DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information

This content will become publicly available on Sat May 04 00:00:00 EDT 2024

Title: Evidence of Long-Range and Short-Range Magnetic Ordering in the Honeycomb Na3Mn2SbO6 Oxide

Abstract

We present a comprehensive study of the synthesis, structure, and magnetic properties of the honeycomb oxide Na3Mn2SbO6 supported by neutron diffraction, heat capacity, and magnetization measurements. The refinements of the neutron diffraction patterns (150, 50, and 45 K) using the Rietveld method confirm the monoclinic (S. G. C2/m) structure. Temperature-dependent magnetic susceptibilities measured at varying fields along with the heat capacity measurements demonstrate the coexistence of long-range ordering (∼42 K) and short-range ordering (∼65 K). The field-dependent isothermal magnetization measurements at 5 K indicate a spin-flop transition around 5 T. Rietveld refinements of the low-temperature (below 45 K) neutron diffraction data further confirm the long-range magnetic ordering. In addition, the temperature variation of the lattice parameters obtained from the neutron powder diffraction analysis exhibited a distinct anomaly near the antiferromagnetic transition temperature. The appearance of the concomitant broadened backgrounds in the neutron powder diffraction data collected at 80, 50, and 45 K supports the short-range ordering. The resultant magnetic structure consists of spins that are aligned antiparallel with the nearest neighbors and also with the spins of the adjacent honeycomb layers. The occurrence of a fully ordered magnetic ground state (Neel antiferromagnetic (AFM)) in Na3Mn2SbO6 consolidates the significance of fabricatingmore » new honeycomb oxides.« less

Authors:
 [1]; ORCiD logo [2]; ORCiD logo [3]; ORCiD logo [4]; ORCiD logo [1]
  1. Univ. of Delhi, New Delhi (India)
  2. Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
  3. Idaho National Laboratory (INL), Idaho Falls, ID (United States)
  4. Univ. of Texas at El Paso, TX (United States)
Publication Date:
Research Org.:
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES); SERB (Govt. of India); University of Delhi
OSTI Identifier:
2000319
Grant/Contract Number:  
AC05-00OR22725; CRG/2021/003714; IoE/2021/12/FRP
Resource Type:
Accepted Manuscript
Journal Name:
Inorganic Chemistry
Additional Journal Information:
Journal Volume: 62; Journal Issue: 19; Journal ID: ISSN 0020-1669
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Layers; Neutron diffraction; Oxides; Quantum mechanics; Transition metals

