Recent developments in coupled cluster nonlinear response theory opened for the first time a route to accurate and systematic ab initio calculations of nonlinear optical and magneto-optical properties. The inclusion of the frequency-dependence (dispersion) at an electron correlated level and the use of systematic correlation consistent basis sets made it possible to achieve accuracies close to those of the best available experiments. The approach has in the mean time been applied to a number of nonlinear properties including frequency-dependent first and second hyperpolarizabilities, fifth harmonic generation, electric-field-gradient-induced birefringence, two-photon absorption, magnetic circular dichroism, Verdet constants, Cotton-Mouton constants, Kerr and ESHG second virial coefficients, etc. Due to the quartic order of the coupled cluster equations, coupled cluster response theory can be cast into a lego-brick like structure with only a limited number of basic building blocks. This allowed to implement high-order response functions which have not been accessible before on an electron correlated level. We give a short review of the latest developments of coupled cluster nonlinear response theory and present a selected number of applications covering electric-field-induced second-harmonic generation, dc Kerr effect, degenerate four wave mixing, third-harmonic and fifth-harmonic generation and electric-field-gradient-induced birefringence to illustrate the strength of the approach.
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