Quantum Effects in Chemical Reactions under Polaritonic Vibrational Strong Coupling

• URL: http://arxiv.org/abs/2109.13690v1
• Date: Tue, 28 Sep 2021 13:04:53 GMT
• Title: Quantum Effects in Chemical Reactions under Polaritonic Vibrational Strong Coupling
• Authors: Peiyun Yang and Jianshu Cao
• Abstract summary: We study the coherent nature of adiabatic reactions and derive the cavity-induced changes in eigen, zero-point-energy, and quantum tunneling. The calculation is further supported by perturbative analysis of polariton normal modes.
• Score: 0.0
• License: http://arxiv.org/licenses/nonexclusive-distrib/1.0/
• Abstract: The electromagnetic field in an optical cavity can dramatically modify and even control chemical reactivity via vibrational strong coupling (VSC). Since the typical vibration and cavity frequencies are considerably higher than thermal energy, it is essential to adopt a quantum description of cavity-catalyzed adiabatic chemical reactions. Using quantum transition state theory (TST), we examine the coherent nature of adiabatic reactions and derive the cavity-induced changes in eigen frequencies, zero-point-energy, and quantum tunneling. The resulting quantum TST calculation allows us to explain and predict the resonance effect (i.e., maximal kinetic modification via tuning the cavity frequency), collective effect (i.e., linear scaling with the molecular density), and selectivity (i.e., cavity-induced control of the branching ratio). The TST calculation is further supported by perturbative analysis of polariton normal modes, which not only provides physical insights to cavity-catalyzed chemical reactions but also presents a general approach to treat other VSC phenomena.

Related papers

• Nonlinear dynamical Casimir effect and Unruh entanglement in waveguide QED with parametrically modulated coupling [83.88591755871734]
  We study theoretically an array of two-level qubits moving relative to a one-dimensional waveguide. When the frequency of this motion approaches twice the qubit resonance frequency, it induces parametric generation of photons and excitation of the qubits. We develop a comprehensive general theoretical framework that incorporates both perturbative diagrammatic techniques and a rigorous master-equation approach.
  arXiv  Detail & Related papers  (2024-08-30T15:54:33Z)
• Quantum interaction of sub-relativistic aloof electrons with mesoscopic samples [91.3755431537592]
  Relativistic electrons experience very slight wave packet distortion and negligible momentum recoil when interacting with nanometer-sized samples. Modelling fast electrons as classical point-charges provides extremely accurate theoretical predictions of energy-loss spectra.
  arXiv  Detail & Related papers  (2022-11-14T15:22:37Z)
• Quantum Dynamics of Vibrational Polariton Chemistry [0.0]
  We employ an exact quantum mechanical simulation technique to investigate a model of cavity-modified chemical reactions in the condensed phase. The model contains the coupling of the reaction coordinate to a generic solvent, cavity coupling to either the reaction coordinate or a non-reactive mode, and the coupling of the cavity to lossy modes.
  arXiv  Detail & Related papers  (2022-10-11T15:45:01Z)
• Reminiscence of classical chaos in driven transmons [117.851325578242]
  We show that even off-resonant drives can cause strong modifications to the structure of the transmon spectrum rendering a large part of it chaotic. Results lead to a photon number threshold characterizing the appearance of chaos-induced quantum demolition effects.
  arXiv  Detail & Related papers  (2022-07-19T16:04:46Z)
• Observation of wave-packet branching through an engineered conical intersection [0.0]
  In chemical reactions, the interplay between coherent evolution and dissipation is central to determining key properties such as the rate and yield. Here, we create a tunable CI in a hybrid qubit-oscillator circuit QED processor. We identify dephasing of the electronic qubit as the mechanism that drives wave-packet branching along the reactive coordinate in our model.
  arXiv  Detail & Related papers  (2022-02-04T19:57:51Z)
• Cavity-Altered Thermal Isomerization Rates and Dynamical Resonant Localization in Vibro-Polaritonic Chemistry [0.0]
  Reaction rates for molecules embedded in microfluidic optical cavities are altered when compared to rates observed under "ordinary" reaction conditions. We study how strong coupling of an optical cavity mode to molecular vibrations affect the reactivity and how resonance behavior emerges.
  arXiv  Detail & Related papers  (2021-09-28T09:06:08Z)
• Demonstration of electron-nuclear decoupling at a spin clock transition [54.088309058031705]
  Clock transitions protect molecular spin qubits from magnetic noise. linear coupling to nuclear degrees of freedom causes a modulation and decay of electronic coherence. An absence of quantum information leakage to the nuclear bath provides opportunities to characterize other decoherence sources.
  arXiv  Detail & Related papers  (2021-06-09T16:23:47Z)
• Nonperturbative Waveguide Quantum Electrodynamics [0.0]
  We study in and out of equilibrium properties of waveguide quantum electrodynamics. We uncover several surprising features ranging from symmetry-protected many-body bound states in the continuum to strong renormalization of the effective mass. Results are relevant to experiments in superconducting qubits interacting with microwave resonators or coupled atoms to photonic crystals.
  arXiv  Detail & Related papers  (2021-05-18T21:15:57Z)
• 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)
• Nonequilibrium effects of cavity leakage and vibrational dissipation in thermally-activated polariton chemistry [0.0]
  We study how dissipative processes, namely those that VSC introduces to the chemical system, affect reactions. We show that such dissipation can change reactivity by accelerating internal thermalization. This phenomenon is attributed mainly to cavity decay, but a supporting role is played by the relaxation between polaritons and dark states.
  arXiv  Detail & Related papers  (2020-11-17T05:55:47Z)
• Probing eigenstate thermalization in quantum simulators via fluctuation-dissipation relations [77.34726150561087]
  The eigenstate thermalization hypothesis (ETH) offers a universal mechanism for the approach to equilibrium of closed quantum many-body systems. Here, we propose a theory-independent route to probe the full ETH in quantum simulators by observing the emergence of fluctuation-dissipation relations. Our work presents a theory-independent way to characterize thermalization in quantum simulators and paves the way to quantum simulate condensed matter pump-probe experiments.
  arXiv  Detail & Related papers  (2020-07-20T18:00:02Z)

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.