Coupled Cluster Theory for Molecular Polaritons: Changing Ground and Excited States

Abstract

We present an ab initio correlated approach to study molecules that interact strongly with quantum fields in an optical cavity. Quantum electrodynamics coupled cluster theory provides a non-perturbative description of cavity-induced effects in ground and excited states. Using this theory, we show how quantum fields can be used to manipulate charge transfer and photochemical properties of molecules. We propose a strategy to lift electronic degeneracies and induce modifications in the ground state potential energy surface close to a conical intersection.

arXiv comment18 pages, 12 figures

References in corpus (21)

• Floquet Topological Insulator in Semiconductor Quantum Wells
• Exciton-polariton condensates
• Atoms and Molecules in Cavities: From Weak to Strong Coupling in QED Chemistry
• Creating stable Floquet-Weyl semimetals by laser-driving of 3D Dirac materials
• Cavity-induced modifications of molecular structure in the strong coupling regime
• Quantum Electrodynamical Density-Functional Theory: Bridging Quantum Optics and Electronic-Structure Theory
• Light-matter interaction in the long-wavelength limit: no ground-state without dipole self-energy
• Resonant catalysis of thermally-activated chemical reactions via vibrational polaritons
• Cavity Casimir-Polder forces and their effects in ground state chemical reactivity
• Time-dependent density functional theory for many-electron systems interacting with cavity photons
• Manipulating azobenzene photoisomerization through strong light-molecule coupling
• Optimized Effective Potential for Quantum Electrodynamical Time-Dependent Density Functional Theory
• Non-adiabatic dynamics of molecules in optical cavities
• eT 1.0: an open source electronic structure program with emphasis on coupled cluster and multilevel methods
• Ab-initio Optimized Effective Potentials for Real Molecules in Optical Cavities: Photon Contributions to the Molecular Ground state
• Cavity control of Excitons in two dimensional Materials
• Cavity Quantum-Electrodynamical Chern Insulator: Route Towards Light-Induced Quantized Anomalous Hall Effect in Graphene
• Control of 1,3-Cyclohexadiene Photoisomerization Using Light-Induced Conical Intersections
• Polaritonic Coupled-Cluster Theory
• Strong coupling with light enhances the photoisomerization quantum yield of azobenzene
• Crossing conditions in coupled cluster theory

Cited by in corpus (79)

