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An instrument and software algorithm are described for the purpose of characterization of large single crystals at the Alignment Facility of the ISIS spallation neutron source. A method for both characterizing the quality of the sample and aligning it in a particular scattering plane is introduced. A software package written for this instrument is presented, and its utility is demonstrated by way of an example of the structural characterization of large single crystals of Pb(Mg 1/3 Nb 2/3 )O 3 . Extensions and modifications of characterization instruments for future improved beamlines are suggested. It is hoped that this software will be used by the neutron community for pre‐characterizing large single crystals for spectroscopy experiments and that in the future such a facility will be included as part of the spectroscopy suite at other spallation neutron sources.

Alignment facility and software for single‐crystal time‐of‐flight neutron spectroscopy