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In this paper we motivate, formulate and analyze the Multi-Configuration Time-Dependent Hartree-Fock (MCTDHF) equations for molecular systems under Coulomb interaction. They consist in approximating the N-particle Schrodinger wavefunction…

Mathematical Physics · Physics 2015-05-13 C. Bardos , I. Catto , N. Mauser , S. Trabelsi

Vibrational polaritons are formed by strong coupling of molecular vibrations and photon modes in an optical cavity. Experiments have demonstrated that vibrational strong coupling can change molecular properties and even affect chemical…

Quantum Physics · Physics 2025-01-14 Thomas Schnappinger , Cyril Falvo , Markus Kowalewski

Strong light-matter coupling enables hybrid states in which photonic and electronic degrees of freedom become correlated even in the ground state. While many-body effects in long-range dispersion interactions are known to reshape electronic…

Chemical Physics · Physics 2025-12-23 Cankut Tasci , Mohammad Hassan , Leon Orlov-Sullivan , Leonardo A. Cunha , Johannes Flick

Molecular polaritons arise when molecules interact so strongly with light that they become entangled with each other. This light-matter hybridization alters the chemical and physical properties of the molecular system and allows chemical…

Chemical Physics · Physics 2023-07-28 Tor S. Haugland , John P. Philbin , Tushar K. Ghosh , Ming Chen , Henrik Koch , Prineha Narang

We present a new ab initio approach to study molecules containing heavy atoms strongly interacting with quantum fields in optical devices. The theory has been derived from the relativistic quantum electrodynamics (QED) introducing the…

Chemical Physics · Physics 2025-07-03 Guillaume Thiam , Riccardo Rossi , Henrik Koch , Leonardo Belpassi , Enrico Ronca

In this work, we provide an overview of how well-established concepts in the fields of quantum chemistry and material sciences have to be adapted when the quantum nature of light becomes important in correlated matter-photon problems.…

Quantum Physics · Physics 2017-04-12 Johannes Flick , Michael Ruggenthaler , Heiko Appel , Angel Rubio

We study light-mediated interactions between spatially separated molecules using real-time quantum electrodynamical time-dependent density functional theory based on the Pauli-Fierz Hamiltonian. An ultrashort delta-kick excitation…

Chemical Physics · Physics 2026-01-22 Yetmgeta Aklilu , Tiany Yang , Cody Covington , Kalman Varga

Silicon quantum computing has the potential to revolutionize technology with capabilities to solve real-life problems that are computationally complex or even intractable for modern computers [1] by offering sufficient high quality qubits…

Mesoscale and Nanoscale Physics · Physics 2024-09-24 Dylan H. Liang , MengKe Feng , Philip Y. Mai , Jesus D. Cifuentes , Andrew S. Dzurak , Andre Saraiva

The electron attachment variant of equation-of-motion coupled-cluster theory (EOM-EA-CC) is generalized to the case of strong light-matter coupling within the framework of cavity quantum electrodynamics (QED). The resulting EOM-EA-QED-CC…

Chemical Physics · Physics 2022-02-23 Marcus D. Liebenthal , Nam Vu , A. Eugene DePrince

We introduce the first multiorbital effective tight-binding model to describe the effect of electron-electron interactions in this system. Upon fixing all the effective hopping parameters in the normal state against an ab initio band…

Strongly Correlated Electrons · Physics 2017-06-27 Lei Su , Chuang-Han Hsu , Hsin Lin , Vitor M. Pereira

Polaritonic chemistry offers the possibility of modifying molecular properties and even influencing chemical reactivity through strong coupling between vibrational transitions and confined light modes in optical cavities. Despite…

Chemical Physics · Physics 2025-05-16 Thomas Schnappinger , Markus Kowalewski

The multiconfiguration time-dependent Hartree-Fock (MCTDHF) method is formulated for treating the coupled electronic and nuclear dynamics of diatomic molecules without the Born- Oppenheimer approximation. The method treats the full…

Computational Physics · Physics 2015-05-27 Daniel J. Haxton , Keith V. Lawler , C. William McCurdy

We present a rigorous formulation of the time-dependent density functional theory for interacting lattice electrons strongly coupled to cavity photons. We start with an example of one particle on a Hubbard dimer coupled to a single photonic…

Strongly Correlated Electrons · Physics 2015-06-22 Mehdi Farzanehpour , I. V. Tokatly

Quantum-electrodynamical density-functional theory (QEDFT) provides a promising avenue for exploring complex light-matter interactions in optical cavities for real materials. Similar to conventional density-functional theory, the Kohn-Sham…

Computational Physics · Physics 2024-02-16 I-Te Lu , Michael Ruggenthaler , Nicolas Tancogne-Dejean , Simone Latini , Markus Penz , Angel Rubio

The rapidly developing and converging fields of polaritonic chemistry and quantum optics necessitate a unified approach to predict strongly-correlated light-matter interactions with atomic-scale resolution. Combining concepts from both…

Quantum Physics · Physics 2018-09-19 Johannes Flick , Prineha Narang

The orientation-dependent strong-field ionization of CO molecules is investigated using the fully propagated three-dimensional time-dependent Hartree-Fock theory. The full ionization results are in good agreement with recent experiments.…

Atomic Physics · Physics 2013-10-30 Bin Zhang , Jianmin Yuan , Zengxiu Zhao

First-order electric dipole response functions are implemented for cavity quantum electrodynamics (QED) generalizations of Hartree-Fock (HF) and Kohn-Sham density functional theory (DFT) in order to assess the degree to which static…

Chemical Physics · Physics 2025-07-31 A. Eugene DePrince , Stephen H. Yuwono

We present unrestricted Hartree Fock method coupled with configuration interaction (CI) method (URHF-CI) suitable for the calculation of ground and excited states of large number of electrons localized by complex gate potentials in…

Mesoscale and Nanoscale Physics · Physics 2009-11-11 Ramin M. Abolfath , Pawel Hawrylak

We present two improvements to the tight-binding approximation of time-dependent density functional theory (TD-DFTB): Firstly, we add an exact Hartree-Fock exchange term, which is switched on at large distances, to the ground state…

Chemical Physics · Physics 2015-10-28 Alexander Humeniuk , Roland Mitric

Cavity quantum electrodynamics (QED) manipulates the coupling of light with matter, and allows for several emitters to couple coherently with one light mode. However, even in a many-body system, the light-matter coupling mechanism was so…

Quantum Gases · Physics 2021-11-10 Hideki Konishi , Kevin Roux , Victor Helson , Jean-Philippe Brantut