An enhanced Coulomb blockade description of single-molecule junctions through complex polarizabilities

Michala D. Jensen; Ellen T. Ekstrøm; Zacharias Liasi; Kurt V. Mikkelsen

doi:10.1016/j.cplett.2025.141958

An enhanced Coulomb blockade description of single-molecule junctions through complex polarizabilities

Michala D. Jensen, Ellen T. Ekstrøm, Zacharias Liasi, Kurt V. Mikkelsen^*

^*Corresponding author for this work

University of Copenhagen

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Abstract

Single-molecule junctions offer a framework for exploring charge transport mechanisms under nonequilibrium conditions. Accurate descriptions are essential, yet challenging, due to the dynamic, interactive nature of molecular junctions. Here, the Coulomb blockade characteristics of subphthalocyanine between gold electrodes are investigated using combined quantum and molecular mechanics. By incorporating complex frequency-dependent polarizabilities for the electrode representation, the viability of using both components of the complex polarizabilities to study Coulomb blockade phenomena is demonstrated. It allows for the consideration of the photo-response of the electrodes through imaginary polarizabilities, direct computation of redox energies, and a straightforward method to explore molecular junctions.

Original language	English
Article number	141958
Journal	Chemical Physics Letters
Volume	866
Number of pages	5
ISSN	0009-2614
DOIs	https://doi.org/10.1016/j.cplett.2025.141958
Publication status	Published - 2025

Keywords

Molecular junctions
Charge transport
Coulomb blockade diamonds
Complex polarizabilities

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title = "An enhanced Coulomb blockade description of single-molecule junctions through complex polarizabilities",

abstract = "Single-molecule junctions offer a framework for exploring charge transport mechanisms under nonequilibrium conditions. Accurate descriptions are essential, yet challenging, due to the dynamic, interactive nature of molecular junctions. Here, the Coulomb blockade characteristics of subphthalocyanine between gold electrodes are investigated using combined quantum and molecular mechanics. By incorporating complex frequency-dependent polarizabilities for the electrode representation, the viability of using both components of the complex polarizabilities to study Coulomb blockade phenomena is demonstrated. It allows for the consideration of the photo-response of the electrodes through imaginary polarizabilities, direct computation of redox energies, and a straightforward method to explore molecular junctions.",

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T1 - An enhanced Coulomb blockade description of single-molecule junctions through complex polarizabilities

AU - Jensen, Michala D.

AU - Ekstrøm, Ellen T.

AU - Liasi, Zacharias

AU - Mikkelsen, Kurt V.

PY - 2025

Y1 - 2025

N2 - Single-molecule junctions offer a framework for exploring charge transport mechanisms under nonequilibrium conditions. Accurate descriptions are essential, yet challenging, due to the dynamic, interactive nature of molecular junctions. Here, the Coulomb blockade characteristics of subphthalocyanine between gold electrodes are investigated using combined quantum and molecular mechanics. By incorporating complex frequency-dependent polarizabilities for the electrode representation, the viability of using both components of the complex polarizabilities to study Coulomb blockade phenomena is demonstrated. It allows for the consideration of the photo-response of the electrodes through imaginary polarizabilities, direct computation of redox energies, and a straightforward method to explore molecular junctions.

AB - Single-molecule junctions offer a framework for exploring charge transport mechanisms under nonequilibrium conditions. Accurate descriptions are essential, yet challenging, due to the dynamic, interactive nature of molecular junctions. Here, the Coulomb blockade characteristics of subphthalocyanine between gold electrodes are investigated using combined quantum and molecular mechanics. By incorporating complex frequency-dependent polarizabilities for the electrode representation, the viability of using both components of the complex polarizabilities to study Coulomb blockade phenomena is demonstrated. It allows for the consideration of the photo-response of the electrodes through imaginary polarizabilities, direct computation of redox energies, and a straightforward method to explore molecular junctions.

KW - Molecular junctions

KW - Charge transport

KW - Coulomb blockade diamonds

KW - Complex polarizabilities

U2 - 10.1016/j.cplett.2025.141958

DO - 10.1016/j.cplett.2025.141958

M3 - Journal article

SN - 0009-2614

VL - 866

JO - Chemical Physics Letters

JF - Chemical Physics Letters

M1 - 141958

ER -

An enhanced Coulomb blockade description of single-molecule junctions through complex polarizabilities

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