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Free-electron laser hard X-ray light sources can provide high fluence,femtosecond pulses, enabling the time-resolved probing of structural dynamicsand elementary relaxation processes in molecules. Traditional X-ray elasticscattering from crystals in the ground state consists of sharp Braggdiffraction peaks that arise from pairs of molecules and reveal the groundstate charge density. Scattering of ultrashort X-ray pulses from gases,liquids, and even single molecules is more complex and involves both single-and two- molecule contributions, diffuse (non-Bragg) features, elastic andinelastic components, contributions of electronic coherences in nonstationarystates, and interferences between scattering off different states (heterodynedetection). We present a unified description that covers all these processesand discuss their relative magnitudes for gas-phase NaI. Conditions for theobservation of holographic (heterodyne) interference, which has been recentlydiscussed [1], are clarified.

Heterodyne-Detected Ultrafast X-Ray Diffraction and Scattering from Nonstationary States