Quantum Monte Carlo methods have recently made it possible to calculate the
electronic structure of relatively large molecular systems with very high
accuracy. These large systems range from positron complexes [NH2,Ps] with N
IO electrons to C-20 isomers with 120 electrons, to silicon crystal structu
res of 250 atoms and 1000 valence electrons. The techniques for such calcul
ations and a sampling of applications are reviewed.