The theory of pump-probe diffraction experiments shows that probabilit
y density distributions of vibrational wave functions are experimental
ly observable. In the experiment a laser prepares a molecule in a sele
cted vibrational state, in either the same or a different electronic m
anifold. The diffraction pattern of the molecule in the excited state
is the Fourier transform image of the nuclear probability density dist
ribution, as determined by the vibrational eigenfunction of the molecu
le. This suggests the possibility to directly observe components of mo
lecular vibrational wave functions. Model calculations illustrate the
concept on iodine molecules, and sodium dimers. The relevance to time-
resolved pump-probe experiments that prepare vibrational wave packets
is discussed. (C) 1998 American Institute of Physics.