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Instrumentation for measuring the X-ray diffraction pattern of optically excited crystals is described. The experiment uses a high-power (~1 W) laser and a single-crystal diffractometer equipped with a helium cryostat (T < 70 K). The laser beam is modulated by a mechanical chopper and the diffraction signal gated in synchronization with the chopper phase. The modulation method is capable of observing small changes (down to about 0.01%) in the structure factors upon excitation of a fraction of the molecules in the crystal, given adequate counting statistics. The technique can be used for relatively long lived electronic excited states (τ ≃ 0.1–10 ms). The optical system is also suitable for time-resolved measurements using the time structure of synchrotron radiation.

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