracene-Based Molecules

Joseph Hamill^*, Ali Ismael^*, Alaa Al-Jobory, Troy L R Bennett, Maryam Alshahrani, Xintai Wang, Maxwell Akers-Douglas, Luke Alexander Wilkinson, Benjamin J Robinson, Nicholas Long, Colin Lambert^*, Tim Albrecht^*

^*Corresponding author for this work

Chemistry

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

Abstract

We report on the single-molecule electronic and thermoelectric properties of strategically chosen anthracene-based molecules with anchor groups capable of binding to noble metal substrates, such as gold and platinum. Specifically, we study the effect of different anchor groups, as well as quantum interference, on the electric conductance and the thermopower of gold/single-molecule/gold junctions and generally find good agreement between theory and experiments. All molecular junctions display transport characteristics consistent with coherent transport and a Fermi alignment approximately in the middle of the highest occupied molecular orbital/lowest unoccupied molecular orbital gap. Single-molecule results are in agreement with previously reported thin-film data, further supporting the notion that molecular design considerations may be translated from the single- to many-molecule devices. For combinations of anchor groups where one binds significantly more strongly to the electrodes than the other, the stronger anchor group appears to dominate the thermoelectric behavior of the molecular junction. For other combinations, the choice of electrode material can determine the sign and magnitude of the thermopower. This finding has important implications for the design of thermoelectric generator devices, where both n- and p-type conductors are required for thermoelectric current generation.

Original language	English
Number of pages	8
Journal	Journal of Physical Chemistry C
Early online date	10 Apr 2023
DOIs	https://doi.org/10.1021/acs.jpcc.3c00069
Publication status	E-pub ahead of print - 10 Apr 2023

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10.1021/acs.jpcc.3c00069Licence: CC BY

Quantum Interference and Contact Effects in the Thermoelectric Performance of Anthracene-Based Molecules
© 2023 The Authors.
Final published version, 2 MBLicence: CC BY

Cite this

Hamill, J., Ismael, A., Al-Jobory, A., Bennett, T. L. R., Alshahrani, M., Wang, X., Akers-Douglas, M., Wilkinson, L. A., Robinson, B. J., Long, N., Lambert, C., & Albrecht, T. (2023). Quantum Interference and Contact Effects in the Thermoelectric Performance of Anthracene-Based Molecules. Journal of Physical Chemistry C. Advance online publication. https://doi.org/10.1021/acs.jpcc.3c00069

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title = "Quantum Interference and Contact Effects in the Thermoelectric Performance of Anthracene-Based Molecules",

abstract = "We report on the single-molecule electronic and thermoelectric properties of strategically chosen anthracene-based molecules with anchor groups capable of binding to noble metal substrates, such as gold and platinum. Specifically, we study the effect of different anchor groups, as well as quantum interference, on the electric conductance and the thermopower of gold/single-molecule/gold junctions and generally find good agreement between theory and experiments. All molecular junctions display transport characteristics consistent with coherent transport and a Fermi alignment approximately in the middle of the highest occupied molecular orbital/lowest unoccupied molecular orbital gap. Single-molecule results are in agreement with previously reported thin-film data, further supporting the notion that molecular design considerations may be translated from the single- to many-molecule devices. For combinations of anchor groups where one binds significantly more strongly to the electrodes than the other, the stronger anchor group appears to dominate the thermoelectric behavior of the molecular junction. For other combinations, the choice of electrode material can determine the sign and magnitude of the thermopower. This finding has important implications for the design of thermoelectric generator devices, where both n- and p-type conductors are required for thermoelectric current generation.",

author = "Joseph Hamill and Ali Ismael and Alaa Al-Jobory and Bennett, {Troy L R} and Maryam Alshahrani and Xintai Wang and Maxwell Akers-Douglas and Wilkinson, {Luke Alexander} and Robinson, {Benjamin J} and Nicholas Long and Colin Lambert and Tim Albrecht",

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AU - Alshahrani, Maryam

AU - Wang, Xintai

AU - Akers-Douglas, Maxwell

AU - Wilkinson, Luke Alexander

AU - Robinson, Benjamin J

AU - Long, Nicholas

AU - Lambert, Colin

AU - Albrecht, Tim

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N2 - We report on the single-molecule electronic and thermoelectric properties of strategically chosen anthracene-based molecules with anchor groups capable of binding to noble metal substrates, such as gold and platinum. Specifically, we study the effect of different anchor groups, as well as quantum interference, on the electric conductance and the thermopower of gold/single-molecule/gold junctions and generally find good agreement between theory and experiments. All molecular junctions display transport characteristics consistent with coherent transport and a Fermi alignment approximately in the middle of the highest occupied molecular orbital/lowest unoccupied molecular orbital gap. Single-molecule results are in agreement with previously reported thin-film data, further supporting the notion that molecular design considerations may be translated from the single- to many-molecule devices. For combinations of anchor groups where one binds significantly more strongly to the electrodes than the other, the stronger anchor group appears to dominate the thermoelectric behavior of the molecular junction. For other combinations, the choice of electrode material can determine the sign and magnitude of the thermopower. This finding has important implications for the design of thermoelectric generator devices, where both n- and p-type conductors are required for thermoelectric current generation.

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