Too Cool for Blackbody Radiation: Overbias Photon Emission in Ambient STM Due to Multielectron Processes

Fung, E-Dean; Venkataraman, Latha

doi:10.1021/acs.nanolett.0c03994

Cited by 18 publications

(42 citation statements)

References 45 publications

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“…These two peaks are not present (or cannot be distinguished from the background) in the spectrum recorded at V s = −1.5 V; thus, we estimate that the onset of the excitonic STML is between −1.8 and −1.5 V. At V s = −1.8 V, overbias emission occurs at a photon energy about 0.2 eV higher than the quantum cutoff e|V s | = 1.8 eV, with clear evidence of neutral A exciton excitation. This inefficient overbias emission may be due to multielectronic processes [25,26]. All together, these observations are consistent with an STML excitation mechanism on hole injection in the valence of an n-doped semiconductor, which is described as channel 1 in Fig.…”

Section: Resultssupporting

confidence: 85%

Electroluminescence of monolayer WS2 in a scanning tunneling microscope: Effect of bias polarity on spectral and angular distribution of emitted light

Román

Pommier²,

Bretel³

et al. 2022

Phys. Rev. B

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Section: Resultssupporting

confidence: 85%

Electroluminescence of monolayer WS2 in a scanning tunneling microscope: Effect of bias polarity on spectral and angular distribution of emitted light

Román

Pommier²,

Bretel³

et al. 2022

Phys. Rev. B

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“…Recent studies − of plasmonic light emission in tunnel junctions have reported a strong upconversion effect, with generated photon energy ( ℏω ) significantly above the energy threshold of the incident electrons ( eV , where V is the applied bias). While multiple processes can produce such above-threshold photons, recent work , has revealed the dominant role of LSP-induced hot carriers for this.…”

Section: Introductionmentioning

confidence: 99%

Thousand-fold Increase in Plasmonic Light Emission via Combined Electronic and Optical Excitations

et al. 2021

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Surface plasmon enhanced processes and hot-carrier dynamics in plasmonic nanostructures are of great fundamental interest to reveal light-matter interactions at the nanoscale. Using plasmonic tunnel junctions as a platform supporting both electrically-and optically excited localized surface plasmons, we report a much greater (over 1000×) plasmonic light emission at upconverted photon energies under combined electro-optical excitation, compared with electrical or optical excitation separately. Two mechanisms compatible with the form of the observed spectra are interactions of plasmon-induced hot carriers and electronic anti-Stokes Raman scattering. Our measurement results are in excellent agreement with a theoretical model combining electro-optical generation of hot carriers through non-radiative plasmon excitation and hot-carrier relaxation. We also discuss the challenge of distinguishing relative contributions of hot carrier emission and the anti-Stokes electronic Raman process. This observed increase in above-threshold emission in plasmonic systems may open avenues in on-chip nanophotonic switching and hot carrier photocatalysis.

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“…Photoemission detection in MJs also represents a powerful tool for determining charge transport mechanisms through molecules [102,103]. In this regard, Tefashe et al recently investigated symmetric SAM junctions consisting of Ru-(bpy) 3 oligomers of varying lengths sandwiched between conducting carbon contacts [104].…”

Section: Photoemission In Mjsmentioning

confidence: 99%

Light-Driven Charge Transport and Optical Sensing in Molecular Junctions

et al. 2022

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Probing charge and energy transport in molecular junctions (MJs) has not only enabled a fundamental understanding of quantum transport at the atomic and molecular scale, but it also holds significant promise for the development of molecular-scale electronic devices. Recent years have witnessed a rapidly growing interest in understanding light-matter interactions in illuminated MJs. These studies have profoundly deepened our knowledge of the structure–property relations of various molecular materials and paved critical pathways towards utilizing single molecules in future optoelectronics applications. In this article, we survey recent progress in investigating light-driven charge transport in MJs, including junctions composed of a single molecule and self-assembled monolayers (SAMs) of molecules, and new opportunities in optical sensing at the single-molecule level. We focus our attention on describing the experimental design, key phenomena, and the underlying mechanisms. Specifically, topics presented include light-assisted charge transport, photoswitch, and photoemission in MJs. Emerging Raman sensing in MJs is also discussed. Finally, outstanding challenges are explored, and future perspectives in the field are provided.

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Too Cool for Blackbody Radiation: Overbias Photon Emission in Ambient STM Due to Multielectron Processes

Cited by 18 publications

References 45 publications

Electroluminescence of monolayer WS2 in a scanning tunneling microscope: Effect of bias polarity on spectral and angular distribution of emitted light

Electroluminescence of monolayer WS2 in a scanning tunneling microscope: Effect of bias polarity on spectral and angular distribution of emitted light

Thousand-fold Increase in Plasmonic Light Emission via Combined Electronic and Optical Excitations

Light-Driven Charge Transport and Optical Sensing in Molecular Junctions

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