Cavity-modulated ionization potentials and electron affinities from quantum electrodynamics coupled-cluster theory.
TLDR
In this paper, a series of sodium halide compounds (NaX, X = F, Cl, Br, and I) are strongly coupled to an optical cavity, and it is demonstrated that EAs are easily modulated by cavity interactions, while IPs for these compounds are far less sensitive to the presence of the cavity.Abstract:
Quantum electrodynamics coupled-cluster (QED-CC) theory is used to model vacuum-field-induced changes to ground-state properties of a series of sodium halide compounds (NaX, X = F, Cl, Br, and I) strongly coupled to an optical cavity. Ionization potentials (IPs) and electron affinities (EAs) are presented, and it is demonstrated that EAs are easily modulated by cavity interactions, while IPs for these compounds are far less sensitive to the presence of the cavity. EAs predicted by QED-CC can be reduced by as much as 0.22 eV (or ≈50%) when considering experimentally accessible coupling parameters.read more
Citations
More filters
Journal ArticleDOI
Quantum-electrodynamical time-dependent density functional theory within Gaussian atomic basis.
TL;DR: In this article, the authors proposed an implementation that uses dimensionless amplitudes for describing the photonic contributions to QED-TDDFT electron-photon eigenstates.
Journal ArticleDOI
Quantum-Electrodynamical Time-Dependent Density Functional Theory. I. A Gaussian Atomic Basis Implementation
TL;DR: In this paper, the authors proposed an implementation that uses dimensionless amplitudes for describing the photonic contributions to quantum-electrodynamical time-dependent density functional theory (QED-TDDFT) electron-photon eigenstates.
Posted Content
Simple Exchange-Correlation Energy Functionals for Strongly Coupled Light-Matter Systems based on the Fluctuation-Dissipation Theorem
TL;DR: In this paper, the gradient-based density functional for the QEDFT exchange-correlation energy derived from the adiabatic-connection fluctuation-dissipation theorem was introduced.
Journal ArticleDOI
Polaritonic Unitary Coupled Cluster for Quantum Computations.
Fabijan Pavošević,Johannes Flick +1 more
TL;DR: In this article, the quantum electrodynamics unitary coupled cluster (QED-UCC) method combined with the variational quantum Eigensolver algorithm, as well as the QED-EOM method formulated in the qubit basis, are presented to calculate ground-state and excited-state properties of strongly coupled light-matter systems suitable for quantum computers.
Posted Content
Polaritonic Unitary Coupled Cluster for Quantum Computations.
Fabijan Pavošević,Johannes Flick +1 more
TL;DR: In this article, the quantum electrodynamics unitary coupled cluster (QED-UCC) method combined with the variational quantum Eigensolver (VQE) algorithm is presented.
References
More filters
Journal ArticleDOI
On the Correlation Problem in Atomic and Molecular Systems. Calculation of Wavefunction Components in Ursell-Type Expansion Using Quantum-Field Theoretical Methods
TL;DR: In this article, a method for the calculation of the matrix elements of the logarithm of an operator which gives the exact wavefunction when operating on the wavefunction in the one-electron approximation is proposed.
Journal ArticleDOI
Coupled-cluster theory in quantum chemistry
Rodney J. Bartlett,Monika Musiał +1 more
TL;DR: In this article, the essential aspects of coupled-cluster theory are explained and illustrated with informative numerical results, showing that the theory offers the most accurate results among the practical ab initio electronic-structure theories applicable to moderate-sized molecules.
Journal ArticleDOI
Insights into Current Limitations of Density Functional Theory
TL;DR: This work characterized and understood the delocalization error and static correlation error of commonly used approximations of density functional theory through the perspective of fractional charges and fractional spins introduced recently.
Journal ArticleDOI
Single-molecule strong coupling at room temperature in plasmonic nanocavities
Rohit Chikkaraddy,Bart de Nijs,Felix Benz,Steven J. Barrow,Oren A. Scherman,Edina Rosta,Angela Demetriadou,P. Fox,Ortwin Hess,Jeremy J. Baumberg +9 more
TL;DR: Statistical analysis of vibrational spectroscopy time series and dark-field scattering spectra provides evidence of single-molecule strong coupling, opening up the exploration of complex natural processes such as photosynthesis and the possibility of manipulating chemical bonds.
Journal ArticleDOI
On some approximations in applications of Xα theory
TL;DR: In this article, an approximate Xα functional is proposed from which the charge density fitting equations follow variationally, and the method independent of the fitting (auxiliary) bases to within 0.02 eV.