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A comprehensive X-ray investigation of the crystal structure of naphthalene is described, in which all the reflexions that lie within the reach of Cu K[alpha] radiation have been examined. Moving-film photographic methods and visual estimates of intensities by independent observers were employed. From the results a total of 644 structure factozs out of a possible 832 have been evaluated, giving 129 structure factors per atom of the asymmetric unit. From the earlier two-dimensional approximation to the naphthalene structure it has been possible to assign phase constants to 612 of the factors with reasonable certainty. These results form the basis of a new three-dimensional determination of the structure which is described in Part II.
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