We present measurements of the positron two-dimensional angular correl
ation of annihilation radiation (2D-ACAR) in TTF-TCNQ. We report also
theoretical simulations of the 2D-ACAR in which the electron wave func
tions were expressed as TTF or TCNQ molecular orbitals obtained from s
elf-consistent quantum chemical calculations. The positron wave functi
on was calculated taking the charge transfer from TTF to TCNQ as a par
ameter. The best agreement with the experiment is obtained for a charg
e transfer of 0.7 electrons from the TTF to the TCNQ molecules. This i
s larger than the value of 0.55 obtained from a study of the Kohn anom
aly. We investigate also the shape and position of the Fermi surface a
nd conclude that a simple planar Fermi surface is consistent with our
measurements.