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Ultrafast disordering in Langmuir–Blodgett (LB) films and TlAP (thallium acid phthalate) crystals has been investigated by optical-pump–X-ray-probe experiments using intense femto­second laser pulses. A laser-produced plasma X-ray source at 7.12 Å wavelength is used to study atomic dynamics by subpicosecond time-resolved X-ray diffraction. It is found that a drop of the X-ray diffracted intensity appears with time constants from below 600 fs up to a few tens of picoseconds in LB films optically excited at laser fluxes from 1.8 to 27 J cm−2. This loss in the diffracted intensity is understood as a displacement of the diffracting atoms by ∼8 Å from their equilibrium position. The response of the TlAP crystal was significantly slower. The relation to the atomic structure of the materials is discussed.

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