Cavity-Born-Oppenheimer Hartree-Fock Ansatz: Light-matter Properties of Strongly Coupled Molecular Ensembles

• URL: http://arxiv.org/abs/2307.02208v1
• Date: Wed, 5 Jul 2023 11:20:24 GMT
• Title: Cavity-Born-Oppenheimer Hartree-Fock Ansatz: Light-matter Properties of Strongly Coupled Molecular Ensembles
• Authors: Thomas Schnappinger, Dominik Sidler, Michael Ruggenthaler, Angel Rubio and Markus Kowalewski
• Abstract summary: We present an ab-initio Hartree-Fock ansatz in the framework of the cavity Born-Oppenheimer approximation. We study the collective effects in ensembles of strongly coupled diatomic hydrogen fluoride molecules.
• Score: 0.0
• License: http://creativecommons.org/licenses/by/4.0/
• Abstract: Experimental studies indicate that optical cavities can affect chemical reactions, through either vibrational or electronic strong coupling and the quantized cavity modes. However, the current understanding of the interplay between molecules and confined light modes is incomplete. Accurate theoretical models, that take into account inter-molecular interactions to describe ensembles, are therefore essential to understand the mechanisms governing polaritonic chemistry. We present an ab-initio Hartree-Fock ansatz in the framework of the cavity Born-Oppenheimer approximation and study molecules strongly interacting with an optical cavity. This ansatz provides a non-perturbative, self-consistent description of strongly coupled molecular ensembles taking into account the cavity-mediated dipole self-energy contributions. To demonstrate the capability of the cavity Born-Oppenheimer Hartree-Fock ansatz, we study the collective effects in ensembles of strongly coupled diatomic hydrogen fluoride molecules. Our results highlight the importance of the cavity-mediated inter-molecular dipole-dipole interactions, which lead to energetic changes of individual molecules in the coupled ensemble.

Related papers

• Disentangling collective coupling in vibrational polaritons with double quantum coherence spectroscopy [0.0]
  Vibrational polaritons are formed by strong coupling of molecular vibrations and photon modes in an optical cavity. We simulate two-dimensional infrared spectra of molecular vibrational polaritons based on the double quantum coherence technique.
  arXiv  Detail & Related papers  (2024-10-01T08:24:40Z)
• Extending the Tavis-Cummings model for molecular ensembles -- Exploring the effects of dipole self energies and static dipole moments [0.0]
  We extend the Tavis-Cummings model for molecular ensembles. We simulate excited-state dynamics and spectroscopy of MgH$+$ molecules resonantly coupled to an optical cavity.
  arXiv  Detail & Related papers  (2024-04-16T15:58:40Z)
• Modeling Non-Covalent Interatomic Interactions on a Photonic Quantum Computer [50.24983453990065]
  We show that the cQDO model lends itself naturally to simulation on a photonic quantum computer. We calculate the binding energy curve of diatomic systems by leveraging Xanadu's Strawberry Fields photonics library. Remarkably, we find that two coupled bosonic QDOs exhibit a stable bond.
  arXiv  Detail & Related papers  (2023-06-14T14:44:12Z)
• Unraveling a cavity induced molecular polarization mechanism from collective vibrational strong coupling [0.0]
  We show that collective vibrational strong coupling of molecules in thermal equilibrium can give rise to significant local electronic polarizations in the thermodynamic limit. Our findings suggest that the thorough understanding of polaritonic chemistry, requires a self-consistent treatment of dressed electronic structure.
  arXiv  Detail & Related papers  (2023-06-09T16:18:51Z)
• Cavity-Catalyzed Hydrogen Transfer Dynamics in an Entangled Molecular Ensemble under Vibrational Strong Coupling [0.0]
  We numerically solve the Schr"odinger equation to study the cavity-induced quantum dynamics in an ensemble of molecules. We show that the cavity indeed enforces hydrogen transfer from an enol to an enethiol configuration with transfer rates significantly increasing with light-matter interaction strength. A non-trivial dependence of the dynamics on ensemble size is found, clearly beyond scaled single-molecule models.
  arXiv  Detail & Related papers  (2023-01-10T16:58:57Z)
• DiffBP: Generative Diffusion of 3D Molecules for Target Protein Binding [51.970607704953096]
  Previous works usually generate atoms in an auto-regressive way, where element types and 3D coordinates of atoms are generated one by one. In real-world molecular systems, the interactions among atoms in an entire molecule are global, leading to the energy function pair-coupled among atoms. In this work, a generative diffusion model for molecular 3D structures based on target proteins is established, at a full-atom level in a non-autoregressive way.
  arXiv  Detail & Related papers  (2022-11-21T07:02:15Z)
• Relativistic aspects of orbital and magnetic anisotropies in the chemical bonding and structure of lanthanide molecules [60.17174832243075]
  We study the electronic and ro-vibrational states of heavy homonuclear lanthanide Er2 and Tm2 molecules by applying state-of-the-art relativistic methods. We were able to obtain reliable spin-orbit and correlation-induced splittings between the 91 Er2 and 36 Tm2 electronic potentials dissociating to two ground-state atoms.
  arXiv  Detail & Related papers  (2021-07-06T15:34:00Z)
• Molecular Interactions Induced by a Static Electric Field in Quantum Mechanics and Quantum Electrodynamics [68.98428372162448]
  We study the interaction between two neutral atoms or molecules subject to a uniform static electric field. Our focus is to understand the interplay between leading contributions to field-induced electrostatics/polarization and dispersion interactions.
  arXiv  Detail & Related papers  (2021-03-30T14:45:30Z)
• Dynamical Strengthening of Covalent and Non-Covalent Molecular Interactions by Nuclear Quantum Effects at Finite Temperature [58.999762016297865]
  Nuclear quantum effects (NQE) tend to generate delocalized molecular dynamics. NQE often enhance electronic interactions and, in turn, can result in dynamical molecular stabilization at finite temperature. Our findings yield new insights into the versatile role of nuclear quantum fluctuations in molecules and materials.
  arXiv  Detail & Related papers  (2020-06-18T14:30:29Z)
• Collective Dissipative Molecule Formation in a Cavity [0.0]
  We propose a mechanism to realize high-yield molecular formation from ultracold atoms. We demonstrate that the molecular yield can be improved by simply increasing the number of atoms.
  arXiv  Detail & Related papers  (2020-02-13T16:25:30Z)
• Quantum decoherence by Coulomb interaction [58.720142291102135]
  We present an experimental study of the Coulomb-induced decoherence of free electrons in a superposition state in a biprism electron interferometer close to a semiconducting and metallic surface. The results will enable the determination and minimization of specific decoherence channels in the design of novel quantum instruments.
  arXiv  Detail & Related papers  (2020-01-17T04:11:44Z)

This list is automatically generated from the titles and abstracts of the papers in this site.

This site does not guarantee the quality of this site (including all information) and is not responsible for any consequences.