Understanding polaritonic chemistry from ab initio quantum electrodynamics
arXiv:2211.04241
Abstract
In this review we present the theoretical foundations and first principles frameworks to describe quantum matter within quantum electrodynamics (QED) in the low-energy regime. Having a rigorous and fully quantized description of interacting photons, electrons and nuclei/ions, from weak to strong light-matter coupling regimes, is pivotal for a detailed understanding of the emerging fields of polaritonic chemistry and cavity materials engineering. The use of rigorous first principles avoids ambiguities and problems stemming from using approximate models based on phenomenological descriptions of light, matter and their interactions. By starting from fundamental physical and mathematical principles, we first review in great detail non-relativistic QED, which allows to study polaritonic systems non-perturbatively by solving a Schrödinger-type equation. The resulting Pauli-Fierz quantum field theory serves as a cornerstone for the development of computational methods, such as quantum-electrodynamical density functional theory, QED coupled cluster or cavity Born-Oppenheimer molecular dynamics. These methods treat light and matter on equal footing and have the same level of accuracy and reliability as established methods of computational chemistry and electronic structure theory. After an overview of the key-ideas behind those novel ab initio QED methods, we explain their benefits for a better understanding of photon-induced changes of chemical properties and reactions. Based on results obtained by ab initio QED methods we identify the open theoretical questions and how a so far missing mechanistic understanding of polaritonic chemistry can be established. We finally give an outlook on future directions within polaritonic chemistry and first principles QED and address the open questions that need to be solved in the next years both from a theoretical as well as experimental viewpoint.
References in corpus (135)
- Quantum Computing in the NISQ era and beyond
- A variational eigenvalue solver on a quantum processor
- Perspective on density functional theory
- Strong coupling between surface plasmon polaritons and emitters
- Quantum Chemistry in the Age of Quantum Computing
- Ultrastrong coupling between light and matter
- Driven quantum transport on the nanoscale
- Conductivity in organic semiconductors hybridized with the vacuum field
- Cavity-controlled chemistry in molecular ensembles
- Atoms and Molecules in Cavities: From Weak to Strong Coupling in QED Chemistry
- Quantum wave packet revivals
- Octopus, a computational framework for exploring light-driven phenomena and quantum dynamics in extended and finite systems
- The Casimir Effect and the Quantum Vacuum
- Cavity-induced modifications of molecular structure in the strong coupling regime
- Two-dimensional semiconductors in the regime of strong light-matter coupling
- Quantum Electrodynamical Density-Functional Theory: Bridging Quantum Optics and Electronic-Structure Theory
- Is there a no-go theorem for superradiant quantum phase transitions in cavity and circuit QED ?
- Molecular polaritons for controlling chemistry with quantum optics
- Light-matter interaction in the long-wavelength limit: no ground-state without dipole self-energy
- Dispersion forces in macroscopic quantum electrodynamics
- Strongly-Correlated Electron-Photon Systems
- Resolution of Gauge Ambiguities in Ultrastrong-Coupling Cavity QED
- Quantization of quasinormal modes for open cavities and plasmonic cavity-QED
- 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
- Superradiant Phase Transitions and the Standard Description of Circuit QED
- Time-dependent density functional theory for many-electron systems interacting with cavity photons
- Magneto-transport controlled by Landau polariton states
- Ab-initio non-relativistic quantum electrodynamics: Bridging quantum chemistry and quantum optics from weak to strong coupling
- Breakdown of gauge invariance in ultrastrong-coupling cavity QED
- Many-molecule reaction triggered by a single photon in polaritonic chemistry
- Cavity-enhanced transport of charge
- The role of the Riemann-Silberstein vector in classical and quantum theories of electromagnetism
- Quantum Electrodynamic Control of Matter: Cavity-Enhanced Ferroelectric Phase Transition
- Kohn-Sham Approach to Quantum Electrodynamical Density Functional Theory: Exact Time-Dependent Effective Potentials in Real Space
- Optimized Effective Potential for Quantum Electrodynamical Time-Dependent Density Functional Theory
- Ultrastrong coupling phenomena beyond the Dicke model
- Optimal-transport formulation of electronic density-functional theory
- Cavity quantum electrodynamics in the non-perturbative regime
- 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
- Electromagnetic coupling in tight-binding models for strongly correlated light and matter
- Can ultrastrong coupling change ground state chemical reactions?
