Complete polarizabilities and first hyperpolarizabilities (which include zero-point-vibrational averaging and other vibrational corrections) have been calculated at the self-consistent-held and Moller-Plesset second order perturbation levels of approximation for CH4, CF4, and CCl4. As well as the static values, alpha(- omega;omega), beta(- omega;omega,0), and beta(-2 omega;omega,omega) have also been determined. The values of beta(-2 omega;omega,omega) for CCl4 are germane to a proposed standard for the determination of nonlinear optical properties in solution. For CCl4, our best estimate of beta(-2 omega;omega,omega) at (h) over bar omega = 0.040 a.u. is 13.6 a.u., the experimentally-derived gas value at (h) over bar omega = 0.043 a.u, is 20.7 +/- 1.6 a.u. This latter value has been used to substantiate the proposed liquid phase value.