Magnetic properties of the Kagomé mixed compounds Co x Ni 1-x 3 V 2 O 8 N. Qureshi* Institute for Materials Science, University of Technology, Petersenstrasse 23, D-64287 Darmstadt, Germany and Institut Max von Laue-Paul Langevin, 6 rue Jules Horowitz, BP 156, 38042 Grenoble Cedex 9, France H. Fuess and H. Ehrenberg Institute for Materials Science, University of Technology, Petersenstrasse 23, D-64287 Darmstadt, Germany T. C. Hansen and C. Ritter Institut Max von Laue-Paul Langevin, 6 rue Jules Horowitz, BP 156, 38042 Grenoble Cedex 9, France K. Prokes and A. Podlesnyak Hahn-Meitner-Institute, Glienicker Strasse 100, D-14109 Berlin, Germany D. Schwabe Institute for Physics, Justus Liebig University, Heinrich-Buff-Ring 16, D-35392 Giessen, Germany Received 23 September 2006; published 19 December 2006 The magnetic properties of the mixed compounds Co x Ni 1-x 3 V 2 O 8 CNVOinvestigated by magnetization and neutron diffraction measurements are presented. Unlike their parent compounds Ni 3 V 2 O 8 NVOand Co 3 V 2 O 8 CVO, only one magnetic phase transition into an antiferromagnetic phase was detected for powder samples with x = 0.27, 0.52, and 0.76. The magnetic structures are modulated according to a propagation vector k = ,0,0with being dependent on the composition parameter x. Furthermore, magnetization data of a CVO single crystal is featured, which is qualitatively different from previous publications and exhibits a controver- sial aspect concerning the behavior of the curve under an applied magnetic field along the b axis. DOI: 10.1103/PhysRevB.74.212407 PACS numbers: 75.25.z, 75.30.Gw, 75.30.Kz, 75.60.Ej I. INTRODUCTION The orthooxovanadates of the 3d transition metals M, which crystallize in the orthorhombic space group Cmca, represent magnetic lattices labeled as Kagomé staircases. The crystal structure of these M 3 V 2 O 8 compounds has been determined by Fuess et al. 1 and again by Sauerbrei et al. 2 The structure is characterized by edge-sharing MO 6 octahe- dra, which form buckled layers separated by nonmagnetic V 5+ ions. Because of the structural anisotropy and two non- equivalent magnetic sites within the staircases Fig. 1, these compounds differ from the ideal Kagomé net, which consists of corner-sharing equilateral triangles. The reduced symme- try relieves the geometrical frustration and results in long- range ordered magnetic structures and rich H-T phase diagrams. 3 Although the parent compounds NVO and CVO have been exhaustively investigated, 110 only structural data about Co 0.5 Ni 0.5 3 V 2 O 8 has been published 11 concerning the cation distribution on the two M sites. In the present work, magnetization measurements of three powder samples of the mixed compounds with x = 0.27, 0.52, and 0.76 were carried out and compared to the pure Ni and Co compounds. The results were confirmed by neutron powder diffraction experi- ments revealing more information about the magnetic struc- tures. In addition, magnetization measurements of CVO are presented that differ from previously published data. 5,8 Pos- sible reasons for this discrepancy will be discussed. II. EXPERIMENTAL Powder samples of CVO and CNVO were synthesized with a reported technique 8 by mixing NiO and CoO in the desired ratio. Single crystals of CVO were grown by the Czochralski method. The crystal structures of the powder samples were investigated by neutron diffraction experi- ments. Therefore, measurements were carried out at the high- resolution neutron powder diffractometers D1A CNVOand D2B CVOat the Institut Laue-Langevin using a wave- length of 1.911 Å at 20 K and 2.3974 Å at 14 K, respec- tively. The single-crystal structure was checked by x-ray dif- fraction on the single-crystal diffractometer Oxford Diffraction XCALIBUR with Mo K at 100 K. The mag- netic phase transitions were examined by magnetization measurements using a superconducting quantum interference device SQUIDmagnetometer Quantum Design. The magnetic structures of CNVO were studied at zero magnetic field by neutron powder diffraction experiments at D1A. Ad- ditionally, neutron single-crystal diffraction experiments on CVO two-axis diffractometer E4 at the Hahn-Meitner- Institut in Berlinwere used to reveal the magnetic phase transitions due to the temperature dependence of the propa- gation vector. FIG. 1. Color onlineVisualization of a Kagomé staircase with the two crystallographic M sites M1 light gray blue, M2 dark gray blue and the different distances between them. PHYSICAL REVIEW B 74, 212407 2006 1098-0121/2006/7421/2124074©2006 The American Physical Society 212407-1