Semi-empirical Quantum Optics for Mid-Infrared Molecular Nanophotonics

Abstract

Nanoscale infrared (IR) resonators with sub-diffraction limited mode volumes and open geometries have emerged as new platforms for implementing cavity quantum electrodynamics (QED) at room temperature. The use of infrared (IR) nano-antennas and tip nanoprobes to study strong light-matter coupling of molecular vibrations with the vacuum field can be exploited for IR quantum control with nanometer and femtosecond resolution. In order to accelerate the development of molecule-based quantum nano-photonic devices in the mid-IR, we develop a generally applicable semi-empirical quantum optics approach to describe light-matter interaction in systems driven by mid-IR femtosecond laser pulses. The theory is shown to reproduce recent experiments on the acceleration of the vibrational relaxation rate in infrared nanostructures, and also provide physical insights for the implementation of coherent phase rotations of the near-field using broadband nanotips. We then apply the quantum framework to develop general tip-design rules for the experimental manipulation of vibrational strong coupling and Fano interference effects in open infrared resonators. We finally propose the possibility of transferring the natural anharmonicity of molecular vibrational levels to the resonator near-field in the weak coupling regime, to implement intensity-dependent phase shifts of the coupled system response with strong pulses. Our semi-empirical quantum theory is equivalent to first-principles techniques based on Maxwell's equations, but its lower computational cost suggests its use a rapid design tool for the development of strongly-coupled infrared nanophotonic hardware for applications ranging from quantum control of materials to quantum information processing.

18 pages, 7 figures

References in corpus (12)

• Photonic quantum technologies
• Ground-state cooling of a micromechanical oscillator: generalized framework for cold damping and cavity-assisted cooling schemes
• Coherent coupling of molecular resonators with a micro-cavity mode
• Cavity QED with Diamond Nanocrystals and Silica Microspheres
• Protecting a Spin Ensemble against Decoherence in the Strong-Coupling Regime of Cavity QED
• Strong phonon-plasmon coupled modes in the graphene/silicon carbide heterosystem
• Macroscopic QED for quantum nanophotonics: Emitter-centered modes as a minimal basis for multi-emitter problems
• Strong coupling in the far-infrared between graphene plasmons and the surface optical phonons of silicon dioxide
• Strong Vibrational Coupling in Room Temperature Plasmonic Resonators
• Enhanced Light-Matter Interaction in B-10 Monoisotopic Boron Nitride Infrared Nanoresonators
• Combining density functional theory with macroscopic QED for quantum light-matter interactions in 2D materials
• Generalization of the Tavis-Cummings model for multi-level anharmonic systems

Cited by in corpus (5)

• Generalization of the Tavis-Cummings model for multi-level anharmonic systems: insights on the second excitation manifold
• Nanocavities for Molecular Optomechanics: their fundamental description and applications
• Open quantum dynamics of strongly coupled oscillators with multi-configuration time-dependent Hartree propagation and Markovian quantum jumps
• Coherent anharmonicity transfer from matter to light in the THz regime
• Impact of light-matter coupling strength on the efficiency of microcavity OLEDs: A unified quantum master equation approach