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Title: Synthesis of a polar ordered oxynitride perovskite

Authors:
; ; ; ; ; ; ;
Publication Date:
Sponsoring Org.:
USDOE
OSTI Identifier:
1372518
Grant/Contract Number:
NA0002006; NA0001974; FG02-99ER45775; AC02-06CH11357
Resource Type:
Journal Article: Publisher's Accepted Manuscript
Journal Name:
Physical Review B
Additional Journal Information:
Journal Volume: 95; Journal Issue: 21; Related Information: CHORUS Timestamp: 2017-06-30 22:11:52; Journal ID: ISSN 2469-9950
Publisher:
American Physical Society
Country of Publication:
United States
Language:
English

Citation Formats

Vadapoo, Rajasekarakumar, Ahart, Muhtar, Somayazulu, Maddury, Holtgrewe, Nicholas, Meng, Yue, Konopkova, Zuzana, Hemley, Russell J., and Cohen, R. E. Synthesis of a polar ordered oxynitride perovskite. United States: N. p., 2017. Web. doi:10.1103/PhysRevB.95.214120.
Vadapoo, Rajasekarakumar, Ahart, Muhtar, Somayazulu, Maddury, Holtgrewe, Nicholas, Meng, Yue, Konopkova, Zuzana, Hemley, Russell J., & Cohen, R. E. Synthesis of a polar ordered oxynitride perovskite. United States. doi:10.1103/PhysRevB.95.214120.
Vadapoo, Rajasekarakumar, Ahart, Muhtar, Somayazulu, Maddury, Holtgrewe, Nicholas, Meng, Yue, Konopkova, Zuzana, Hemley, Russell J., and Cohen, R. E. Fri . "Synthesis of a polar ordered oxynitride perovskite". United States. doi:10.1103/PhysRevB.95.214120.
@article{osti_1372518,
title = {Synthesis of a polar ordered oxynitride perovskite},
author = {Vadapoo, Rajasekarakumar and Ahart, Muhtar and Somayazulu, Maddury and Holtgrewe, Nicholas and Meng, Yue and Konopkova, Zuzana and Hemley, Russell J. and Cohen, R. E.},
abstractNote = {},
doi = {10.1103/PhysRevB.95.214120},
journal = {Physical Review B},
number = 21,
volume = 95,
place = {United States},
year = {Fri Jun 30 00:00:00 EDT 2017},
month = {Fri Jun 30 00:00:00 EDT 2017}
}

Journal Article:
Free Publicly Available Full Text
This content will become publicly available on June 30, 2018
Publisher's Accepted Manuscript

