Bipolar single-molecule electroluminescence and electrofluorochromism

Understanding the fundamental mechanisms of optoelectronic excitation and relaxation pathways on the single-molecule level has only recently been started by combining scanning tunneling microscopy (STM) and spectroscopy (STS) with STM-induced luminescence (STML). In this paper, we investigate cation...

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Main Authors: Tzu-Chao Hung, Roberto Robles, Brian Kiraly, Julian H. Strik, Bram A. Rutten, Alexander A. Khajetoorians, Nicolas Lorente, Daniel Wegner
Format: Article
Language:English
Published: American Physical Society 2023-07-01
Series:Physical Review Research
Online Access:http://doi.org/10.1103/PhysRevResearch.5.033027
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author Tzu-Chao Hung
Roberto Robles
Brian Kiraly
Julian H. Strik
Bram A. Rutten
Alexander A. Khajetoorians
Nicolas Lorente
Daniel Wegner
author_facet Tzu-Chao Hung
Roberto Robles
Brian Kiraly
Julian H. Strik
Bram A. Rutten
Alexander A. Khajetoorians
Nicolas Lorente
Daniel Wegner
author_sort Tzu-Chao Hung
collection DOAJ
description Understanding the fundamental mechanisms of optoelectronic excitation and relaxation pathways on the single-molecule level has only recently been started by combining scanning tunneling microscopy (STM) and spectroscopy (STS) with STM-induced luminescence (STML). In this paper, we investigate cationic and anionic fluorescence of individual zinc phthalocyanine (ZnPc) molecules adsorbed on ultrathin NaCl films on Ag(111) by using STML. They depend on the tip-sample bias polarity and appear at threshold voltages that are correlated with the onset energies of particular molecular orbitals, as identified by STS. We also find that the fluorescence is caused by a single-electron tunneling process. Comparing with results from density functional theory calculations, we propose an alternative many-body picture to describe the charging and electroluminescence mechanism. In this paper, we provide aspects toward well-defined voltage selectivity of bipolar electrofluorochromism as well as fundamental insights regarding the role of transiently charged states of emitter molecules within organic light-emitting diode devices.
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spelling doaj.art-cec296d5a24b483ea8c10446269d62392024-04-12T17:32:28ZengAmerican Physical SocietyPhysical Review Research2643-15642023-07-015303302710.1103/PhysRevResearch.5.033027Bipolar single-molecule electroluminescence and electrofluorochromismTzu-Chao HungRoberto RoblesBrian KiralyJulian H. StrikBram A. RuttenAlexander A. KhajetooriansNicolas LorenteDaniel WegnerUnderstanding the fundamental mechanisms of optoelectronic excitation and relaxation pathways on the single-molecule level has only recently been started by combining scanning tunneling microscopy (STM) and spectroscopy (STS) with STM-induced luminescence (STML). In this paper, we investigate cationic and anionic fluorescence of individual zinc phthalocyanine (ZnPc) molecules adsorbed on ultrathin NaCl films on Ag(111) by using STML. They depend on the tip-sample bias polarity and appear at threshold voltages that are correlated with the onset energies of particular molecular orbitals, as identified by STS. We also find that the fluorescence is caused by a single-electron tunneling process. Comparing with results from density functional theory calculations, we propose an alternative many-body picture to describe the charging and electroluminescence mechanism. In this paper, we provide aspects toward well-defined voltage selectivity of bipolar electrofluorochromism as well as fundamental insights regarding the role of transiently charged states of emitter molecules within organic light-emitting diode devices.http://doi.org/10.1103/PhysRevResearch.5.033027
spellingShingle Tzu-Chao Hung
Roberto Robles
Brian Kiraly
Julian H. Strik
Bram A. Rutten
Alexander A. Khajetoorians
Nicolas Lorente
Daniel Wegner
Bipolar single-molecule electroluminescence and electrofluorochromism
Physical Review Research
title Bipolar single-molecule electroluminescence and electrofluorochromism
title_full Bipolar single-molecule electroluminescence and electrofluorochromism
title_fullStr Bipolar single-molecule electroluminescence and electrofluorochromism
title_full_unstemmed Bipolar single-molecule electroluminescence and electrofluorochromism
title_short Bipolar single-molecule electroluminescence and electrofluorochromism
title_sort bipolar single molecule electroluminescence and electrofluorochromism
url http://doi.org/10.1103/PhysRevResearch.5.033027
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