Cavity-Mediated Collective Resonant Suppression of Local Molecular Vibrations

• URL: http://arxiv.org/abs/2502.10917v1
• Date: Sat, 15 Feb 2025 22:21:44 GMT
• Title: Cavity-Mediated Collective Resonant Suppression of Local Molecular Vibrations
• Authors: Vasil Rokaj, Ilia Tutunnikov, H. R. Sadeghpour,
• Abstract summary: Recent advances in polaritonic chemistry suggest that chemical reactions can be controlled via collective vibrational strong coupling (VSC) in a cavity. We provide an analytical framework for the dynamics of a molecular ensemble under VSC, revealing that strong collective coupling induces a collective beating. Our model offers insights into how collective VSC can resonantly dampen local molecular vibrations in the collective regime, potentially altering chemical reactivity.
• Score: 0.0
• License:
• Abstract: Recent advances in polaritonic chemistry suggest that chemical reactions can be controlled via collective vibrational strong coupling (VSC) in a cavity. We provide an analytical framework for the dynamics of a molecular ensemble under VSC, revealing that strong collective coupling induces a collective beating, with a period inversely proportional to the collective vacuum Rabi splitting. This emergent beating period occurs over significantly longer time scales than either the individual molecular vibration or cavity field oscillation period, and peaks at the cavity-molecule resonance, consistent with polaritonic chemistry experiments. Most importantly, the collective beating is imprinted on the local dynamics and resonantly suppresses individual molecular vibrations when the molecules are vibrationally excited, as in activated complexes, formed in chemical reactions. The cavity mediates an energy exchange between the excited and the ground-state molecules, affecting the dynamics of the whole ensemble. In the ultrastrong coupling regime, we find that the local vibrations are modified by the cavity even at short time scales. Our analytical model offers insights into how collective VSC can resonantly dampen local molecular vibrations in the collective regime, potentially altering chemical reactivity.

Related papers

• Steering Non-Equilibrium Molecular Dynamics in Optical Cavities [11.581137921729066]
  We study cooperative vibrational strong coupling in an open quantum system. Our work offers a pathway to steer stability of chemical bonds for chemical reactivity under cooperative vibrational strong coupling.
  arXiv  Detail & Related papers  (2024-12-10T15:28:00Z)
• Flipping electric dipole in the vibrational wave packet dynamics of carbon monoxide [0.0]
  Recently Rydberg atom-ion bound states have been observed using a high resolution ion microscope. We investigate whether a similar behavior can also occur for ground state diatomic molecules.
  arXiv  Detail & Related papers  (2024-03-06T21:32:22Z)
• Probing dynamics of a two-dimensional dipolar spin ensemble using single qubit sensor [62.997667081978825]
  We experimentally investigate individual spin dynamics in a two-dimensional ensemble of electron spins on the surface of a diamond crystal. We show that this anomalously slow relaxation rate is due to the presence of strong dynamical disorder. Our work paves the way towards microscopic study and control of quantum thermalization in strongly interacting disordered spin ensembles.
  arXiv  Detail & Related papers  (2022-07-21T18:00:17Z)
• Chemical reactivity under collective vibrational strong coupling [0.0]
  We study unimolecular dissociation reactions of many molecules collectively interacting with an infrared cavity mode. We find that the reaction rate can slow down by increasing the number of aligned molecules if the cavity mode is resonant with a vibrational frequency of the molecules.
  arXiv  Detail & Related papers  (2022-06-17T00:56:12Z)
• Dynamics of Transmon Ionization [94.70553167084388]
  We numerically explore the dynamics of a driven transmon-resonator system under strong and nearly resonant measurement drives. We find clear signatures of transmon ionization where the qubit escapes out of its cosine potential.
  arXiv  Detail & Related papers  (2022-03-21T18:00:15Z)
• Entanglement and correlations in fast collective neutrino flavor oscillations [68.8204255655161]
  Collective neutrino oscillations play a crucial role in transporting lepton flavor in astrophysical settings. We study the full out-of-equilibrium flavor dynamics in simple multi-angle geometries displaying fast oscillations. We present evidence that these fast collective modes are generated by the same dynamical phase transition.
  arXiv  Detail & Related papers  (2022-03-05T17:00:06Z)
• Cavity-modified unimolecular dissociation reactions via intramolecular vibrational energy redistribution [0.0]
  We show that an optical cavity resonantly coupled to particular anharmonic vibrational modes can interfere with unimolecular dissociation reaction rates. In particular, when the cavity is initially empty, the dissociation rate decreases, while when the cavity is initially hotter than the molecule, the cavity can instead accelerate the reaction rate.
  arXiv  Detail & Related papers  (2021-09-09T14:37:39Z)
• Molecular polaritonics in dense mesoscopic disordered ensembles [0.3058685580689604]
  We study the dependence of the vacuum Rabi splitting (VRS) on frequency disorder, vibrations, near-field effects and density in molecular polaritonics.
  arXiv  Detail & Related papers  (2020-10-14T15:16:08Z)
• Collective spontaneous emission of two entangled atoms near an oscillating mirror [50.591267188664666]
  We consider the cooperative spontaneous emission of a system of two identical atoms, interacting with the electromagnetic field in the vacuum state. Using time-dependent theory, we investigate the spectrum of the radiation emitted by the two-atom system. We show that it is modulated in time, and that the presence of the oscillating mirror can enhance or inhibit the decay rate.
  arXiv  Detail & Related papers  (2020-10-07T06:48:20Z)
• Analog cosmological reheating in an ultracold Bose gas [58.720142291102135]
  We quantum-simulate the reheating-like dynamics of a generic cosmological single-field model in an ultracold Bose gas. Expanding spacetime as well as the background oscillating inflaton field are mimicked in the non-relativistic limit. The proposed experiment has the potential of exploring the evolution up to late times even beyond the weak coupling regime.
  arXiv  Detail & Related papers  (2020-08-05T18:00:26Z)
• 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)

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.