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  • For decades, numerous attempts have been made to produce polar oxynitride perovskites, where some of the oxygen is replaced by nitrogen, but a polar ordered oxynitride has never been demonstrated. Caracas and Cohen [Appl. Phys. Lett. 91, 092902 (2007)] studied possible ordered polar oxynitrides within density-functional theory (DFT) and found a few candidates that were predicted to be insulating and at least metastable. YSi O 2 N stood out with huge predicted polarization and nonlinear optic coefficients. In this study, we demonstrate the synthesis of perovskite-structured YSi O 2 N by using a combination of a diamond-anvil cell and inmore » situ laser-heating techniques. Subsequent in situ x-ray diffraction, second-harmonic generation, and Raman-scattering measurements confirm that it is polar and a strong nonlinear optical material, with structure and properties similar to those predicted by DFT.« less
  • The synthesis, structural characterization, and magnetic property studies of SrLaMnSbO6 double perovskite oxide are reported. The crystal structure of SrLaMnSbO6 has been solved by powder X-ray (PXD) and neutron diffraction (NPD) data in the monoclinic space group P21/n (a = 5.6878(3) Angstroms, b = 5.6990(2) Angstroms, c = 8.0499(4) Angstroms and {beta} = 89.98(2); 295 K, NPD data). The Mn and Sb atoms are nearly completely ordered over the B-site of the perovskite structure. The octahedral framework displays significant tilting distortion according to the Glazer's tilt system a-a-c+. X-ray absorption near-edge spectroscopic (XAS) studies show the presence of Mn2+ andmore » Sb5+ formal oxidation states. The magnetic susceptibility data of SrLaMnSbO6 indicate the presence of ferromagnetic correlations; the calculated effective paramagnetic moment, {mu}calcd = 5.92 {mu}B (for HS Mn2+(3d5), S = 5/2; as evidenced by XAS data) is in good agreement with the value obtained experimentally ({mu}exp = 5.70 {mu}B). Variable temperature neutron diffraction data show no evidence of structural transition down to 3.7 K. A long-range antiferromagnetic ordering is established at TN = 8 K as evidenced by the magnetic susceptibility and specific heat measurements. The magnetic structure at 3.7 K is characterized by k = 0 propagation vector and m1x = -m2x, m1y = m2y = 0, m1z = -m2z (mx = 1.26(7) {mu}B, mz = 1.82(6) {mu}B) coupling of magnetic moments on the Mn1 (1/2,0,0) and Mn2 (0,1/2,1/2) atoms with the ordered magnetic moment of 2.21(4) {mu}B.« less
  • LaSrMnNbO{sub 6} has been synthesized by high temperature solid state reaction under 1% H{sub 2}/Ar dynamic flow. The structure is determined by Rietveld refinement of the powder X-ray diffraction data. It crystallizes in the monoclinic space group P2{sub 1}/n with the unit cell parameters: a = 5.69187(12), b = 5.74732(10), c = 8.07018(15) {angstrom} and {beta} = 90.0504(29){sup o}, which were also confirmed by electron diffraction. The Mn{sup 2+} and Nb{sup 5+} ions, whose valence states are confirmed by X-ray absorption near-edge spectroscopy, are almost completely ordered over the B-site (<1% inversion) of the perovskite structure due to the largemore » differences of both cationic size (0.19 {angstrom}) and charge. The octahedral framework displays significant tilting distortion according to Glazer's tilt system a{sup -}b{sup -}c{sup +}. Upon heating, LaSrMnNbO{sub 6} decomposes at 690 C under O{sup 2} flow or at 775 C in air. The magnetic susceptibility data indicate the presence of long-range antiferromagnetic ordering at T{sub N} = 8 K; the experimentally observed effective paramagnetic moment, {mu}{sub eff} = 5.76 {micro}{sub B} for high spin Mn{sup 2+} (3d{sup 5}, S = 5/2) is in good agreement with the calculated value ({mu}{sub calcd} = 5.92 {micro}B).« less
  • Polycrystalline Cd{sub 3-x-y}Cu {sub x} A {sub y}TeO{sub 6} (A = Li, Na) samples were prepared by solid-state reaction, and their crystal structure and electrical properties were investigated. In Cd{sub 3-x}Cu {sub x}TeO{sub 6} and Cd{sub 3-y} A {sub y}TeO{sub 6} (A = Li, Na), the maxim solubility of x and y was 0.15 and 0.15 for A = Li, 0.05 for A = Na, respectively. For co-substituted samples Cd{sub 2.9-y}Cu{sub 0.1}Li {sub y}TeO{sub 6} and Cd{sub 2.9-y}Cu{sub 0.1}Na {sub y}TeO{sub 6}, the maxim solubility of x was the same as single substitution above-mentioned. The alkali-metal substituted samples Cd{sub 3-y}more » A {sub y}TeO{sub 6} (A = Li, Na) showed a negative Seebeck coefficient, which indicates that the major conduction carriers are electron. On the other hand, the co-substituted samples Cd{sub 2.9-y}Cu{sub 0.1} A {sub y}TeO{sub 6} (A = Li, Na) represented a positive Seebeck coefficient, and major conduction carriers were hole through substitution by copper ions.« less
  • LaSrMnNbO{sub 6} has been synthesized by high temperature solid state reaction under 1% H{sub 2}/Ar dynamic flow. The structure is determined by Rietveld refinement of the powder X-ray diffraction data. It crystallizes in the monoclinic space group P2{sub 1}/n with the unit cell parameters: a=5.69187(12), b=5.74732(10), c=8.07018(15) A and {beta}=90.0504(29){sup o}, which were also confirmed by electron diffraction. The Mn{sup 2+} and Nb{sup 5+} ions, whose valence states are confirmed by X-ray absorption near-edge spectroscopy, are almost completely ordered over the B-site (<1% inversion) of the perovskite structure due to the large differences of both cationic size (0.19 A) andmore » charge. The octahedral framework displays significant tilting distortion according to Glazer's tilt system a{sup -}b{sup -}c{sup +}. Upon heating, LaSrMnNbO{sub 6} decomposes at 690 {sup o}C under O{sub 2} flow or at 775 {sup o}C in air. The magnetic susceptibility data indicate the presence of long-range antiferromagnetic ordering at T{sub N}=8 K; the experimentally observed effective paramagnetic moment, {mu}{sub eff}=5.76 {mu}{sub B} for high spin Mn{sup 2+} (3d{sup 5}, S=5/2) is in good agreement with the calculated value ({mu}{sub calcd}=5.92 {mu}{sub B}). -- Graphical abstract: An ordered double perovskite, LaSrMnNbO{sub 6} has been synthesized in the monoclinic space group P2{sub 1}/n. The Mn{sup 2+} and Nb{sup 5+} ions, whose valence states are confirmed by X-ray absorption near-edge spectroscopy, are ordered over the B-site. The magnetic susceptibility data indicate long-range antiferromagnetic ordering at T{sub N}=8 K. Display Omitted« less