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000189315 0247_ $$2doi$$a10.1021/ic502061w
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000189315 1001_ $$0P:(DE-HGF)0$$aKazem, Nasrin$$b0
000189315 245__ $$aEu$_{9}$Cd$_{4–x}$CM$_{2+x–y□y}$Sb$_{9}$: Ca$_{9}$Mn$_{4}$Bi$_{9}$-Type Structure Stuffed with Coinage Metals (Cu, Ag, and Au) and the Challenges with Classical Valence Theory in Describing These Possible Zintl Phases
000189315 260__ $$aWashington, DC$$bAmerican Chemical Society$$c2015
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000189315 520__ $$aThe synthesis, crystal structure, magnetic properties, and europium Mössbauer spectroscopy of the new members of the 9–4–9 Zintl family of Eu9Cd4–xCM2+x–y□ySb9 (CM = coinage metal: Au, Ag, and Cu) are reported. These compounds crystallize in the Ca9Mn4Bi9 structure type (9–4–9) with the 4g interstitial site almost half-occupied by coinage metals; these are the first members in the 9–4–9 family where the interstitial positions are occupied by a monovalent metal. All previously known compounds with this structure type include divalent interstitials where these interstitials are typically the same as the transition metals in the anionic framework. Single-crystal magnetic susceptibility data indicate paramagnetic behavior for all three compounds with antiferromagnetic ordering below 10 K (at 100 Oe) that shifts to lower temperature (<7 K) by applying a 3 T magnetic field. 151Eu Mössbauer spectra were collected on polycrystalline powder samples of Eu9Cd4–xCM2+x–y□ySb9 at 50 and 6.5 K in order to evaluate the valence of Eu cations. Although the Zintl formalism states that the five crystallographically distinct Eu sites in Eu9Cd4–xCM2+x–y□ySb9 should bear Eu2+, the Mössbauer spectral isomer shifts are clearly indicative of both 2+ and 3+ valence of the Eu cations with the Cu- and Au-containing compounds showing higher amounts of Eu3+. This electronic configuration leads to an excess of negative charge in these compounds that contradicts the expected valence-precise requirement of Zintl phases. The spectra obtained at 6.5 K reveal magnetic ordering for both Eu2+ and Eu3+. The field dependence of Eu2+ indicates two distinct magnetic sublattices, with higher and lower fields, and of a small field for Eu3+. The site symmetry of the five Eu sites is not distinguishable from the Mössbauer data.
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000189315 536__ $$0G:(DE-HGF)POF3-6213$$a6213 - Materials and Processes for Energy and Transport Technologies (POF3-621)$$cPOF3-621$$fPOF III$$x2
000189315 536__ $$0G:(DE-HGF)POF3-6G4$$a6G4 - Jülich Centre for Neutron Research (JCNS) (POF3-623)$$cPOF3-623$$fPOF III$$x3
000189315 536__ $$0G:(DE-HGF)POF3-6212$$a6212 - Quantum Condensed Matter: Magnetism, Superconductivity (POF3-621)$$cPOF3-621$$fPOF III$$x4
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000189315 7001_ $$0P:(DE-HGF)0$$aHurtado, Antonio$$b1
000189315 7001_ $$0P:(DE-Juel1)144500$$aKlobes, Benedikt$$b2
000189315 7001_ $$0P:(DE-HGF)0$$aKauzlarich, Susan M.$$b3$$eCorresponding Author
000189315 7001_ $$0P:(DE-Juel1)130706$$aHermann, Raphael$$b4
000189315 773__ $$0PERI:(DE-600)1484438-2$$a10.1021/ic502061w$$gVol. 54, no. 3, p. 850 - 859$$n3$$p850 - 859$$tInorganic chemistry$$v54$$x1520-510X$$y2015
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