Magnetic Structure and Exchange Interactions in Quasi-One-Dimensional MnCl2(urea)2

Manson, Jamie L.; Huang, Qing-zhen; Brown, Craig M.; Lynn, Jeffrey W.; Stone, Matthew B.; Singleton, John; Xiao, Fan

doi:10.1021/acs.inorgchem.5b02162

Title: Magnetic Structure and Exchange Interactions in Quasi-One-Dimensional MnCl₂(urea)₂

Journal Article · Tue Dec 08 00:00:00 EST 2015 · Inorganic Chemistry

DOI:https://doi.org/10.1021/acs.inorgchem.5b02162· OSTI ID:1457261

Manson, Jamie L. ^[1]; Huang, Qing-zhen ^[2]; Brown, Craig M. ^[3]; Lynn, Jeffrey W. ^[2]; Stone, Matthew B. ^[4];

^[5]; Xiao, Fan ^[6]

Eastern Washington University, Cheney, WA (United States)
National Inst. of Standards and Technology (NIST), Gaithersburg, MD (United States)
National Inst. of Standards and Technology (NIST), Gaithersburg, MD (United States); Univ. of Delaware, Newark, DE (United States)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
Durham Univ. (United Kingdom)

MnCl₂(urea)₂ is a new linear chain coordination polymer that exhibits slightly counter-rotated Mn₂Cl₂ rhomboids along the chain-axis. The material crystallizes in the noncentrosymmetric orthorhombic space group Iba2, with each Mn(II) ion equatorially surrounded by four Cl^- that lead to bibridged ribbons. Urea ligands coordinate via O atoms in the axial positions. Hydrogen bonds of the Cl···H–N and O···H–N type link the chains into a quasi-3D network. Magnetic susceptibility data reveal a broad maximum at 9 K that is consistent with short-range magnetic order. Pulsed-field magnetization measurements conducted at 0.6 K show that a fully polarized magnetic state is achieved at B_sat = 19.6 T with another field-induced phase transition occurring at 2.8 T. Zero-field neutron diffraction studies made on a powdered sample of MnCl₂(urea)₂ reveal that long-range magnetic order occurs below T_N = 3.2(1) K. Additional Bragg peaks due to antiferromagnetic (AFM) ordering can be indexed according to the Ib'a2' magnetic space group and propagation vector τ = [0, 0, 0]. Rietveld profile analysis of these data revealed a Néel-type collinear ordering of Mn(II) ions with an ordered magnetic moment of 4.06(6) μB (5 μB is expected for isotropic S = 5/2) oriented along the b-axis, i.e., perpendicular to the chain-axis that runs along the c-direction. Owing to the potential for spatial exchange anisotropy and the pitfalls in modeling bulk magnetic data, we analyzed inelastic neutron scattering data to retrieve the exchange constants: J_c = 2.22 K (intrachain), J_a = -0.10 K (interchain), and D = -0.14 K with J > 0 assigned to AFM coupling. This J configuration is most unusual and contrasts the more commonly observed AFM interchain coupling of 1D chains.

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Research Organization:: Los Alamos National Laboratory (LANL), Los Alamos, NM (United States); Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC52-06NA25396; AC05-00OR22725

OSTI ID:: 1457261

Alternate ID(s):: OSTI ID: 1528743

Report Number(s):: LA-UR-15-27162

Journal Information:: Inorganic Chemistry, Vol. 54, Issue 24; ISSN 0020-1669

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 17 works

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