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Title: Pb2MnTeO6 Double Perovskite: An Antipolar Anti-ferromagnet

Abstract

Pb2MnTeO6, a new double perovskite, has been synthesized. Its crystal structure was determined by synchrotron X-ray and powder neutron diffraction.Pb2MnTeO6 is monoclinic (I2/m) at room temperature with a regular arrangement of all the cations in their polyhedra. However, when the temperature is lowered to ~120 K it undergoes a phase transition from I2/m to C2/c structure. This transition is accompanied by a displacement of the Pb atoms from the center of their polyhedra due to the 6s2 lone-pair electrons, together with a surprising off-centering of Mn2+ (d5) magnetic cations. This strong first-order phase transition is also evidenced by specific heat, dielectric, Raman, and infrared spectroscopy measurements. The magnetic characterizations indicate an anti-ferromagnetic (AFM) order below TN ≈ 20 K; analysis of powder neutron diffraction data confirms the magnetic structure with propagation vector k = (0 1 0) and collinear AFM spins. The observed jump in dielectric permittivity near ~150 K implies possible anti-ferroelectric behavior; however, the absence of switching suggests that Pb2MnTeO6 can only be antipolar. First-principle calculations confirmed that the crystal and magnetic structures determined are locally stable and that anti-ferroelectric switching is unlikely to be observed in Pb2MnTeO6.

Authors:
 [1];  [2];  [1];  [3];  [4];  [4];  [1];  [5];  [2];  [2];  [2];  [6];  [7];  [8];  [9];  [2];  [5];  [4];  [2];  [1]
  1. Rutgers Univ., Piscataway, NJ (United States). Dept. of Chemistry and Chemical Biology
  2. Czech Academy of Sciences, Prague (Czech Republic). Inst. of Physics
  3. Univ. of Antwerp, Antwerp (Belgium); Moscow State Univ., Moscow (Russian Federation). Chemistry Dept.
  4. Rutgers Univ., Piscataway, NJ (United States). Dept. of Physics and Astronomy
  5. Cornell Univ., Ithaca, NY (United States). Dept. of Applied and Engineering Physics
  6. Charles Univ., Prague (Czech Republic). Dept. of Condensed Matter Physics
  7. Brookhaven National Lab. (BNL), Upton, NY (United States). Photon Sciences Directorate
  8. State Univ. of New York (SUNY), Plattsburgh, NY (United States). Dept. of Physics and Astronomy
  9. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Spallation Neutron Source (SNS)
Publication Date:
Research Org.:
Brookhaven National Lab. (BNL), Upton, NY (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF); Russian Science Foundation; US Army Research Office (ARO); US Department of the Navy, Office of Naval Research (ONR)
OSTI Identifier:
1340407
Report Number(s):
BNL-113214-2016-JA
Journal ID: ISSN 0020-1669
Grant/Contract Number:  
SC00112704; DMR-0966829; ARO-DOD-VV911NF-12-1-0172; N00014-12-1-1040; AC05-00OR22725; AC02-98CH10886; W911NF-10-1-0345
Resource Type:
Accepted Manuscript
Journal Name:
Inorganic Chemistry
Additional Journal Information:
Journal Volume: 55; Journal Issue: 9; Journal ID: ISSN 0020-1669
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY

Citation Formats

Retuerto, Maria, Skiadopoulou, Stella, Li, Man-Rong, Abakumov, Artem M., Croft, Mark., Ignatov, Alexander, Sarkar, Tapati, Abbett, Brian M., Pokorný, Jan, Savinov, Maxim, Nuzhnyy, Dmitry, Prokleška, Jan, Abeykoon, Milinda, Stephens, Peter W., Hodges, Jason P., Vaněk, Přemysl, Fennie, Craig J., Rabe, Karin M., Kamba, Stanislav, and Greenblatt, Martha. Pb2MnTeO6 Double Perovskite: An Antipolar Anti-ferromagnet. United States: N. p., 2016. Web. https://doi.org/10.1021/acs.inorgchem.6b00054.
Retuerto, Maria, Skiadopoulou, Stella, Li, Man-Rong, Abakumov, Artem M., Croft, Mark., Ignatov, Alexander, Sarkar, Tapati, Abbett, Brian M., Pokorný, Jan, Savinov, Maxim, Nuzhnyy, Dmitry, Prokleška, Jan, Abeykoon, Milinda, Stephens, Peter W., Hodges, Jason P., Vaněk, Přemysl, Fennie, Craig J., Rabe, Karin M., Kamba, Stanislav, & Greenblatt, Martha. Pb2MnTeO6 Double Perovskite: An Antipolar Anti-ferromagnet. United States. https://doi.org/10.1021/acs.inorgchem.6b00054
Retuerto, Maria, Skiadopoulou, Stella, Li, Man-Rong, Abakumov, Artem M., Croft, Mark., Ignatov, Alexander, Sarkar, Tapati, Abbett, Brian M., Pokorný, Jan, Savinov, Maxim, Nuzhnyy, Dmitry, Prokleška, Jan, Abeykoon, Milinda, Stephens, Peter W., Hodges, Jason P., Vaněk, Přemysl, Fennie, Craig J., Rabe, Karin M., Kamba, Stanislav, and Greenblatt, Martha. Fri . "Pb2MnTeO6 Double Perovskite: An Antipolar Anti-ferromagnet". United States. https://doi.org/10.1021/acs.inorgchem.6b00054. https://www.osti.gov/servlets/purl/1340407.
@article{osti_1340407,
title = {Pb2MnTeO6 Double Perovskite: An Antipolar Anti-ferromagnet},
author = {Retuerto, Maria and Skiadopoulou, Stella and Li, Man-Rong and Abakumov, Artem M. and Croft, Mark. and Ignatov, Alexander and Sarkar, Tapati and Abbett, Brian M. and Pokorný, Jan and Savinov, Maxim and Nuzhnyy, Dmitry and Prokleška, Jan and Abeykoon, Milinda and Stephens, Peter W. and Hodges, Jason P. and Vaněk, Přemysl and Fennie, Craig J. and Rabe, Karin M. and Kamba, Stanislav and Greenblatt, Martha},
abstractNote = {Pb2MnTeO6, a new double perovskite, has been synthesized. Its crystal structure was determined by synchrotron X-ray and powder neutron diffraction.Pb2MnTeO6 is monoclinic (I2/m) at room temperature with a regular arrangement of all the cations in their polyhedra. However, when the temperature is lowered to ~120 K it undergoes a phase transition from I2/m to C2/c structure. This transition is accompanied by a displacement of the Pb atoms from the center of their polyhedra due to the 6s2 lone-pair electrons, together with a surprising off-centering of Mn2+ (d5) magnetic cations. This strong first-order phase transition is also evidenced by specific heat, dielectric, Raman, and infrared spectroscopy measurements. The magnetic characterizations indicate an anti-ferromagnetic (AFM) order below TN ≈ 20 K; analysis of powder neutron diffraction data confirms the magnetic structure with propagation vector k = (0 1 0) and collinear AFM spins. The observed jump in dielectric permittivity near ~150 K implies possible anti-ferroelectric behavior; however, the absence of switching suggests that Pb2MnTeO6 can only be antipolar. First-principle calculations confirmed that the crystal and magnetic structures determined are locally stable and that anti-ferroelectric switching is unlikely to be observed in Pb2MnTeO6.},
doi = {10.1021/acs.inorgchem.6b00054},
journal = {Inorganic Chemistry},
number = 9,
volume = 55,
place = {United States},
year = {2016},
month = {4}
}

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