Optimized Effective Potential for Quantum Electrodynamical Time-Dependent Density Functional Theory

Abstract

We propose a practical approximation to the exchange-correlation functional of (time-dependent) density functional theory for many-electron systems coupled to photons. The (time non-local) optimized effective potential (OEP) equation for the electron- photon system is derived. We test the new approximation in the Rabi model from weak to strong coupling regimes. It is shown that the OEP (i) improves the classical description, (ii) reproduces the quantitative behavior of the exact ground-state properties and (iii) accurately captures the dynamics entering the ultra-strong coupling regime. The present formalism opens the path to a first-principles description of correlated electron-photon systems, bridging the gap between electronic structure methods and quantum optics for real material applications.

5 pages, 2 figures

References in corpus (8)

• Beyond the Jaynes-Cummings model: circuit QED in the ultrastrong coupling regime
• An Open-System Quantum Simulator with Trapped Ions
• Photon-mediated interactions between distant artificial atoms
• Quantum Electrodynamical Density-Functional Theory: Bridging Quantum Optics and Electronic-Structure Theory
• Real-time electron dynamics with exact-exchange time-dependent density-functional theory
• Dynamical correlation functions and the quantum Rabi model
• Quantum electrodynamical time-dependent density functional theory on a lattice
• Non-adiabatic and time-resolved photoelectron spectroscopy for molecular systems

Cited by in corpus (68)

