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Structural relaxations are intrinsic to all liquids and glasses. They are thefundamental processes underlying many material properties. However, themechanism of structural relaxations is still unclear due to the experimentaldifficulties in directly characterizing the atomic-scale relaxations. Thelatter exhibit a broad range of timescales from geological times tosub-picoseconds. Here we show that, using split-delay coherent pulses of X-rayfree electron lasers (XFEL), we can achieve the femtosecond temporal andatomic-scale spatial resolutions of the X-ray photon correlation spectroscopy(fs-XPCS). The latter allows us to directly observe atomic-scale relaxationdynamics and determine the intermediate scattering function in a high-fluidityfragile liquid. We find that the beam characteristics of the double pulses fromthe split-delay drift over time, the correction of which is essential to obtainthe accurate intermediate scattering functions from speckle contrasts. Ourfinding demonstrates a new avenue of direct experimental studies of relaxationdynamics with the femtosecond resolution, a 12 orders of magnitude extensionfrom the sub-seconds regime of the synchrotron-based XPCS.

Femtosecond atomic-scale X-ray photon correlation spectroscopy enables direct probing of relaxation dynamics in fragile liquid