Bimodal exciton-plasmon light sources controlled by local charge carrier injection

Merino, Pablo; Rosławska, Anna; Große, Christoph; Leon, Christopher C.; Kuhnke, Klaus; Kern, Klaus

doi:10.1126/sciadv.aap8349

Cited by 23 publications

(39 citation statements)

References 31 publications

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“…For consistency, we show that the emission spectra are identical at all three positions (Fig. 2c) exhibiting no plasmonic contribution 28,32 and varying only in intensity. We record the electroluminescence transients at the marked positions and plot them in Fig.…”

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confidence: 61%

Gigahertz Frame Rate Imaging of Charge-Injection Dynamics in a Molecular Light Source

et al. 2021

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Light sources on the scale of single molecules can be addressed and characterized on their proper subnanometer scale by scanning tunneling microscopy induced luminescence (STML). Such a source can be driven by defined short charge pulses while the luminescence is detected with sub-nanosecond resolution. We introduce an approach to concurrently image the molecular emitter, which is based on an individual defect, with its local environment along with its luminescence dynamics at a resolution of a billion frames per second. The observed dynamics can be assigned to the single electron capture occurring in the low-nanosecond regime. While the emitter's location on the surface remains fixed, the scanning of

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confidence: 61%

Gigahertz Frame Rate Imaging of Charge-Injection Dynamics in a Molecular Light Source

et al. 2021

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“…In this work, the tip–sample distance is in the neighborhood of 0.4 nm estimated from z -spectroscopy approach curves. Of interest in this study are regions of molecularly thick C 60 , free of emission centers, , whose emission is purely plasmonic with no evidence for any excitonic contribution known to occur at the different types of defects reported earlier. ,, Consequently, the light spectrum contains only broad plasmonic modes, such as the features seen at 2 and 1.8 eV in Figure a, excited by inelastic scattering events in the tunnel junction. , This spectrum typically consists of several plasmon modes whose positions and intensities change substantially with tip shape and tip apex preparation. An energy level cartoon of the light emission process is shown in Figure b.…”

Section: Results and Discussionmentioning

confidence: 87%

“…The light emission of molecular C 60 thin films induced by scanning tunneling microscopy can be plasmonic (as in this work), excitonic, or a mixture of both. It is a strong function of tip, sample, and tunneling parameters.…”

Section: Results and Discussionmentioning

confidence: 92%

Single Photon Emission from a Plasmonic Light Source Driven by a Local Field-Induced Coulomb Blockade

et al. 2020

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A hallmark of quantum control is the ability to manipulate quantum emission at the nanoscale. Through scanning tunneling microscopy induced luminescence (STML) we are able to generate plasmonic light originating from inelastic tunneling processes that occur in a few-nanometer thick molecular film of C 60 deposited on Ag(111). Single photon emission, not of excitonic origin, occurs with a 1/e lifetime of a tenth of a nanosecond or less, as shown through Hanbury Brown and Twiss photon intensity interferometry. We have performed tight-binding calculations of the electronic structure for the combined Ag-C 60 -tip system and obtained good agreement with experiment. The tunneling happens through electric field induced split-off states below the C 60 LUMO band, which leads to a Coulomb

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“…The highly localized tunneling current of STM can also be used to induce light emission from a molecule, enabling the investigation of molecular optical properties at sub-molecular spa-tial resolution in a well-defined manner [Figure 1(a)]. STM-induced light emission (STM-LE) spectroscopy has been applied to investigate molecular electroluminescence, [51][52][53][54][55][56][57][58][59][60][61][62] energy transfer between individual molecules, [63][64][65] and the interplay between the dielectric response of metals and intra-molecular electronic excitations. [24][25][26][66][67][68] For STM-LE from a single molecule, a few atomic layers of insulator have been used to partially decouple the molecular electronic structure from the electronic states of the underlying metal substrate.…”

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confidence: 99%

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

et al. 2019

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Electron transport and optical properties of a single molecule in contact with conductive materials have attracted considerable attention owing to their scientific importance and potential applications. With recent progresses of experimental techniques, especially by the 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 becomes possible to investigate single-molecule properties at sub-nanometer spacial resolution. Despite extensive experimental studies, the microscopic mechanism of electronic excitation of a single molecule in STM-induced light emission is 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 intra-molecular 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 intra-molecular Coulomb interaction is crucial for reproducing recent experiments for a single phthalocyanine molecule. The developed theory provides a unified description of both 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.

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Bimodal exciton-plasmon light sources controlled by local charge carrier injection

Abstract: Exciton and plasmon emission can be separately controlled on organic films by using different charge injection channels.

Cited by 23 publications

References 31 publications

Gigahertz Frame Rate Imaging of Charge-Injection Dynamics in a Molecular Light Source

Gigahertz Frame Rate Imaging of Charge-Injection Dynamics in a Molecular Light Source

Single Photon Emission from a Plasmonic Light Source Driven by a Local Field-Induced Coulomb Blockade

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

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