• Atoms and Molecules in Cavities: From Weak to Strong Coupling in QED Chemistry
• Octopus, a computational framework for exploring light-driven phenomena and quantum dynamics in extended and finite systems
• Cavity Born-Oppenheimer Approximation for Correlated Electron-Nuclear-Photon Systems
• Coupled Cluster Theory for Molecular Polaritons: Changing Ground and Excited States
• Molecular polaritonics: Chemical Dynamics under strong Light-Matter Coupling
• Theoretical Challenges in Polaritonic Chemistry
• Ab-initio non-relativistic quantum electrodynamics: Bridging quantum chemistry and quantum optics from weak to strong coupling
• Shining Light on the Microscopic Resonant Mechanism Responsible for Cavity-Mediated Chemical Reactivity
• Kohn-Sham Approach to Quantum Electrodynamical Density Functional Theory: Exact Time-Dependent Effective Potentials in Real Space
• Intermolecular interactions in optical cavities: an ab initio QED study
• Light-Matter Response in Non-Relativistic Quantum Electrodynamics: Quantum Modifications of Maxwell's Equations
• Ab-initio Optimized Effective Potentials for Real Molecules in Optical Cavities: Photon Contributions to the Molecular Ground state
• Cavity correlated electron-nuclear dynamics from first principles
• Real-time solutions of coupled Ehrenfest-Maxwell-Pauli-Kohn-Sham equations: fundamentals, implementation, and nano-optical applications
• Cavity control of Excitons in two dimensional Materials
• A perspective on ab initio modeling of polaritonic chemistry: The role of non-equilibrium effects and quantum collectivity
• Polaritonic Coupled-Cluster Theory
• Cavity-modulated ionization potentials and electron affinities from quantum electrodynamics coupled-cluster theory
• Topical Review: optics of exciton-plasmon nanomaterials
• Quantum-Electrodynamical Time-Dependent Density Functional Theory. I. A Gaussian Atomic Basis Implementation
• The Free Electron Gas in Cavity Quantum Electrodynamics
• Light-Matter Interactions via the Exact Factorization Approach
• Capturing Vacuum Fluctuations and Photon Correlations in Cavity Quantum Electrodynamics with Multi-Trajectory Ehrenfest Dynamics
• Variational theory of non-relativistic quantum electrodynamics
• Benchmarking Semiclassical and Perturbative Methods for Real-time Simulations of Cavity-Bound Emission and Interference
• Quantum Floquet engineering with an exactly solvable tight-binding chain in a cavity
• Equation-of-motion cavity quantum electrodynamics coupled-cluster theory for electron attachment
• Enhanced diastereocontrol via strong light-matter interactions in an optical cavity
• Time-dependent many-body treatment of electron-boson dynamics: application to plasmon-accompanied photoemission
• Time-linear scaling NEGF methods for real-time simulations of interacting electrons and bosons. I. Formalism
• Quasiclassical Modeling of Cavity Quantum Electrodynamics
• Shedding Light on Correlated Electron-Photon States using the Exact Factorization
• Assessing the Effects of Orbital Relaxation and the Coherent-State Transformation in Quantum Electrodynamics Density Functional and Coupled-Cluster Theories
• Simple Exchange-Correlation Energy Functionals for Strongly Coupled Light-Matter Systems based on the Fluctuation-Dissipation Theorem
• Many-body Green's function theory for electron-phonon interactions: the Kadanoff-Baym approach to spectral properties of the Holstein dimer
• Density-functional theory for systems with noncollinear spin: orbital-dependent exchange-correlation functionals and their application to the Hubbard dimer
• Real-Space, Real-Time Approach to Quantum-Electrodynamical Time-Dependent Density Functional Theory
• Conserving approximations in cavity quantum electrodynamics: Implications for density functional theory of electron-photon systems
• Machine Learning Exchange-Correlation Potential in Time Dependent Density Functional Theory
• Machine Learning for Polaritonic Chemistry: Accessing chemical kinetics
• Reduced-density-matrix-based ab initio cavity quantum electrodynamics
• Ab initio calculations of quantum light-matter interactions in general electromagnetic environments
• Cavity engineering of solid-state materials without external driving
• Exact functionals for correlated electron-photon systems
• Effective single mode methodology for strongly coupled multimode molecular-plasmon nanosystems
• Nonadiabatic Field: A Conceptually Novel Approach for Nonadiabatic Quantum Molecular Dynamics
• Cavity Induced Collective Behavior in the Polaritonic Ground State
• Ultrastrong time-dependent light-matter interactions are gauge-relative
• A Snapshot of Time-Dependent Density-Functional Theory
• Photon Many-body Dispersion: an Exchange-correlation Functional for Strongly Coupled Light-matter Systems
• Cavity-induced charge transfer in periodic systems: length-gauge formalism
• Down-conversion processes in ab-initio non-relativistic quantum electrodynamics
• Cavity engineering of Hubbard $U$ via phonon polaritons
• A Mean-Field Treatment of Vacuum Fluctuations in Strong Light-Matter Coupling
• Virial relations for electrons coupled to quantum field modes
• Understanding polaritonic chemistry from ab initio quantum electrodynamics
• Phaseless auxiliary-field quantum Monte Carlo method for cavity-QED matter systems
• Dissipation and spontaneous emission in quantum electrodynamical density functional theory based on optimized effective potential: A proof of concept study
• Hedin equations in resonant micro-cavities
• Quantum-Electrodynamical Density-Functional Theory Exemplified by the Quantum Rabi Model
• Full configuration interaction quantum Monte Carlo for coupled electron--boson systems and infinite spaces
• Ehrenfest Modeling of Cavity Vacuum Fluctuations and How to Achieve Emission from a Three-Level Atom
• Focused Sampling for Low-Cost and Accurate Ehrenfest Modeling of Cavity Quantum Electrodynamics
• Many Electrons and the Photon Field -- The many-body structure of nonrelativistic quantum electrodynamics
• The light-matter correlation energy functional of the cavity-coupled two-dimensional electron gas via quantum Monte Carlo simulations
• Wavefunction Embedding for Molecular Polaritons
• Making ab initio QED functional(s): Non-perturbative and photon-free effective frameworks for strong light-matter coupling
• Density-Functional Tight Binding Meets Maxwell: Unraveling the Mysteries of (Strong) Light-Matter Coupling Efficiently