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Short-wavelength free-electron lasers with their ultrashort pulses at highintensities have originated new approaches for tracking molecular dynamics fromthe vista of specific sites. X-ray pump X-ray probe schemes even allow toaddress individual atomic constituents with a 'trigger'-event that preludes thesubsequent molecular dynamics while being able to selectively probe theevolving structure with a time-delayed second X-ray pulse. Here, we use alinearly polarized X-ray photon to trigger the photolysis of a prototypicalchiral molecule, namely trifluoromethyloxirane (C$_3$H$_3$F$_3$O), at thefluorine K-edge at around 700 eV. The evolving fluorine-containing fragmentsare then probed by a second, circularly polarized X-ray pulse of higher photonenergy in order to investigate the chemically shifted inner-shell electrons ofthe ionic motherfragment for their stereochemical sensitivity. Weexperimentally demonstrate and theoretically support how two-color X-ray pumpX-ray probe experiments with polarization control enable XFELs as tools forchiral recognition.

Site-specific Interrogation of an Ionic Chiral Fragment During Photolysis Using an X-ray Free-Electron Laser