current work employs the Hay-Wadt-type ab-initio effective core potentials which are more suitable for the HF-type approaches. Among other factors, use of pseudopotentials and basis sets which are more appropriate for the DFT approaches, may alleviate some of the discrepancies encountered here and an undertaking along this direction may be initiated in future. Furthermore, large deviations in atomization energies have also been found in other recent DFT works involving all-electron calculations and more extended basis sets as well (see for example [45]). In any case, this is an evolving process and does not interfere with the main objective of the present work. Also note that there may be some cancellation of errors in the LDA case. Finally note that the extension of this approach to the “all-electron” atomic, molecular calculations as well as for very large systems would be relatively difficult compared to the present pseudopotential case in terms of the grid requirement, because of the presence of extra core electrons. Nevertheless reasonable full calculation of small to medium molecules are possible. This is suggested from some of our preliminary studies in this direction which I am currently engaged into and may be considered in some future communication. Pseudopotential density functional calculations were performed for atoms and molecules within the LCGTF framework using CCG in conjunction with an accurate, efficient Fourier convolution technique to represent the classical Hartree potential in real grid. In essence, our previous work (I) on the LDA XC functionals has been extended to test its performance and validity in the case of gradient-corrected XC functionals which would be necessary for its further applications to realistic physical situations. For this purpose, the widely used BLYP XC functional was chosen. The calculated results of a variety of quantities such as energy components, eigenvalues, potential energy curves, ionization energies, atomization energies clearly reveal that, they are practically of the same quality as obtained from the available theoretical methods. Furthermore, companion LDA and BLYP calculations were performed for a large number of molecules (41) to illustrate its scope of applicability for a broad range of systems. Comparison with experiments has been made wherever possible. Additionally, for all the molecules studied, the LBVWN results show significant improvements in the HOMO energies. This has important relevance to our prospective future works on studying IV. CONCLUDING REMARKS 15