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We present an ab initio method for computing vibro-polariton and phonon-polariton spectra of molecules and solids coupled to the photon modes of optical cavities. We demonstrate that if interactions of cavity photon modes with both nuclear and electronic degrees of freedom are treated on the level of the cavity Born–Oppenheimer approximation, spectra can be expressed in terms of the matter response to electric fields and nuclear displacements, which are readily available in standard density functional perturbation theory implementations. In this framework, results over a range of cavity parameters can be obtained without the need for additional electronic structure calculations, enabling efficient calculations on a wide range of parameters. Furthermore, this approach enables results to be more readily interpreted in terms of the more familiar cavity-independent molecular electric field response properties, such as polarizability and Born effective charges, which enter into the vibro-polariton calculation. Using corresponding electric field response properties of bulk insulating systems, we are also able to obtain the Γ point phonon-polariton spectra of two dimensional (2D) insulators. Results for a selection of cavity-coupled molecular and 2D crystal systems are presented to demonstrate the method. 

Abstract Motivated by recent experimental demonstrations of Floquet topological insulators, there have been several theoretical proposals for using structured light, either spatial or spectral, to create other properties such as flat bands and vortex states. In particular, the generation of vortex states in a massive Dirac fermion insulator irradiated by light carrying nonzero orbital angular momentum (OAM) has been proposed. Here, we evaluate the orbital magnetization and optical conductivity as physical observables for such a system. We show that the OAM of light induces nonzero orbital magnetization and current density. The orbital magnetization density increases linearly as a function of the OAM degree. In certain regimes, we find that orbital magnetization density is independent of the system size, width, and Rabi frequency of light. It is shown that the orbital magnetization arising from our Floquet theory is large and can be probed by magnetometry measurements. Furthermore, we study the optical conductivity for various types of electron transitions between different states such as vortex, edge, and bulk that are present in the system. Based on the peaks in conductance, a scheme for the detection of vortex states is proposed.