Christof Hättig
Forschungszentrum Karlsruhe, Institute of Nanotechnology, P.O. Box 3640,D-76021 Karlsruhe, Germany

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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• Frequency-dependent first hyperpolarizabilities using coupled cluster quadratic response theory
  
  
• Response functions from Fourier component variational perturbation theory applied to a time-averaged quasienergy
  
  
• Coupled Cluster calculations of Verdet Constants
  
  
• Frequency-dependent second hyperpolarizabilities using coupled cluster cubic response theory
  
  
• Estimate of the experimental static hyperpolarizability of Neon based on coupled cluster response calculations
  
  
• Multiphoton transition moments and absorption cross sections in coupled cluster response theory employing variational transition moment functional
  
  
• Coupled cluster response calculations of twophoton transition probability rate constants for helium, neon and argon
  
  
• Dispersion formulas for hyperpolarizability averages
  
  
• Coupled cluster calculations of the frequency-dependent second hyperpolarizabilities of Ne, Ar, N2 and CH4
  
  
• A basis set study of coupled cluster and full configuration interaction calculations of molecular electric properties of BH
  
  
• Dispersion coefficients for first hyperpolarizabilities using coupled cluster quadratic response theory
  
  
• Derivation of coupled cluster excited states response functions and multiphoton transition moments between two excited states as derivatives of variational functionals
  
  
• Static and frequency-dependent polarizabilities of the lowest excited states of s-tetrazine and pyrimidine using coupled cluster response theory
  
  
• Ground and excited state polarizabilities and dipole transition moments of benzene from coupled cluster response theory
  
  
• Dispersion formulas for the second hyperpolarizability components
  
  
• Dispersion coefficients for second hyperpolarizabilities using coupled cluster cubic response theory
  
  
• Coupled cluster investigation of the electric field gradient induced birefringence of H2, N2, CH4 and C2H4
  
  
• Polarizabilities and first hyperpolarizabilities of HF, Ne and BH from full configuration interaction and coupled cluster calculations
  
  
• Dispersion coefficients for polarizabilities, and first and second hyperpolarizabilities using full configuration interaction theory
  
  
• The electric-field-gradient-induced birefringence of Helium, Neon, Argon and SF6
  
  
• Correlated frequency-dependent first hyperpolarizability of small push-pull conjugated chains
  
  
• Ab initio study of the electric-field-gradient-induced birefringence of a polar molecule: CO
  
  

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