Linear and nonlinear optical response of LiNbO3 calculated from first principles

The dielectric function and second-harmonic generation spectrum of ferroelectric LiNbO₃ are calculated from first principles. The calculations are based on the electronic structure obtained within density functional theory. The use of the GW approach to account for quasiparticle effects and the subsequent solution of the Bethe-Salpeter equation lead to a dielectric function in excellent agreement with measured data. The second harmonic generation spectrum calculated within the independent (quasi) particle approximation predicts strong nonlinear coefficients for photon energies above about 1.5 eV. The comparison with measured data suggests that the inclusion of self-energy effects in the nonlinear response improves the agreement with experiment.