• Theoretical Challenges in Polaritonic Chemistry
• Intermolecular interactions in optical cavities: an ab initio QED study
• Catalysis by Dark States in Vibropolaritonic Chemistry
• A perspective on ab initio modeling of polaritonic chemistry: The role of non-equilibrium effects and quantum collectivity
• Cavity-modulated ionization potentials and electron affinities from quantum electrodynamics coupled-cluster theory
• The Free Electron Gas in Cavity Quantum Electrodynamics
• Quantum-Electrodynamical Time-Dependent Density Functional Theory. I. A Gaussian Atomic Basis Implementation
• Exploring Superconductivity under Strong Coupling with the Vacuum Electromagnetic Field
• Cavity molecular dynamics simulations of vibrational polariton enhanced molecular nonlinear absorption
• Strong coupling between localized surface plasmons and molecules by coupled cluster theory
• Unraveling a cavity induced molecular polarization mechanism from collective vibrational strong coupling
• Quantum Coherent Control of a Single Molecular-Polariton Rotation
• Equation-of-motion cavity quantum electrodynamics coupled-cluster theory for electron attachment
• Enhanced diastereocontrol via strong light-matter interactions in an optical cavity
• Strong coupling in chiral cavities: nonperturbative framework for enantiomer discrimination
• Nonequilibrium effects of cavity leakage and vibrational dissipation in thermally-activated polariton chemistry
• Chiral Polaritonics: Analytic Solutions, Intuition and its Use
• Dimensionality reduction of many-body problem using coupled-cluster sub-system flow equations: classical and quantum computing perspective
• Beyond Cavity Born-Oppenheimer: On Non-Adiabatic Coupling and Effective Ground State Hamiltonians in Vibro-Polaritonic Chemistry
• Nonadiabatic Field on Quantum Phase Space: A Century after Ehrenfest
• Assessing the Effects of Orbital Relaxation and the Coherent-State Transformation in Quantum Electrodynamics Density Functional and Coupled-Cluster Theories
• Semiclassical Real-Time Nuclear-Electronic Orbital Dynamics for Molecular Polaritons: Unified Theory of Electronic and Vibrational Strong Couplings
• Simple Exchange-Correlation Energy Functionals for Strongly Coupled Light-Matter Systems based on the Fluctuation-Dissipation Theorem
• Molecular polaritonics in dense mesoscopic disordered ensembles
• Variational Lang-Firsov approach plus Møller-Plesset perturbation theory with applications to ab initio polariton chemistry
• Real-Space, Real-Time Approach to Quantum-Electrodynamical Time-Dependent Density Functional Theory
• A Shortcut to Self-Consistent Light-Matter Interaction and Realistic Spectra from First-Principles
• On the characteristic features of ionization in QED environments
• Machine Learning for Polaritonic Chemistry: Accessing chemical kinetics
• Collective Strong Coupling Modifies Aggregation and Solvation
• Reduced-density-matrix-based ab initio cavity quantum electrodynamics
• Non-Hermitian molecular dynamics simulations of exciton-polaritons in lossy cavities
• Collective response in light-matter interactions: The interplay between strong coupling and local dynamics
• A non-perturbative no-go theorem for photon condensation in approximate models
• Cavity engineering of solid-state materials without external driving
• Coupled Cluster Downfolding Methods: the effect of double commutator terms on the accuracy of ground-state energies
• Automatic derivation of fermionic many-body theories based on general Fermi vacua
• Nonadiabatic Field with Triangle Window Functions on Quantum Phase Space
• Exact Ansatz of Fermion-Boson Systems for a Quantum Device
• Do Molecular Geometries Change Under Vibrational Strong Coupling?
• Effective single mode methodology for strongly coupled multimode molecular-plasmon nanosystems
• Polaritonic Quantum Matter
• Multidimensional quantum calculation of the infrared spectra under polaritonic vibrational strong and ultrastrong coupling
• Sub-system self-consistency in coupled cluster theory
• Cavity Induced Collective Behavior in the Polaritonic Ground State
• An efficient and flexible approach for computing rovibrational polaritons from first principles
• Dissociation slowdown by collective optical response under strong coupling conditions
• Quantum interference and the time-dependent radiation of nanojunctions
• Photon Many-body Dispersion: an Exchange-correlation Functional for Strongly Coupled Light-matter Systems
• Down-conversion processes in ab-initio non-relativistic quantum electrodynamics
• Molecular Polarizability under Vibrational Strong Coupling
• Photon condensation, Van Vleck paramagnetism, and chiral cavities
• Extending the Tavis-Cummings model for molecular ensembles -- Exploring the effects of dipole self energies and static dipole moments
• Selective Excitation of IR-Inactive Modes via Vibrational Polaritons: Insights from Atomistic Simulations
• Virial relations for electrons coupled to quantum field modes
• Photon-photon polaritons in chi(2) microresonators
• Mapping renormalized coupled cluster methods to quantum computers through a compact unitary representation of non-unitary operators
• Understanding polaritonic chemistry from ab initio quantum electrodynamics
• Phaseless auxiliary-field quantum Monte Carlo method for cavity-QED matter systems
• Impact of dipole self-energy on cavity-induced nonadiabatic dynamics
• The role of dark polariton states for electronic strong coupling in molecules
• Quantum-Electrodynamical Density-Functional Theory Exemplified by the Quantum Rabi Model
• Pauli principle in polaritonic chemistry
• Multipolar quantum electrodynamics of localized charge-current distributions: Spectral theory and renormalization
• Full configuration interaction quantum Monte Carlo for coupled electron--boson systems and infinite spaces
• Deep quantum Monte Carlo approach for polaritonic chemistry
• Coupled-cluster theory for trapped bosonic mixtures
• Simulating polaritonic ground states on noisy quantum devices
• Cavity Born-Oppenheimer Coupled Cluster Theory: Towards Electron Correlation in the Vibrational Strong Light-Matter Coupling Regime
• Ab Initio Polaritonic Chemistry on Diverse Quantum Computing Platforms: Qubit, Qudit, and Hybrid Qubit-Qumode Architectures
• Master Equation for a Quantum Gas of Polarizable Particles in Cavities
• Cavity-Modified Zeeman Effect via Spin-Polariton Formation
• The light-matter correlation energy functional of the cavity-coupled two-dimensional electron gas via quantum Monte Carlo simulations
• Wavefunction Embedding for Molecular Polaritons
• Polariton-induced Purcell effects via a reduced semiclassical electrodynamics approach
• Real-time equation-of-motion CC cumulant and CC Green's function simulations of photoemission spectra of water and water dimer
• Density-Functional Tight Binding Meets Maxwell: Unraveling the Mysteries of (Strong) Light-Matter Coupling Efficiently
• Scalable Quantum Monte Carlo Method for Polariton Chemistry via Mixed Block Sparsity and Tensor Hypercontraction Method
• Coupled cluster theory for positron binding in anions and polyatomic molecules