Citation Formats

Yadav, Dileep Kumar, Zhang, Qiang, Gofryk, Krzysztof, Nair, Harikrishnan S., and Uma, Sitharaman. Evidence of Long-Range and Short-Range Magnetic Ordering in the Honeycomb Na3Mn2SbO6 Oxide. United States: N. p., 2023. Web. doi:10.1021/acs.inorgchem.3c00666.
Yadav, Dileep Kumar, Zhang, Qiang, Gofryk, Krzysztof, Nair, Harikrishnan S., & Uma, Sitharaman. Evidence of Long-Range and Short-Range Magnetic Ordering in the Honeycomb Na3Mn2SbO6 Oxide. United States. https://doi.org/10.1021/acs.inorgchem.3c00666
Yadav, Dileep Kumar, Zhang, Qiang, Gofryk, Krzysztof, Nair, Harikrishnan S., and Uma, Sitharaman. Thu . "Evidence of Long-Range and Short-Range Magnetic Ordering in the Honeycomb Na3Mn2SbO6 Oxide". United States. https://doi.org/10.1021/acs.inorgchem.3c00666.
@article{osti_2000319,
title = {Evidence of Long-Range and Short-Range Magnetic Ordering in the Honeycomb Na3Mn2SbO6 Oxide},
author = {Yadav, Dileep Kumar and Zhang, Qiang and Gofryk, Krzysztof and Nair, Harikrishnan S. and Uma, Sitharaman},
abstractNote = {We present a comprehensive study of the synthesis, structure, and magnetic properties of the honeycomb oxide Na3Mn2SbO6 supported by neutron diffraction, heat capacity, and magnetization measurements. The refinements of the neutron diffraction patterns (150, 50, and 45 K) using the Rietveld method confirm the monoclinic (S. G. C2/m) structure. Temperature-dependent magnetic susceptibilities measured at varying fields along with the heat capacity measurements demonstrate the coexistence of long-range ordering (∼42 K) and short-range ordering (∼65 K). The field-dependent isothermal magnetization measurements at 5 K indicate a spin-flop transition around 5 T. Rietveld refinements of the low-temperature (below 45 K) neutron diffraction data further confirm the long-range magnetic ordering. In addition, the temperature variation of the lattice parameters obtained from the neutron powder diffraction analysis exhibited a distinct anomaly near the antiferromagnetic transition temperature. The appearance of the concomitant broadened backgrounds in the neutron powder diffraction data collected at 80, 50, and 45 K supports the short-range ordering. The resultant magnetic structure consists of spins that are aligned antiparallel with the nearest neighbors and also with the spins of the adjacent honeycomb layers. The occurrence of a fully ordered magnetic ground state (Neel antiferromagnetic (AFM)) in Na3Mn2SbO6 consolidates the significance of fabricating new honeycomb oxides.},
doi = {10.1021/acs.inorgchem.3c00666},
journal = {Inorganic Chemistry},
number = 19,
volume = 62,
place = {United States},
year = {Thu May 04 00:00:00 EDT 2023},
month = {Thu May 04 00:00:00 EDT 2023}
}

Journal Article:
Free Publicly Available Full Text
This content will become publicly available on May 4, 2024
Publisher's Version of Record

Save / Share:

Works referenced in this record:

Crystal structure of Li4ZnTeO6 and revision of Li3Cu2SbO6
journal, March 2013


Li4NiTeO6 as a positive electrode for Li-ion batteries
journal, January 2013

  • Sathiya, M.; Ramesha, K.; Rousse, G.
  • Chemical Communications, Vol. 49, Issue 97
  • DOI: 10.1039/c3cc46842a

Static and Dynamic Magnetic Response of Fragmented Haldane-like Spin Chains in Layered Li 3 Cu 2 SbO 6
journal, August 2016

  • Koo, Changhyun; Zvereva, Elena A.; Shukaev, Igor L.
  • Journal of the Physical Society of Japan, Vol. 85, Issue 8
  • DOI: 10.7566/JPSJ.85.084702

Structure and Magnetic Properties of Cu 3 Ni 2 SbO 6 and Cu 3 Co 2 SbO 6 Delafossites with Honeycomb Lattices
journal, April 2013

  • Roudebush, J. H.; Andersen, N. H.; Ramlau, R.
  • Inorganic Chemistry, Vol. 52, Issue 10
  • DOI: 10.1021/ic400415h

Anomalous Ferromagnetic Behavior in Orthorhombic Li3Co2SbO6
journal, July 2022


Structure and basic magnetic properties of the honeycomb lattice compounds Na2Co2TeO6 and Na3Co2SbO6
journal, March 2007


Zigzag antiferromagnetic quantum ground state in monoclinic honeycomb lattice antimonates A 3 N i 2 Sb O 6 ( A = Li , Na )
journal, October 2015


A review of cation-ordered rock salt superstructure oxides
journal, January 2000

  • Mather, Glenn C.; Dussarrat, Christian; Etourneau, Jean
  • Journal of Materials Chemistry, Vol. 10, Issue 10
  • DOI: 10.1039/b000817f

Honeycomb Compound Na3Ni2BiO6as Positive Electrode Material in Na Cells
journal, January 2016

  • Zheng, Lituo; Obrovac, M. N.
  • Journal of The Electrochemical Society, Vol. 163, Issue 10
  • DOI: 10.1149/2.0991610jes

