Density-functional theory of linear and nonlinear time-dependent molecular properties

摘要: We present density-functional theory for linear and nonlinear response functions using an explicit exponential parametrization of the density operator. The are derived two alternative variation principles, namely, Ehrenfest principle quasienergy principle, giving different but numerically equivalent formulas. present, first time, calculations dynamical hyperpolarizabilities hybrid functionals including exchange-correlation at general gradient-approximation level fractional exact Hartree–Fock exchange. Sample presented hyperpolarizability para-nitroaniline molecule a porphyrin push–pull molecule, showing good agreement with available experimental data.