Communication: Dynamical embedding: Correct quantum response from coupling TDDFT for a small cluster with classical near-field electrodynamics for an extended region

Gao, Yi; Neuhauser, Daniel

doi:10.1063/1.4804544

Cited by 12 publications

(26 citation statements)

References 28 publications

(26 reference statements)

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“…The proposed hybrid approach shares similarities with other hybrid methods [27][28][29] and, in principle, can be also coupled to a finite-difference time-domain (FDTD) description of the electromagnetic field. On the other hand, an accurate FDTD model is less crucial if the SQD and MNP are sufficiently far apart.…”

Section: Discussionmentioning

confidence: 99%

“…These hybrid approaches make use of numerical methods such as the finite-difference time domain (FDTD) to solve the classical electrodynamics problem -namely, the Maxwell's equations -while the dynamics of the molecular electrons are solved by means of time-dependent DFT. The overall dynamics are made self-consistent by including the electromagnetic field generated by the MNP into the molecular evolution and vice versa [26][27][28][29] .…”

Section: Introductionmentioning

confidence: 99%

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Projected equations of motion approach to hybrid quantum/classical dynamics in dielectric-metal composites

2016

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Grüning, M. (2016)We introduce a hybrid method for dielectric-metal composites that describes the dynamics of the metallic system classically whilst retaining a quantum description of the dielectric. The timedependent dipole moment of the classical system is mimicked by the introduction of projected equations of motion (PEOM) and the coupling between the two systems is achieved through an effective dipole-dipole interaction. To benchmark this method, we model a test system (semiconducting quantum dot-metal nanoparticle hybrid). We begin by examining the energy absorption rate, showing agreement between the PEOM method and the analytical rotating wave approximation (RWA) solution. We then investigate population inversion and show that the PEOM method provides an accurate model for the interaction under ultrashort pulse excitation where the traditional RWA breaks down.

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Section: Discussionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Projected equations of motion approach to hybrid quantum/classical dynamics in dielectric-metal composites

2016

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“…[2][3][4][5][6][7][8][9][10][11] At the nanoscale, details of atomistic disposition can be critical to the overall properties of the system. 7,8 Multiscale approaches have been recently applied to electronic devices, [3][4][5][6] where quantum mechanical models [12][13][14][15][16][17] are solved in conjunction with classical electromagnetics. One way to include appropriate multiple length scales is to connect atomistic models with continuum models.…”

Section: Introductionmentioning

confidence: 99%

A multiscale quantum mechanics/electromagnetics method for device simulations

et al. 2015

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Multiscale modeling has become a popular tool for research applying to different areas including materials science, microelectronics, biology, chemistry, etc. In this tutorial review, we describe a newly developed multiscale computational method, incorporating quantum mechanics into electronic device modeling with the electromagnetic environment included through classical electrodynamics. In the quantum mechanics/electromagnetics (QM/EM) method, the regions of the system where active electron scattering processes take place are treated quantum mechanically, while the surroundings are described by Maxwell's equations and a semiclassical drift-diffusion model. The QM model and the EM model are solved, respectively, in different regions of the system in a self-consistent manner. Potential distributions and current densities at the interface between QM and EM regions are employed as the boundary conditions for the quantum mechanical and electromagnetic simulations, respectively. The method is illustrated in the simulation of several realistic systems. In the case of junctionless field-effect transistors, transfer characteristics are obtained and a good agreement between experiments and simulations is achieved. Optical properties of a tandem photovoltaic cell are studied and the simulations demonstrate that multiple QM regions are coupled through the classical EM model. Finally, the study of a carbon nanotube-based molecular device shows the accuracy and efficiency of the QM/EM method.

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“…Several time-dependent embedding theories have been developed to study the interactions between molecules and metals: metals often have been represented with simplified models, 41 or the interactions between molecules and metals have been described by classical electrodynamics. [42][43][44][45][46][47] More sophisticated quantum mechanical approaches have appeared recently. By treating the plasmons in metals as a perturbation, Masiello and Schatz developed a many-body perturbation theory approach to simulate surface-enhanced Raman spectroscopy.…”

Section: Introductionmentioning

confidence: 99%

Time-dependent potential-functional embedding theory

Huang

Libisch

Peng

et al. 2014

The Journal of Chemical Physics

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We introduce a time-dependent potential-functional embedding theory (TD-PFET), in which atoms are grouped into subsystems. In TD-PFET, subsystems can be propagated by different suitable time-dependent quantum mechanical methods and their interactions can be treated in a seamless, first-principles manner. TD-PFET is formulated based on the time-dependent quantum mechanics variational principle. The action of the total quantum system is written as a functional of the time-dependent embedding potential, i.e., a potential-functional formulation. By exploiting the Runge-Gross theorem, we prove the uniqueness of the time-dependent embedding potential under the constraint that all subsystems share a common embedding potential. We derive the integral equation that such an embedding potential needs to satisfy. As proof-of-principle, we demonstrate TD-PFET for a Na4 cluster, in which each Na atom is treated as one subsystem and propagated by time-dependent Kohn-Sham density functional theory (TDDFT) using the adiabatic local density approximation (ALDA). Our results agree well with a direct TDDFT calculation on the whole Na4 cluster using ALDA. We envision that TD-PFET will ultimately be useful for studying ultrafast quantum dynamics in condensed matter, where key regions are solved by highly accurate time-dependent quantum mechanics methods, and unimportant regions are solved by faster, less accurate methods.

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Communication: Dynamical embedding: Correct quantum response from coupling TDDFT for a small cluster with classical near-field electrodynamics for an extended region

Cited by 12 publications

References 28 publications

Projected equations of motion approach to hybrid quantum/classical dynamics in dielectric-metal composites

Projected equations of motion approach to hybrid quantum/classical dynamics in dielectric-metal composites

A multiscale quantum mechanics/electromagnetics method for device simulations

Time-dependent potential-functional embedding theory

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