Controlling the Entropy of a Single-Molecule Junction

Eugenia Pyurbeeva; Chunwei Hsu; David Vogel; Christina Wegeberg; Marcel Mayor; Herre Van Der Zant; Jan A. Mol; Pascal Gehring

doi:10.1021/acs.nanolett.1c03591

Controlling the Entropy of a Single-Molecule Junction

Eugenia Pyurbeeva, Chunwei Hsu, David Vogel, Christina Wegeberg, Marcel Mayor, Herre Van Der Zant, Jan A. Mol^*, Pascal Gehring

^*Corresponding author for this work

QN/van der Zant Lab

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

6 Citations (Scopus)

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Abstract

Single molecules are nanoscale thermodynamic systems with few degrees of freedom. Thus, the knowledge of their entropy can reveal the presence of microscopic electron transfer dynamics that are difficult to observe otherwise. Here, we apply thermocurrent spectroscopy to directly measure the entropy of a single free radical molecule in a magnetic field. Our results allow us to uncover the presence of a singlet to triplet transition in one of the redox states of the molecule, not detected by conventional charge transport measurements. This highlights the power of thermoelectric measurements which can be used to determine the difference in configurational entropy between the redox states of a nanoscale system involved in conductance without any prior assumptions about its structure or microscopic dynamics.

Original language	English
Pages (from-to)	9715-9719
Journal	Nano Letters
Volume	21
Issue number	22
DOIs	https://doi.org/10.1021/acs.nanolett.1c03591
Publication status	Published - 2021

Bibliographical note

Green Open Access added to TU Delft Institutional Repository ‘You share, we take care!’ – Taverne project https://www.openaccess.nl/en/you-share-we-take-care Otherwise as indicated in the copyright section: the publisher is the copyright holder of this work and the author uses the Dutch legislation to make this work public.

Keywords

Molecular electronics
entropy
molecular thermoelectrics
quantum thermodynamics
thermocurrent spectroscopy

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10.1021/acs.nanolett.1c03591

acs.nanolett.1c03591Final published version, 970 KB

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title = "Controlling the Entropy of a Single-Molecule Junction",

abstract = "Single molecules are nanoscale thermodynamic systems with few degrees of freedom. Thus, the knowledge of their entropy can reveal the presence of microscopic electron transfer dynamics that are difficult to observe otherwise. Here, we apply thermocurrent spectroscopy to directly measure the entropy of a single free radical molecule in a magnetic field. Our results allow us to uncover the presence of a singlet to triplet transition in one of the redox states of the molecule, not detected by conventional charge transport measurements. This highlights the power of thermoelectric measurements which can be used to determine the difference in configurational entropy between the redox states of a nanoscale system involved in conductance without any prior assumptions about its structure or microscopic dynamics.",

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author = "Eugenia Pyurbeeva and Chunwei Hsu and David Vogel and Christina Wegeberg and Marcel Mayor and Zant, {Herre Van Der} and Mol, {Jan A.} and Pascal Gehring",

note = "Green Open Access added to TU Delft Institutional Repository {\textquoteleft}You share, we take care!{\textquoteright} – Taverne project https://www.openaccess.nl/en/you-share-we-take-care Otherwise as indicated in the copyright section: the publisher is the copyright holder of this work and the author uses the Dutch legislation to make this work public. ",

year = "2021",

doi = "10.1021/acs.nanolett.1c03591",

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AU - Pyurbeeva, Eugenia

AU - Hsu, Chunwei

AU - Vogel, David

AU - Wegeberg, Christina

AU - Mayor, Marcel

AU - Zant, Herre Van Der

AU - Mol, Jan A.

AU - Gehring, Pascal

N1 - Green Open Access added to TU Delft Institutional Repository ‘You share, we take care!’ – Taverne project https://www.openaccess.nl/en/you-share-we-take-care Otherwise as indicated in the copyright section: the publisher is the copyright holder of this work and the author uses the Dutch legislation to make this work public.

PY - 2021

Y1 - 2021

N2 - Single molecules are nanoscale thermodynamic systems with few degrees of freedom. Thus, the knowledge of their entropy can reveal the presence of microscopic electron transfer dynamics that are difficult to observe otherwise. Here, we apply thermocurrent spectroscopy to directly measure the entropy of a single free radical molecule in a magnetic field. Our results allow us to uncover the presence of a singlet to triplet transition in one of the redox states of the molecule, not detected by conventional charge transport measurements. This highlights the power of thermoelectric measurements which can be used to determine the difference in configurational entropy between the redox states of a nanoscale system involved in conductance without any prior assumptions about its structure or microscopic dynamics.

AB - Single molecules are nanoscale thermodynamic systems with few degrees of freedom. Thus, the knowledge of their entropy can reveal the presence of microscopic electron transfer dynamics that are difficult to observe otherwise. Here, we apply thermocurrent spectroscopy to directly measure the entropy of a single free radical molecule in a magnetic field. Our results allow us to uncover the presence of a singlet to triplet transition in one of the redox states of the molecule, not detected by conventional charge transport measurements. This highlights the power of thermoelectric measurements which can be used to determine the difference in configurational entropy between the redox states of a nanoscale system involved in conductance without any prior assumptions about its structure or microscopic dynamics.

KW - Molecular electronics

KW - entropy

KW - molecular thermoelectrics

KW - quantum thermodynamics

KW - thermocurrent spectroscopy

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SP - 9715

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JO - Nano Letters

JF - Nano Letters

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ER -

Controlling the Entropy of a Single-Molecule Junction

Abstract

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Thermoelectricity in single-molecule quantum dots

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Controlling the Entropy of a Single-Molecule Junction

Abstract

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Activities

Thermoelectricity in single-molecule quantum dots

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