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Single-crystal time-of-flight (TOF) neutron diffraction data have been collected for Cr3Si and MnF2 with the Argonne Intense Pulsed Neutron Source. The purpose of this study was to test the accuracy of the TOF technique by a comparison with results from recent γ-ray, X-ray and neutron diffraction experiments. The results show that for simple crystal structures the positional and thermal parameters obtained from TOF data approach those obtained by other diffraction methods.