- Cavity correlated electron-nuclear dynamics from first principles
- Few-mode Field Quantization of Arbitrary Electromagnetic Spectral Densities
- Theory of Photon Condensation in a Spatially-Varying Electromagnetic Field
- Excitonic spectral features in strongly-coupled organic polaritons
- Coherent dynamics in cavity femtochemistry: application of the multi-configuration time-dependent Hartree method
- Dark state semilocalization of quantum emitters in a cavity
- Real-time solutions of coupled Ehrenfest-Maxwell-Pauli-Kohn-Sham equations: fundamentals, implementation, and nano-optical applications
- Catalysis by Dark States in Vibropolaritonic Chemistry
- Strong plasmon-molecule coupling at the nanoscale revealed by first-principles modeling
- Density functional theory for strongly interacting electrons
- Virtual photons in the ground state of a dissipative system
- The Ferroelectric Photo-Groundstate of SrTiO: Cavity Materials Engineering
- A perspective on ab initio modeling of polaritonic chemistry: The role of non-equilibrium effects and quantum collectivity
- Resolution of Gauge Ambiguities in Molecular Cavity Quantum Electrodynamics
- Polaritonic Coupled-Cluster Theory
- Room temperature Organic Exciton-Polariton Condensate in a Lattice
- Perspective: Quantum Hamiltonians for Optical Interactions
- Cavity Quantum Electrodynamics at Arbitrary Light-Matter Coupling Strengths
- Cavity-modulated ionization potentials and electron affinities from quantum electrodynamics coupled-cluster theory
- Large Enhancement of Ferro-Magnetism under Collective Strong Coupling of YBCO Nanoparticles
- Photo-induced electron transfer in the strong coupling regime: Waveguide-plasmon polaritons
- Molecular orbital theory in cavity QED environments
- Photoprotecting uracil by coupling with lossy nanocavities
- On the applicability of quantum-optical concepts in strong-coupling nanophotonics
- On the Quantum Theory of Molecules
- Time-dependent Kohn-Sham approach to quantum electrodynamics
- Langevin Approach to Quantum Optics with Molecules
- Quantum-Electrodynamical Time-Dependent Density Functional Theory. I. A Gaussian Atomic Basis Implementation
- Quantum many-body dynamics in a Lagrangian frame: II. Geometric formulation of time-dependent density functional theory
- Light-Matter Interactions via the Exact Factorization Approach
- Exact Potential Energy Surface for Molecules in Cavities
- Polariton condensation with saturable molecules dressed by vibrational modes
- Fast Green's function method for ultrafast electron-boson dynamics
- Capturing Vacuum Fluctuations and Photon Correlations in Cavity Quantum Electrodynamics with Multi-Trajectory Ehrenfest Dynamics
- Ensemble-induced strong light-matter coupling of a single quantum emitter
- Variational theory of non-relativistic quantum electrodynamics
- Cavity-assisted mesoscopic transport of fermions: Coherent and dissipative dynamics
- Benchmarking Semiclassical and Perturbative Methods for Real-time Simulations of Cavity-Bound Emission and Interference
- Polaritonic Hofstadter Butterfly and Cavity-Control of the Quantized Hall Conductance
- Strong coupling between localized surface plasmons and molecules by coupled cluster theory
- Entangled Photonic-Nuclear Molecular Dynamics of LiF in Quantum Optical Cavities
- Quantum Electrodynamical Bloch Theory with Homogeneous Magnetic Fields
- Weak-to-Strong Light-Matter Coupling and Dissipative Dynamics from First Principles
- Simulating Photodissociation Reactions in Bad Cavities with the Lindblad Equation
- Existence, Uniqueness, and Construction of the Density-Potential Mapping in Time-Dependent Density-Functional Theory
- Mixed Quantum-Classical Electrodynamics: Understanding Spontaneous Decay and Zero Point Energy
