The Shape of the Electric Dipole Function Determines the Sub-Picosecond Dynamics of Anharmonic Vibrational Polaritons

• URL: http://arxiv.org/abs/2003.07783v1
• Date: Tue, 17 Mar 2020 15:55:09 GMT
• Title: The Shape of the Electric Dipole Function Determines the Sub-Picosecond Dynamics of Anharmonic Vibrational Polaritons
• Authors: Johan F. Triana, Federico J. Hern\'andez, Felipe Herrera
• Abstract summary: We describe for the first time the essential role of permanent dipole moments in the femtosecond dynamics of vibrational polariton wavepackets. We propose a non-adiabatic state preparation scheme to generate vibrational polaritons using nanoscale infrared antennas and UV-vis photochemistry or electron tunneling.
• Score: 0.0
• License: http://arxiv.org/licenses/nonexclusive-distrib/1.0/
• Abstract: We develop a fully quantum mechanical methodology to describe the static properties and the dynamics of a single anharmonic vibrational mode interacting with a quantized infrared cavity field in the strong and ultrastrong coupling regimes. By comparing multiconfiguration time-dependent Hartree (MCTDH) simulations for a Morse oscillator in a cavity, with an equivalent formulation of the problem in Hilbert space, we describe for the first time the essential role of permanent dipole moments in the femtosecond dynamics of vibrational polariton wavepackets. We show that depending on the shape of the electric dipole function $d_e(q)$ along the vibrational mode coordinate $q$, molecules can be classified into three general families. For molecules that are polar and have a positive slope of the dipole function at equilibrium, we show that an initial diabatic light-matter product state without vibrational or cavity excitations can evolve into a polariton wavepacket with a large number of intracavity photons, for interaction strengths at the onset of ultrastrong coupling. This build up of intracavity photon amplitude is accompanied by an effective $lengthening$ of the vibrational mode of nearly $10\%$, comparable with a laser-induced vibrational excitation in free space. In contrast, molecules that are also polar at equilibrium but have a negative slope of the dipole function, experience an effective mode $shortening$ under equivalent coupling conditions. Our model predictions are numerically validated using realistic $ab$-$initio$ potentials and dipole functions for HF and CO$_2$ molecules in their ground electronic states. We finally propose a non-adiabatic state preparation scheme to generate vibrational polaritons using nanoscale infrared antennas and UV-vis photochemistry or electron tunneling, to enable the far-field detection of spontaneously generated infrared quantum light.

Related papers

• Zeeman polaritons as a platform for probing Dicke physics in condensed matter [2.523996579776851]
  We show that a spin--boson system is more compatible with the Dicke model and has advantages over boson--boson systems for pursuing experimental realizations of phenomena predicted for ultrastrongly coupled light--matter hybrids. This finding demonstrates that a spin--boson system is more compatible with the Dicke model and has advantages over boson--boson systems for pursuing experimental realizations of phenomena predicted for ultrastrongly coupled light--matter hybrids.
  arXiv  Detail & Related papers  (2024-09-25T20:28:01Z)
• Mode-multiplexing deep-strong light-matter coupling [0.0]
  We show a new regime of record-strong light-matter interaction which exploits the cooperative dipole moments of multiple, highly non-resonant magnetoplasmon modes. The extreme interaction drives strongly subcycle exchange of vacuum energy between multiple bosonic modes. This offers avenues towards tailoring phase transitions by coupling otherwise non-interacting modes.
  arXiv  Detail & Related papers  (2023-09-13T12:27:35Z)
• Quantum vibrational mode in a cavity confining a massless spinor field [91.3755431537592]
  We analyse the reaction of a massless (1+1)-dimensional spinor field to the harmonic motion of one cavity wall. We demonstrate that the system is able to convert bosons into fermion pairs at the lowest perturbative order.
  arXiv  Detail & Related papers  (2022-09-12T08:21:12Z)
• 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)
• Generalization of the Tavis-Cummings model for multi-level anharmonic systems: insights on the second excitation manifold [0.0]
  This work contrasts predictions from the Tavis-Cummings (TC) model, in which the material is a collection of two-level systems. We simplify the brute-force diagonalization of a gigantic $N2times N2$ Hamiltonian. We find resonant conditions between bipolaritons and anharmonic transitions where two-photon absorption can be enhanced.
  arXiv  Detail & Related papers  (2022-02-03T06:33:42Z)
• Ultrafast modulation of vibrational polaritons for controlling the quantum field statistics at mid-infrared frequencies [0.0]
  We show that by coupling molecular vibrations with a confined mid-infrared cavity vacuum, the photocount and quadrature field statistics of the cavity field can be reversibly manipulated over sub-picosecond timescales. This work paves the way for the development of molecule-based mid-infrared quantum optical devices at room temperature.
  arXiv  Detail & Related papers  (2021-11-12T14:06:58Z)
• Long-Range Non-Equilibrium Coherent Tunneling Induced by Fractional Vibronic Resonances [0.0]
  We study the influence of a linear energy bias on a non-equilibrium excitation on a chain of molecules coupled to local phonons. We uncover structured and discrete vibronic resonance behavior fundamentally different from both linear response theory and homogeneous polaron dynamics. Potential applications range from molecular electronics to optical lattices and artificial light harvesting via vibronic engineering of coherent quantum transport.
  arXiv  Detail & Related papers  (2021-11-11T10:40:38Z)
• 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)
• Controlled coherent dynamics of [VO(TPP)], a prototype molecular nuclear qudit with an electronic ancilla [50.002949299918136]
  We show that [VO(TPP)] (vanadyl tetraphenylporphyrinate) is a promising system suitable to implement quantum computation algorithms. It embeds an electronic spin 1/2 coupled through hyperfine interaction to a nuclear spin 7/2, both characterized by remarkable coherence.
  arXiv  Detail & Related papers  (2021-03-15T21:38:41Z)
• Open-cavity in closed-cycle cryostat as a quantum optics platform [47.50219326456544]
  We present a fiber-based open Fabry-P'erot cavity in a closed-cycle cryostat exhibiting ultra-high mechanical stability. This set of results manifests open-cavity in a closed-cycle cryostat as a versatile and powerful platform for low-temperature cavity QED experiments.
  arXiv  Detail & Related papers  (2021-03-09T18:41:48Z)
• $\mathcal{P}$,$\mathcal{T}$-odd effects for RaOH molecule in the excited vibrational state [77.34726150561087]
  Triatomic molecule RaOH combines the advantages of laser-coolability and the spectrum with close opposite-parity doublets. We obtain the rovibrational wave functions of RaOH in the ground electronic state and excited vibrational state using the close-coupled equations derived from the adiabatic Hamiltonian.
  arXiv  Detail & Related papers  (2020-12-15T17:08:33Z)

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.