The weakly interacting S=1/2 dimers system Sr3Cr2O8 has been investigated by
powder neutron diffraction and inelastic neutron scattering. Our data reveal a
structural phase transition below room temperature corresponding to an
antiferro-orbital ordering with nearly 90 degrees arrangement of the occupied
3z^2-r^2 d-orbital. This configuration leads to a drastic reduction of the
inter-dimer exchange energies with respect to the high temperature
orbital-disorder state, as shown by a spin-dimer analysis of the
super-superexchange interactions performed using the Extended Huckel Tight
Binding method. Inelastic neutron scattering reveals the presence of a quasi
non-dispersive magnetic excitation at 5.4 meV, in agreement with the picture of
weakly-interacting dimers