A Green's Function Approach for Determining Surface Induced Broadening and Shifting of Molecular Energy Levels

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Standard

A Green's Function Approach for Determining Surface Induced Broadening and Shifting of Molecular Energy Levels. / Zelovich, Tamar; Hansen, Thorsten; Tuckerman, Mark E.

I: Nano Letters, Bind 22, Nr. 24, 2022, s. 9854–9860.

Publikation: Bidrag til tidsskrift › Tidsskriftartikel › Forskning › fagfællebedømt

Harvard

Zelovich, T, Hansen, T & Tuckerman, ME 2022, 'A Green's Function Approach for Determining Surface Induced Broadening and Shifting of Molecular Energy Levels', Nano Letters, bind 22, nr. 24, s. 9854–9860. https://doi.org/10.1021/acs.nanolett.2c02910

APA

Zelovich, T., Hansen, T., & Tuckerman, M. E. (2022). A Green's Function Approach for Determining Surface Induced Broadening and Shifting of Molecular Energy Levels. Nano Letters, 22(24), 9854–9860. https://doi.org/10.1021/acs.nanolett.2c02910

Vancouver

Zelovich T, Hansen T, Tuckerman ME. A Green's Function Approach for Determining Surface Induced Broadening and Shifting of Molecular Energy Levels. Nano Letters. 2022;22(24):9854–9860. https://doi.org/10.1021/acs.nanolett.2c02910

Author

Zelovich, Tamar ; Hansen, Thorsten ; Tuckerman, Mark E. / A Green's Function Approach for Determining Surface Induced Broadening and Shifting of Molecular Energy Levels. I: Nano Letters. 2022 ; Bind 22, Nr. 24. s. 9854–9860.

Bibtex

@article{ec9632fd615244debbf838510a1ee6c3,
title = "A Green's Function Approach for Determining Surface Induced Broadening and Shifting of Molecular Energy Levels",
abstract = "Upon adsorption of a molecule onto a surface, the molecular energy levels (MELs) broaden and change their alignment. This phenomenon directly affects electron transfer across the interface and is, therefore, a fundamental observable that influences electrochemical device performance. Here, we propose a rigorous parameter-free framework, built upon the theoretical construct of Green's functions, for studying the interface between a molecule and a bulk surface and its effect on MELs. The method extends beyond the usual wide-band limit approximation, and its generality allows its use with any level of electronic structure theory. We demonstrate its ability to predict the broadening and shifting of MELs as a function of intramolecular coupling, molecule/surface coupling, and the surface density of states for a molecule with two MELs adsorbed on a one-dimensional model metal surface. The new approach could help provide guidelines for the design and experimental characterization of electrochemical devices with optimal electron transport.",
keywords = "Molecule/Surface Interface, Molecular Energy Levels, Shifting, Broadening, Alignment, Molecule Adsorption, LI-ION BATTERIES, CHARGE-TRANSPORT, ELECTRONIC DEVICES, ALIGNMENT, SPECTROSCOPY, INTERFACES, JUNCTIONS, SCATTERING",
author = "Tamar Zelovich and Thorsten Hansen and Tuckerman, {Mark E.}",
year = "2022",
doi = "10.1021/acs.nanolett.2c02910",
language = "English",
volume = "22",
pages = "9854–9860",
journal = "Nano Letters",
issn = "1530-6984",
publisher = "American Chemical Society",
number = "24",

}

RIS

TY - JOUR

T1 - A Green's Function Approach for Determining Surface Induced Broadening and Shifting of Molecular Energy Levels

AU - Zelovich, Tamar

AU - Hansen, Thorsten

AU - Tuckerman, Mark E.

PY - 2022

Y1 - 2022

N2 - Upon adsorption of a molecule onto a surface, the molecular energy levels (MELs) broaden and change their alignment. This phenomenon directly affects electron transfer across the interface and is, therefore, a fundamental observable that influences electrochemical device performance. Here, we propose a rigorous parameter-free framework, built upon the theoretical construct of Green's functions, for studying the interface between a molecule and a bulk surface and its effect on MELs. The method extends beyond the usual wide-band limit approximation, and its generality allows its use with any level of electronic structure theory. We demonstrate its ability to predict the broadening and shifting of MELs as a function of intramolecular coupling, molecule/surface coupling, and the surface density of states for a molecule with two MELs adsorbed on a one-dimensional model metal surface. The new approach could help provide guidelines for the design and experimental characterization of electrochemical devices with optimal electron transport.

AB - Upon adsorption of a molecule onto a surface, the molecular energy levels (MELs) broaden and change their alignment. This phenomenon directly affects electron transfer across the interface and is, therefore, a fundamental observable that influences electrochemical device performance. Here, we propose a rigorous parameter-free framework, built upon the theoretical construct of Green's functions, for studying the interface between a molecule and a bulk surface and its effect on MELs. The method extends beyond the usual wide-band limit approximation, and its generality allows its use with any level of electronic structure theory. We demonstrate its ability to predict the broadening and shifting of MELs as a function of intramolecular coupling, molecule/surface coupling, and the surface density of states for a molecule with two MELs adsorbed on a one-dimensional model metal surface. The new approach could help provide guidelines for the design and experimental characterization of electrochemical devices with optimal electron transport.

KW - Molecule/Surface Interface

KW - Molecular Energy Levels

KW - Shifting

KW - Broadening

KW - Alignment

KW - Molecule Adsorption

KW - LI-ION BATTERIES

KW - CHARGE-TRANSPORT

KW - ELECTRONIC DEVICES

KW - ALIGNMENT

KW - SPECTROSCOPY

KW - INTERFACES

KW - JUNCTIONS

KW - SCATTERING

U2 - 10.1021/acs.nanolett.2c02910

DO - 10.1021/acs.nanolett.2c02910

M3 - Journal article

C2 - 36525585

VL - 22

SP - 9854

EP - 9860

JO - Nano Letters

JF - Nano Letters

SN - 1530-6984

IS - 24

ER -

ID: 332197572