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Motivated by the recent developments in terahertz spectroscopy using pump-probe setups, we develop the theory of finite frequency nonlinear electro-optical responses in centrosymmetric metals starting from basic time dependent perturbation theory. We express the nonlinear current kernel as a sum of several causal response functions. These functions cannot be evaluated using perturbative field theory methods. Consequently, we associate each response function with an imaginary time ordered current correlation function, which can be factorized using Wicks theorem. The mapping between the response functions and the correlation functions, suitably analytically continued to real frequencies, is proven exactly. We derive constraints satisfied by the nonlinear current kernel and we prove a generalized $f$-sum rule for the nonlinear conductivity, all of which are consequences of particle number conservation. We apply the theory to compute the gauge invariant nonlinear conductivity of a system of noninteracting electrons in the presence of weak disorder. As special cases of this generalized nonlinear response, we discuss its third harmonic and its instantaneous terahertz Kerr signals. Our formalism can be used to compute the nonlinear conductivity in symmetry broken phases such as density waves and nematic states.
We theoretically study THz-light-driven high-harmonic generation (HHG) in the spin-liquid states of the Kitaev honeycomb model with a magnetostriction coupling between spin and electric polarization. To compute the HHG spectra, we numerically solve t
Chiral magnets, which break both spatial inversion and time reversal symmetries, carry a potential for quadratic optical responses. Despite the possibility of enhanced and controlled responses through the magnetic degree of freedom, the systematic un
Strong optical pulses at mid-infrared and terahertz frequencies have recently emerged as a powerful tool to manipulate and control the solid state and especially complex condensed matter systems with strongly correlated electrons. The recent developm
Nonlinear optical (NLO) responses of topological materials are under active research in recent years. Yet by far most studies focused on the bulk properties, whereas the surface effects and the difference between surface and bulk responses have not b
Chiral topological semimetals are materials that break both inversion and mirror symmetries. They host interesting phenomena such as the quantized circular photogalvanic effect (CPGE) and the chiral magnetic effect. In this work, we report a comprehe