  In this paper we motivate, formulate and analyze the Multi-Configuration
Time-Dependent Hartree-Fock (MCTDHF) equations for molecular systems under
Coulomb interaction. They consist in approximating the N-particle Schrodinger
wavefunction by a (time-dependent) linear combination of (time-dependent)
Slater determinants. The equations of motion express as a system of ordinary
differential equations for the expansion coefficients coupled to nonlinear
Schrodinger-type equations for mono-electronic wavefunctions. The invertibility
of the one-body density matrix (full-rank hypothesis) plays a crucial role in
the analysis. Under the full-rank assumption a fiber bundle structure shows up
and produces unitary equivalence between convenient representations of the
equations. We discuss and establish existence and uniqueness of maximal
solutions to the Cauchy problem in the energy space as long as the density
matrix is not singular. A sufficient condition in terms of the energy of the
initial data ensuring the global-in-time invertibility is provided (first
result in this direction). Regularizing the density matrix breaks down energy
conservation, however a global well-posedness for this system in L^2 is
obtained with Strichartz estimates. Eventually solutions to this regularized
system are shown to converge to the original one on the time interval when the
density matrix is invertible.
