EFFECT OF CONFIGURATION-INTERACTION ON CALCULATED POLARIZED UV-VIS ABSORPTION-SPECTRA - A MOLECULAR-DYNAMICS BASED STUDY

Inclusion of configuration interaction through the use of second-order perturbation theory in the calculation of the 364x364 energy matrix f or Nd3+ in Nd3+:YAG and Nd3+:LiYF4 is shown to improve agreement with experimentally observed polarized W-VIS absorption spectra significant ly. The effect of taking account of electric-dipole and inhomogeneous dielectric mechanisms has been assessed in calculating the polarized o scillator strengths. The A(tp) parameters have been calculated by dire ct summation over the multipole-expanded environments, and the polariz ed oscillator strengths calculated for a sequence of molecular-dynamic s generated environments. The correlation coefficients are 0.55, 0.61, and 0.63 for Nd3+:YAG, sigma-polarized Nd3+:LiYF4, and pi-polarized N d3+:LiYF4, respectively.