Spin-Gap Behavior of Na 3 Cu 2 SbO 6 with Distorted Honeycomb Structure
journal, August 2006

  • Miura, Yoko; Hirai, Riu; Kobayashi, Yoshiaki
  • Journal of the Physical Society of Japan, Vol. 75, Issue 8
  • DOI: 10.1143/JPSJ.75.084707

Na 2 Ni 2 TeO 6 : Evaluation as a cathode for sodium battery
journal, December 2013


Nuclear and incommensurate magnetic structure of NaFeGe2O6 between 5 K and 298 K and new data on multiferroic NaFeSi2O6
journal, August 2010

  • Redhammer, Günther J.; Senyshyn, Anatoliy; Meven, Martin
  • Physics and Chemistry of Minerals, Vol. 38, Issue 2
  • DOI: 10.1007/s00269-010-0390-3

New P2-Type Honeycomb-Layered Sodium-Ion Conductor: Na2Mg2TeO6
journal, April 2018

  • Li, Yuyu; Deng, Zhi; Peng, Jian
  • ACS Applied Materials & Interfaces, Vol. 10, Issue 18
  • DOI: 10.1021/acsami.8b03938

GSAS-II : the genesis of a modern open-source all purpose crystallography software package
journal, March 2013


VESTA 3 for three-dimensional visualization of crystal, volumetric and morphology data
journal, October 2011


Synthesis and characterization of O3-Na3LiFeSbO6: A new honeycomb ordered layered oxide
journal, February 2014


Phase diagram of the J 1 J 2 J 3 Heisenberg model on the honeycomb lattice: A series expansion study
journal, September 2011


Neutron scattering lengths and cross sections
journal, January 1992


Long-range and short-range ordering in 2D honeycomb-lattice magnet Na2Ni2TeO6
journal, April 2020

  • Kurbakov, Alexander I.; Korshunov, Artem N.; Podchezertsev, Stanislav Yu
  • Journal of Alloys and Compounds, Vol. 820
  • DOI: 10.1016/j.jallcom.2019.153354

High-resolution X-ray diffraction, DIFFaX, NMR and first principles study of disorder in the Li2MnO3–Li[Ni1/2Mn1/2]O2 solid solution
journal, September 2005

  • Bréger, Julien; Jiang, Meng; Dupré, Nicolas
  • Journal of Solid State Chemistry, Vol. 178, Issue 9, p. 2575-2585
  • DOI: 10.1016/j.jssc.2005.05.027

Mixed oxides of sodium, antimony (5+) and divalent metals (Ni, Co, Zn or Mg)
journal, March 2010

  • Politaev, V. V.; Nalbandyan, V. B.; Petrenko, A. A.
  • Journal of Solid State Chemistry, Vol. 183, Issue 3
  • DOI: 10.1016/j.jssc.2009.12.002

On AgRhO2, and the new quaternary delafossites AgLi1/3M2/3O2, syntheses and analyses of real structures
journal, May 2011


Magnetic and electrode properties, structure and phase relations of the layered triangular-lattice tellurate Li4NiTeO6
journal, May 2015

  • Zvereva, Elena A.; Nalbandyan, Vladimir B.; Evstigneeva, Maria A.
  • Journal of Solid State Chemistry, Vol. 225
  • DOI: 10.1016/j.jssc.2014.12.003

A new layered triangular antiferromagnet Li 4 FeSbO 6 : spin order, field-induced transitions and anomalous critical behavior
journal, January 2013

  • Zvereva, E. A.; Savelieva, O. A.; Titov, Ya. D.
  • Dalton Trans., Vol. 42, Issue 5
  • DOI: 10.1039/C2DT31938A

New series of honeycomb ordered oxides, Na3M2SbO6 (M(ii) = Mn, Fe, (Mn, Fe), (Mn, Co)): synthesis, structure and magnetic properties
journal, January 2019

