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Title: Many-Body State Description of Single-Molecule Electroluminescence Driven by a Scanning Tunneling Microscope

Abstract

Electron transport and optical properties of a single molecule in contact with conductive materials have attracted considerable attention because of their scientific importance and potential applications. With the recent progress in experimental techniques, especially by virtue of scanning tunneling microscope (STM)-induced light emission, where the tunneling current of the STM is used as an atomic-scale source for induction of light emission from a single molecule, it has become possible to investigate single-molecule properties at subnanometer spatial resolution. Despite extensive experimental studies, the microscopic mechanism of electronic excitation of a single molecule in STM-induced light emission has yet to be clarified. Here we present a formulation of single-molecule electroluminescence driven by electron transfer between a molecule and metal electrodes based on a many-body state representation of the molecule. The effects of intramolecular Coulomb interaction on conductance and luminescence spectra are investigated using the nonequilibrium Hubbard Green’s function technique combined with first-principles calculations. We compare simulation results with experimental data and find that the intramolecular Coulomb interaction is crucial for reproducing recent experiments for a single phthalocyanine molecule. The developed theory provides a unified description of the electron transport and optical properties of a single molecule in contact with metal electrodes drivenmore » out of equilibrium, and thereby, it contributes to a microscopic understanding of optoelectronic conversion in single molecules on solid surfaces and in nanometer-scale junctions.« less

Authors:
 [1];  [2];  [3];  [3]; ORCiD logo [4]; ORCiD logo [2]
  1. RIKEN, Wako (Japan). Surface and Interface Science Lab.; Univ. of California, San Diego, CA (United States). Dept. of Chemistry and Biochemistry
  2. RIKEN, Wako (Japan). Surface and Interface Science Lab.
  3. RIKEN, Wako (Japan). Surface and Interface Science Lab.; Univ. of Tokyo (Japan). Dept. of Advanced Materials Science, Graduate School of Frontier Science
  4. Univ. of California, San Diego, CA (United States). Dept. of Chemistry and Biochemistry
Publication Date:
Research Org.:
Univ. of California, San Diego, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1507150
Grant/Contract Number:  
SC0018201
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Nano Letters
Additional Journal Information:
Journal Volume: 19; Journal Issue: 5; Journal ID: ISSN 1530-6984
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
77 NANOSCIENCE AND NANOTECHNOLOGY; STM-induced light emission; single phthalocyanine molecule junction; Hubbard nonequilibrium Green's functions

Citation Formats

Miwa, Kuniyuki, Imada, Hiroshi, Imai-Imada, Miyabi, Kimura, Kensuke, Galperin, Michael, and Kim, Yousoo. Many-Body State Description of Single-Molecule Electroluminescence Driven by a Scanning Tunneling Microscope. United States: N. p., 2019. Web. doi:10.1021/acs.nanolett.8b04484.
Miwa, Kuniyuki, Imada, Hiroshi, Imai-Imada, Miyabi, Kimura, Kensuke, Galperin, Michael, & Kim, Yousoo. Many-Body State Description of Single-Molecule Electroluminescence Driven by a Scanning Tunneling Microscope. United States. https://doi.org/10.1021/acs.nanolett.8b04484
Miwa, Kuniyuki, Imada, Hiroshi, Imai-Imada, Miyabi, Kimura, Kensuke, Galperin, Michael, and Kim, Yousoo. 2019. "Many-Body State Description of Single-Molecule Electroluminescence Driven by a Scanning Tunneling Microscope". United States. https://doi.org/10.1021/acs.nanolett.8b04484. https://www.osti.gov/servlets/purl/1507150.
@article{osti_1507150,
title = {Many-Body State Description of Single-Molecule Electroluminescence Driven by a Scanning Tunneling Microscope},
author = {Miwa, Kuniyuki and Imada, Hiroshi and Imai-Imada, Miyabi and Kimura, Kensuke and Galperin, Michael and Kim, Yousoo},
abstractNote = {Electron transport and optical properties of a single molecule in contact with conductive materials have attracted considerable attention because of their scientific importance and potential applications. With the recent progress in experimental techniques, especially by virtue of scanning tunneling microscope (STM)-induced light emission, where the tunneling current of the STM is used as an atomic-scale source for induction of light emission from a single molecule, it has become possible to investigate single-molecule properties at subnanometer spatial resolution. Despite extensive experimental studies, the microscopic mechanism of electronic excitation of a single molecule in STM-induced light emission has yet to be clarified. Here we present a formulation of single-molecule electroluminescence driven by electron transfer between a molecule and metal electrodes based on a many-body state representation of the molecule. The effects of intramolecular Coulomb interaction on conductance and luminescence spectra are investigated using the nonequilibrium Hubbard Green’s function technique combined with first-principles calculations. We compare simulation results with experimental data and find that the intramolecular Coulomb interaction is crucial for reproducing recent experiments for a single phthalocyanine molecule. The developed theory provides a unified description of the electron transport and optical properties of a single molecule in contact with metal electrodes driven out of equilibrium, and thereby, it contributes to a microscopic understanding of optoelectronic conversion in single molecules on solid surfaces and in nanometer-scale junctions.},
doi = {10.1021/acs.nanolett.8b04484},
url = {https://www.osti.gov/biblio/1507150}, journal = {Nano Letters},
issn = {1530-6984},
number = 5,
volume = 19,
place = {United States},
year = {2019},
month = {1}
}

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Cited by: 8 works
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Works referencing / citing this record:

Selective triplet exciton formation in a single molecule
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Single-molecule tautomerization tracking through space- and time-resolved fluorescence spectroscopy
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Electronic friction in interacting systems
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