Diffraction-Detected Sum Frequency Generation: Novel Ultrafast X-ray Probe of Molecular Dynamics.

We propose a novel time-resolved diffraction technique based on sum frequency generation that combines an optical pump with an X-ray stimulated Raman probe. Simulations are presented for formyl fluoride, which is nonchiral in the ground state and evolves into a chiral nonplanar structure in the first excited state upon excitation by a circularly polarized UV pump. A coherently controlled elliptically polarized pump is used to prepare the molecule in a selected enantiomer and the chiral interconversion dynamics is then monitored by the probe diffraction.