- Disorder enhanced vibrational entanglement and dynamics in polaritonic chemistry
- Ehrenfest+R Dynamics I: A Mixed Quantum-Classical Electrodynamics Simulation of Spontaneous Emission
- Uniqueness of the Phase Transition in Many-Dipole Cavity Quantum Electrodynamical Systems
- Quantum nonlinear optics with polar J-aggregates in microcavities
- Reduced Density-Matrix Approach to Strong Matter-Photon Interaction
- Dynamic of Single Molecules in Collective Light-Matter States from First Principles
- Energy-efficient pathway for selectively exciting solute molecules to high vibrational states via solvent vibration-polariton pumping
- Light-matter hybrid-orbital-based first-principles methods: the influence of the polariton statistics
- Shedding Light on Correlated Electron-Photon States using the Exact Factorization
- The Vacua of Dipolar Cavity Quantum Electrodynamics
- Molecular photodissociation enabled by ultrafast plasmon decay
- Simple Exchange-Correlation Energy Functionals for Strongly Coupled Light-Matter Systems based on the Fluctuation-Dissipation Theorem
- A quantum optics approach to photoinduced electron transfer in cavities
- Molecule-photon interactions in phononic environments
- Combining density functional theory with macroscopic QED for quantum light-matter interactions in 2D materials
- Conserving approximations in cavity quantum electrodynamics: Implications for density functional theory of electron-photon systems
- Chemical reactivity under collective vibrational strong coupling
- Quasi-Diabatic Propagation Scheme for Simulating Polariton Chemistry
- A Shortcut to Self-Consistent Light-Matter Interaction and Realistic Spectra from First-Principles
- Quantum Control with Quantum Light of Molecular Nonadiabaticity
- Charge-Transfer Chemical Reactions in Nanofluidic Fabry-P{é}rot Cavities
- Force Balance Approach for Advanced Approximations in Density Functional Theories
- Case Studies of the Time-Dependent Potential Energy Surface for Dynamics in Cavities
- Unique continuation for many-body Schrödinger operators and the Hohenberg-Kohn theorem
- Single-photon emission mediated by single-electron tunneling in plasmonic nanojunctions
- Enhancement of the electron-phonon scattering induced by intrinsic surface plasmon-phonon polaritons
- Exact functionals for correlated electron-photon systems
- Three-player polaritons: nonadiabatic fingerprints in an entangled atom-molecule-photon system
- Engineering long-lived vibrational states for an organic molecule
- Cooperative molecular structure in polaritonic and dark states
- Ehrenfest+R Dynamics II: A Semiclassical QED Framework for Raman Scattering
- Dipolar coupling of nanoparticle-molecule assemblies: An efficient approach for studying strong coupling
- Cavity Induced Collective Behavior in the Polaritonic Ground State
- Stochastic Variational Approach to Small Atoms and Molecules Coupled to Quantum Field Modes
- Pauli-Fierz model with Kato-class potentials and exponential decays
- Down-conversion processes in ab-initio non-relativistic quantum electrodynamics
- On the Spectral Analysis of Quantum Electrodynamics with Spatial Cutoffs. I
- Virial relations for electrons coupled to quantum field modes
- Self-adjointness of semi-relativistic Pauli-Fierz Hamiltonian
- Molecular van der Waals fluids in cavity quantum electrodynamics
- Existence of ground states of hydrogen-like atoms in relativistic QED II: The no-pair operator
- The Density-Potential Mapping in Quantum Dynamics
- Collective dynamics Using Truncated Equations (CUT-E): simulating the collective strong coupling regime with few-molecule models
- Exact Solution for A Real Polaritonic System Under Vibrational Strong Coupling in Thermodynamic Equilibrium: Absence of Zero Temperature and Loss of Light-Matter Entanglement