CHEMICAL APPLICATIONS OF DENSITY FUNCTIONAL THEORY - COMPARISON TO EXPERIMENT, HARTREE-FOCK, AND PERTURBATION-THEORY

Density functional theory (DFT) offers an alternative method for the quantum mechanical computation of chemical properties. Although initial results have been very positive, the method still lacks the long history of calibration which exists for more conventional methods. This calibration is important for identifying particular strengths and weaknesses of each method. The present study attempts to establish such a calibration for DFT. Results are obtained for structures, vibrational frequencies, and heats of reaction. Results are generally comparable in accuracy to MP2 calculations. Certain properties are reproduced rather poorly by local density functional methods; the predicted values of some of these properties are improved by the use of nonlocal corrections, added perturbatively at the end of the local DFT calculation.