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We show that time-resolved x-ray scattering from molecules prepared in asuperposition of electronic states moving through an avoided crossing has newfeatures not found in diffraction from the corresponding classical mixed state.Photoabsorption in molecular iodine at 520 nm produces a superposition of twodipole-allowed nearly degenerate electronic states, which interact due tonon-adiabatic coupling. We show experimental evidence that the mixing of thenuclear wavepackets from the two electronic states at the avoided crossingleads to ultrafast changes in the angular composition of the scatteringpattern. This provides a novel means to study transitions in excited molecularsystems. We reconstruct a movie of the nuclear probability density arising fromthis interference.

Filming non-radiative population transfer: Time-resolved x-ray scattering near an avoided crossing