We have measured the momentum distribution of the electron-positron an
nihilating pair in diamond as a function of crystallographic orientati
on, using the Doppler broadening technique of positron annihilation sp
ectroscopy. A 1% variation in the longitudinal projection of the momen
tum distribution was observed as the sample was rotated about the [110
] axis. This anisotropic distribution shows an excellent agreement wit
h a theoretical calculation performed based on two component density f
unctional theory in the local density approximation. The results sugge
st strongly that the bulk positron density, though delocalized and inh
omogeneous, has sufficient amplitude at the intra-bond regions such th
at the annihilation characteristics are dominated by the bond electron
density and momentum distribution.