This book contains the transcripts of the lectures presented at the NATO Advanced study Institute on "Computational Techniques in Quantum Chemistry and Molecular Physics," held at Ramsau, Germany, 4th - 21st Sept. 1974. Quantum theory was developed in the early decades of this century and was first applied to problems in chemistry and molecular physics as early as 1927. It soon emerged however, that it was impossible to con sider any but the simplest systems in any quantita tive detail because of the complexity of Schrodinger's equation which is the basic equation for chemical and molecular physics applications. This remained the si tuation until the development, after 1950, of elec tronic digital computers. It then became possible to attempt approximate solutions of Schrodinger's equa tion for fairly complicated systems, to yield results which were sufficiently accurate to make comparison with experiment meaningful. Starting in the early nineteen sixties in the United States at a few centres with access to good computers an enormous amount of work went into the development and implementation of schemes for approximate solu tions of Schrodinger's equation, particularly the de velopment of the Hartree-Fock self-consistent-field scheme. But it was soon found that the integrals needed for application of the methods to molecular problems are far from trivial to evaluate and cannot be easily approximated."

"Imagination and shrewd guesswork are powerful instruments for acquiring scientific knowledge . . . " 1. H. van't Hoff The last decades have witnessed a rapid growth of quantum chemistry and a tremendous increase in the number of very accurate ab initio calculations of the electronic structure of molecules yielding results of admirable accuracy. This dramatic progress has opened a new stage in the quantum mechanical description of matter at the molecular level. In the first place, highly accurate results provide severe tests of the quantum mecha nics. Secondly, modern quantitative computational ab initio methods can be synergetically combined with various experimen tal techniques thus enabling precise numerical characterization of molecular properties better than ever anticipated earlier. However, the role of theory is not exhausted in disclosing the fundamental laws of Nature and production of ever increasing sets of data of high accuracy. It has to provide additionally a means of systematization, recognition of regularities, and ratio nalization of the myriads of established facts avoiding in this way complete chaos. Additional problems are represented by molecular wavefunctions provided by the modern high-level computational quantum chemistry methods. They involve, in principle, all the information on molecular system, but they are so immensely complex that can not be immediately understood in simple and physically meaningful terms. Both of these aspects, categorization and interpretation, call for conceptual models which should be preferably pictorial, transparent, intuitively appealing and well-founded, being sometimes useful for semi quantitative purposes."

This book contains the transcripts of the lectures presented at the NATO Advanced study Institute on "Computational Techniques in Quantum Chemistry and Molecular Physics," held at Ramsau, Germany, 4th - 21st Sept. 1974. Quantum theory was developed in the early decades of this century and was first applied to problems in chemistry and molecular physics as early as 1927. It soon emerged however, that it was impossible to con sider any but the simplest systems in any quantita tive detail because of the complexity of Schrodinger's equation which is the basic equation for chemical and molecular physics applications. This remained the si tuation until the development, after 1950, of elec tronic digital computers. It then became possible to attempt approximate solutions of Schrodinger's equa tion for fairly complicated systems, to yield results which were sufficiently accurate to make comparison with experiment meaningful. Starting in the early nineteen sixties in the United States at a few centres with access to good computers an enormous amount of work went into the development and implementation of schemes for approximate solu tions of Schrodinger's equation, particularly the de velopment of the Hartree-Fock self-consistent-field scheme. But it was soon found that the integrals needed for application of the methods to molecular problems are far from trivial to evaluate and cannot be easily approximated."