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Hartree-Fock pairings all tested on small lattices; large lattices (&geq 3-10x smaller dimensions of lattice) yield density matrices which are very likely to contain substantial electron-hole repulsion (12). Hartree-Fock gives quite good energies for a much larger number of systems than the density matrix method (13). Density matrix method : Hartree-Fock mean-field method. This is one of the simplest methods for describing a many-body system (first-order, least-squares approximation to the electron-electron repulsion), the only difficulty is that for large systems it is still not very accurate. It has been intensively used in quantum chemistry and molecular physics (14). Basic approach : In this method, which is a direct application of Hartree-Fock, the ansatz is the same as in Hartree-Fock, the only difference is that the electron-electron repulsion is approximate, using spherical and atomic-like orbitals. Its goal is to provide a good variational wavefunction for a system of fermions which is also suitable for use in numerical calculations of large systems. In these cases, the Coulomb repulsion can be calculated at first order in the density by counting the number of particles on overlapping spheres, since the density changes very little inside a sphere (Fig. In general, the ROC analysis becomes more accurate as the accuracy of the approximation to the Coulomb repulsion is improved, and numerical tests have shown that an optimized Coulomb function (13) performs well. In cases where the error of the Coulomb function is below 10%, a variational wavefunction is usually a good approximation. The wavefunction is built as follows : the system is divided into discrete, overlapping spheres, represented by a single Slater determinant (22). The positions of the sphere centres can be optimised, by minimising the total energy, by gradient descent methods (22). In the first experiments on quantum dots (23), molecules and aggregates (24,25), the molecular orbitals were simply Gaussian functions (the most primitive possible), which has the advantage of giving a simple yet excellent variational wavefunction. The atomic orbitals were linear combinations of atomic orbitals, generated by the standard fast atomic code at the centre. We have first investigated the energy minimisation for spheres of various sizes (Fig. For the cases where the error is below 10%, the variational wavefunction describes the system quite accurately. This is not
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