A reliable and highly efficient ab initio tight-binding-like electronic structure calculation method is developed. The method starts from a similar approach outlined by Horsfield ( Phys. Rev. B 56, 6594(1997)), but integral evaluations for the exchange-correlation matrix elements are achieved with reasonable accuracy by higher order many-center expansions. All the integrals are obtained by the use of look-up tables and the efficiency of the calculation is further improved by optimizing the way to choose the integrals in the look-up tables. Calculations on molecular properties, such as equilibrium geometries, dipole moments, and the reaction energies for hydrogenation reactions for a series of molecules containing H, C, N, and O atoms show that the method thus developed can be used as a general tool for the electronic structure calculations.

References

Tu & Laaksonen, “Towards first-principles simulations of macromolecules: From reliable semi-empirical schemes to ab initio TB-DFT”.
(Eds. C. Chipot, R. Elber, A. Laaksonen, B. Leimkuhler, A. Mark, T. Schlick, C. Schuette, R. Skeel),  
Lecture Notes in Computational Science & Engineering, Springer Verlag, 2005

Yaoquan Tu, Sven. P. Jacobsson and Aatto Laaksonen,
Efficient ab initio tight-binding-like method for electronic structure calculations.
Phys. Rev. B 74, 205104 (2006)