  • Yadav, Dileep Kumar; Sethi, Aanchal; Shalu, Shalu
  • Dalton Transactions, Vol. 48, Issue 24
  • DOI: 10.1039/C9DT01194C

Honeycomb layered oxides: structure, energy storage, transport, topology and relevant insights
journal, January 2021

  • Kanyolo, Godwill Mbiti; Masese, Titus; Matsubara, Nami
  • Chemical Society Reviews, Vol. 50, Issue 6
  • DOI: 10.1039/D0CS00320D

Phase diagram of a frustrated Heisenberg antiferromagnet on the honeycomb lattice: The J 1 - J 2 - J 3 model
journal, October 2012


Synthesis, Crystal Structure, and Magnetic Properties of Bi 3 Mn 4 O 12 (NO 3 ) Oxynitrate Comprising S = 3/2 Honeycomb Lattice
journal, June 2009

  • Smirnova, Olga; Azuma, Masaki; Kumada, Nobuhiro
  • Journal of the American Chemical Society, Vol. 131, Issue 23
  • DOI: 10.1021/ja901922p

Influence of oxidation state and ionic size in the formation of honeycomb ordered structures, Li3Mn2SbO6 and Li4CoSbO6
journal, April 2022

  • Yadav, Dileep Kumar; Pal, Sachin; Uma, Sitharaman
  • Journal of Physics and Chemistry of Solids, Vol. 163
  • DOI: 10.1016/j.jpcs.2021.110559

Temperature-Dependent Na-Ion Conduction and Its Pathways in the Crystal Structure of the Layered Battery Material Na 2 Ni 2 TeO 6
journal, January 2020

  • Bera, Anup Kumar; Yusuf, Seikh M.
  • The Journal of Physical Chemistry C, Vol. 124, Issue 8
  • DOI: 10.1021/acs.jpcc.9b11191

Absence of long-range magnetic order in lithium-containing honeycombs in the Li–Cr–Sb(Te)–O phases
journal, June 2021

  • Mandujano, H. Cein; Gonzalez, Sandra L.; Episcopo, Nathan
  • Journal of Physics: Condensed Matter, Vol. 33, Issue 29
  • DOI: 10.1088/1361-648X/abff90

Electrochemical Properties of Three Li 2 Ni 2 TeO 6 Structural Polymorphs
journal, October 2019


Monoclinic honeycomb-layered compound Li3Ni2SbO6: preparation, crystal structure and magnetic properties
journal, January 2012

  • Zvereva, Elena A.; Evstigneeva, Maria A.; Nalbandyan, Vladimir B.
  • Dalton Trans., Vol. 41, Issue 2
  • DOI: 10.1039/C1DT11322D

Spin 1 / 2 Delafossite Honeycomb Compound Cu 5 SbO 6
journal, December 2011

  • Climent-Pascual, E.; Norby, P.; Andersen, N. H.
  • Inorganic Chemistry, Vol. 51, Issue 1
  • DOI: 10.1021/ic202066n

Ordering, metastability and phase transitions in two-dimensional systems
journal, April 1973

  • Kosterlitz, J M; Thouless, D J
  • Journal of Physics C: Solid State Physics, Vol. 6, Issue 7, p. 1181-1203
  • DOI: 10.1088/0022-3719/6/7/010

New Layered Compounds with Honeycomb Ordering: Li 3 Ni 2 BiO 6 , Li 3 NiM′BiO 6 (M′ = Mg, Cu, Zn), and the Delafossite Ag 3 Ni 2 BiO 6
journal, April 2012

  • Berthelot, Romain; Schmidt, Whitney; Muir, Sean
  • Inorganic Chemistry, Vol. 51, Issue 9
  • DOI: 10.1021/ic300351t

Crucial Role of Site Disorder and Frustration in Unusual Magnetic Properties of Quasi-2D Triangular Lattice Antimonate Na4FeSbO6
journal, June 2015

