Crystallography Reports, Vol. 47, No. 3, 2002, pp. 347–361. From Kristallografiya, Vol. 47, No. 3, 2002, pp. 391–405. Original English Text Copyright © 2002 by Jean-Pierre Vidal, Genevieve Vidal-Valat, Kaarle Kurki-Suonio, Riitta Kurki-Suonio. DIFFRACTION AND SCATTERING OF X-RAY AND SYNCHROTRON RADIATION To the Memory of Riitta Kurki-Suonio Indications of the Magnetic State in the Charge Distributions in MnO, CoO, and NiO. I: Para- and Antiferromagnetism of MnO1 Jean-Pierre Vidal*, Genevieve Vidal-Valat*, Kaarle Kurki-Suonio**, and Riitta Kurki-Suonio**† * Laboratoire d’Analyse Multipolaire des Repartitions de Charges Experimentales, Université Montpellier 2, 34095 Montpellier Cedex 05, France e-mail:
[email protected] ** Physics Department, P.O. Box 9, FIN-00014 University of Helsinki, Finland Received May 28, 2001 Abstract—X-ray diffraction intensities from MnO and CoO were measured above and below their Néel tem- peratures and from NiO, below the Néel temperature. To detect possible characteristics of the paramagnetic and antiferromagnetic states of the crystals, the data were subjected to direct multipole analysis of the atomic- charge densities. For MnO, both spherical and nonspherical accumulation-of-charge densities indicate the exchange of the roles played by manganese and oxygen in the magnetic phase transition. Both spherical and nonspherical features characteristic of the ionic nature are inherent in both states. The electron counts of the density peaks correspond to Mn2+ and O1–, with the tenth electron of O2– being distributed in a wider region. In the paramagnetic state, there is an electronic Mn–Mn bond which seems to be formed due to coupling with the tenth electron of O2– and builds up a three-dimensional net of the charge density with the “cages” surround- ing oxygen atoms.