Electroluminescence in Molecular Junctions: A Diagrammatic Approach

Goswami, Himangshu Prabal; Hua, Weijie; Zhang, Yu; Mukamel, Shaul; Harbola, Upendra

doi:10.1021/acs.jctc.5b00500

Cited by 11 publications

(15 citation statements)

References 43 publications

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“…This results in a variety of optoelectronic formulations. For example, quasiparticle language was employed in currentinduced light emission, [22][23][24][25][26][27][28] light-induced current, [29][30][31][32] Raman scattering, [33][34][35][36][37] and multidimensional spectroscopy in junctions. 38,39 Many-body formulations are usually restricted to the Lindblad/Redfield quantum master equation (QME) level of theory.…”

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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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confidence: 99%

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

et al. 2019

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“…We note in passing that similar considerations employing bare perturbation theory in the molecule-bath coupling are at the heart of nonlinear optical spectroscopy studies. [230][231][232][233][234] While completely justifiable in isolated systems or for strictly Markovian open system dynamics, utilization of bare perturbation theory in open systems with essentially non-Markovian dynamics is known to violate conservation laws, 235,236 and bare perturbative corrections can lead to qualitatively incorrect predictions. 237 Recently, a conserving flavor of nonlinear optical spectroscopy methods based on GF analysis was presented in Ref.…”

Section: B Many-body Wavefunction Methodsmentioning

confidence: 99%

Green’s function methods for single molecule junctions

Cohen

Galperin

2020

J. Chem. Phys.

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We present a brief pedagogical review of theoretical Green's function methods applicable to open quantum systems out of equilibrium in general, and single molecule junctions in particular. We briefly describe experimental advances in molecular electronics, then discuss different theoretical approaches. We then focus on Green's function methods. Two characteristic energy scales governing the physics are many-body interactions within the junctions, and molecule-contact coupling. We therefore discuss weak interactions and weak coupling, as two limits that can be conveniently treated within, respectively, the standard nonequilibrium Green's function (NEGF) method and its many-body flavors (pseudoparticle and Hubbard NEGF). We argue that the intermediate regime, where the two energy scales are comparable, can in many cases be efficiently treated within the recently introduced superperturbation dual fermion approach. Finally, we review approaches for going beyond these analytically accessible limits, as embodied by recent developments in numerically exact methods based on Green's functions. arXiv:2001.06008v2 [cond-mat.mes-hall]

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“…These advantages were mentioned in many works on optical spectroscopy. 132,139,164,165,169,204,234,235 At the same time the bare PT and utilization of the regression formula may be problematic. The former fails to adequately describe open systems when radiation field is treated quantum mechanically.…”

Section: Liouville Space Formulationmentioning

confidence: 99%

“…31,128,129 In particular, these advancements resulted in necessity to combine theoretical tools of optical spectroscopy with those of quantum transport. Corresponding formulations were developed and applied to description of absorption and current-induced light emission, 51,[130][131][132][133][134][135][136][137][138][139][140][141][142][143] as well as light-induced current in junctions. 60,104,105,130,[144][145][146][147][148][149][150] In these studies light-matter interaction mostly was treated combining classical electrodynamics of radiation field with quantum mechanical description of the molecule.…”

Section: Introductionmentioning

confidence: 99%

Photonics and spectroscopy in nanojunctions: a theoretical insight

Galperin

2017

Chem. Soc. Rev.

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The progress of experimental techniques at the nanoscale in the last decade made optical measurements in current-carrying nanojunctions a reality, thus indicating the emergence of a new field of research coined optoelectronics. Optical spectroscopy of open nonequilibrium systems is a natural meeting point for (at least) two research areas: nonlinear optical spectroscopy and quantum transport, each with its own theoretical toolbox. We review recent progress in the field comparing theoretical treatments of optical response in nanojunctions as is accepted in nonlinear spectroscopy and quantum transport communities. A unified theoretical description of spectroscopy in nanojunctions is presented. We argue that theoretical approaches of the quantum transport community (and in particular, the Green function based considerations) yield a convenient tool for optoelectronics when the radiation field is treated classically, and that differences between the toolboxes may become critical when studying the quantum radiation field in junctions.

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Electroluminescence in Molecular Junctions: A Diagrammatic Approach

Cited by 11 publications

References 43 publications

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

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

Green’s function methods for single molecule junctions

Photonics and spectroscopy in nanojunctions: a theoretical insight

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