Unraveling a cavity induced molecular polarization mechanism from collective vibrational strong coupling

• URL: http://arxiv.org/abs/2306.06004v4
• Date: Wed, 27 Mar 2024 13:32:51 GMT
• Title: Unraveling a cavity induced molecular polarization mechanism from collective vibrational strong coupling
• Authors: Dominik Sidler, Thomas Schnappinger, Anatoly Obzhirov, Michael Ruggenthaler, Markus Kowalewski, Angel Rubio,
• Abstract summary: 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.
• Score: 0.0
• License: http://creativecommons.org/licenses/by/4.0/
• Abstract: We demonstrate that collective vibrational strong coupling of molecules in thermal equilibrium can give rise to significant local electronic polarizations in the thermodynamic limit. We do so by first showing that the full non-relativistic Pauli-Fierz problem of an ensemble of strongly-coupled molecules in the dilute-gas limit reduces in the cavity Born-Oppenheimer approximation to a cavity-Hartree equation for the electronic structure. Consequently, each individual molecule experiences a self-consistent coupling to the dipoles of all other molecules, which amount to non-negligible values in the thermodynamic limit (large ensembles). Thus collective vibrational strong coupling can alter individual molecules strongly for localized "hotspots" within the ensemble. Moreover, the discovered cavity-induced polarization pattern possesses a zero net polarization, which resembles a continuous form of a spin glass (or better polarization glass). Our findings suggest that the thorough understanding of polaritonic chemistry, requires a self-consistent treatment of dressed electronic structure, which can give rise to numerous, so far overlooked, physical mechanisms.

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)
• Collective rovibronic dynamics of a diatomic gas coupled by cavity [0.0]
  We consider an ensemble of homonuclear diatomic molecules coupled to the two polarization directions of a Fabry-P'erot cavity. We identify a coupling mechanism mediated simultaneously by the two perpendicular polarizations, and inducing polaritonic relaxation towards molecular rotations. Our simulations indicate that the molecular rotational dynamics in gas-phase cavity-coupled systems can serve as a novel probe for non-radiative polaritonic decay towards the dark-states manifold.
  arXiv  Detail & Related papers  (2024-01-19T14:35:35Z)
• Cavity-Born-Oppenheimer Hartree-Fock Ansatz: Light-matter Properties of Strongly Coupled Molecular Ensembles [0.0]
  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.
  arXiv  Detail & Related papers  (2023-07-05T11:20:24Z)
• Observation of Rydberg blockade due to the charge-dipole interaction between an atom and a polar molecule [52.77024349608834]
  We demonstrate Rydberg blockade due to the charge-dipole interaction between a single Rb atom and a single RbCs molecule confined in optical tweezers. Results open up the prospect of a hybrid platform where quantum information is transferred between individually trapped molecules using Rydberg atoms.
  arXiv  Detail & Related papers  (2023-03-10T18:41:20Z)
• 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)
• Chemical tuning of spin clock transitions in molecular monomers based on nuclear spin-free Ni(II) [52.259804540075514]
  We report the existence of a sizeable quantum tunnelling splitting between the two lowest electronic spin levels of mononuclear Ni complexes. The level anti-crossing, or magnetic clock transition, associated with this gap has been directly monitored by heat capacity experiments. The comparison of these results with those obtained for a Co derivative, for which tunnelling is forbidden by symmetry, shows that the clock transition leads to an effective suppression of intermolecular spin-spin interactions.
  arXiv  Detail & Related papers  (2021-03-04T13:31:40Z)
• 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)
• Quantum coherent spin-electric control in a molecular nanomagnet at clock transitions [57.50861918173065]
  Electrical control of spins at the nanoscale offers architectural advantages in spintronics. Recent demonstrations of electric-field (E-field) sensitivities in molecular spin materials are tantalising. E-field sensitivities reported so far are rather weak, prompting the question of how to design molecules with stronger spin-electric couplings.
  arXiv  Detail & Related papers  (2020-05-03T09:27:31Z)
• Optically pumped spin polarization as a probe of many-body thermalization [50.591267188664666]
  We study the spin diffusion dynamics of 13C in diamond, which we dynamically polarize at room temperature via optical spin pumping of engineered color centers. We find good thermal contact throughout the nuclear spin bath, virtually independent of the hyperfine coupling strength. Our results open intriguing opportunities to study the onset of thermalization in a system by controlling the internal interactions within the bath.
  arXiv  Detail & Related papers  (2020-05-01T23:16:33Z)
• 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)

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.