  • Zvereva, Elena A.; Presniakov, Igor A.; Whangbo, Myung-Hwan
  • Applied Magnetic Resonance, Vol. 46, Issue 10
  • DOI: 10.1007/s00723-015-0700-5

Structure and Magnetic Properties of the α-NaFeO 2 -Type Honeycomb Compound Na 3 Ni 2 BiO 6
journal, November 2013

  • Seibel, Elizabeth M.; Roudebush, J. H.; Wu, Hui
  • Inorganic Chemistry, Vol. 52, Issue 23
  • DOI: 10.1021/ic402131e

Zig-zag magnetic ordering in honeycomb-layered Na3Co2SbO6
journal, November 2016


Rechargeable potassium-ion batteries with honeycomb-layered tellurates as high voltage cathodes and fast potassium-ion conductors
journal, September 2018


Evidence of cationic mixing and ordering in the honeycomb layer of Li 4 MSbO 6 (M( iii ) = Cr, Mn, Al, Ga) (S.G. C2/c) oxides
journal, January 2014

  • Bhardwaj, Neha; Gupta, Akanksha; Uma, S.
  • Dalton Trans., Vol. 43, Issue 31
  • DOI: 10.1039/C4DT00887A

A New Family of Fast Sodium Ion Conductors: Na 2 M 2 TeO 6 (M = Ni, Co, Zn, Mg)
journal, March 2011

  • Evstigneeva, Maria A.; Nalbandyan, Vladimir B.; Petrenko, Aleksandr A.
  • Chemistry of Materials, Vol. 23, Issue 5
  • DOI: 10.1021/cm102629g

Synthesis-Controlled Polymorphism and Magnetic and Electrochemical Properties of Li 3 Co 2 SbO 6
journal, October 2019


Magnetic structure, excitations and short-range order in honeycomb Na2Ni2TeO6
journal, July 2021

  • Episcopo, Nathan; Chang, Po-Hao; Heitmann, Thomas W.
  • Journal of Physics: Condensed Matter, Vol. 33, Issue 37
  • DOI: 10.1088/1361-648X/ac0ea6

Novel Lithium-Containing Honeycomb Structures
journal, October 2012

  • Kumar, Vinod; Bhardwaj, Neha; Tomar, Nobel
  • Inorganic Chemistry, Vol. 51, Issue 20
  • DOI: 10.1021/ic301125n

Antiferromagnetic Order and Spin-Canting Transition in the Corrugated Square Net Compound Cu3(TeO4)(SO4)·H2O
journal, June 2021


A Honeycomb-Layered Na 3 Ni 2 SbO 6 : A High-Rate and Cycle-Stable Cathode for Sodium-Ion Batteries
journal, July 2014


Microscopic magnetic modeling for the S = 1 2 alternating-chain compounds Na 3 Cu 2 SbO 6 and Na 2 Cu 2 TeO 6
journal, May 2014


Synthesis, Structure, and Magnetic Properties of the Layered Copper(II) Oxide Na 2 Cu 2 TeO 6
journal, July 2005

  • Xu, Jianxiao; Assoud, Abdeljalil; Soheilnia, Navid
  • Inorganic Chemistry, Vol. 44, Issue 14
  • DOI: 10.1021/ic0502832

Formation of honeycomb ordered monoclinic Li2M2TeO6 (M = Cu, Ni) and disordered orthorhombic Li2Ni2TeO6 oxides
journal, January 2013

  • Kumar, Vinod; Gupta, Akanksha; Uma, S.
  • Dalton Transactions, Vol. 42, Issue 42
  • DOI: 10.1039/c3dt51604k

X-Ray Diffraction in Random Layer Lattices
journal, May 1941


Solid solution studies of layered honeycomb-ordered phases O3–Na3M2SbO6 (M=Cu, Mg, Ni, Zn)
journal, May 2013


Magnetism of two-dimensional honeycomb layered Na2Ni2TeO6 driven by intermediate Na-layer crystal structure
journal, January 2022