skip to main content
DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information

This content will become publicly available on June 3, 2020

Title: Chemical disorder and spin-liquid-like magnetism in the van der Waals layered 5 d transition metal halide Os 0.55 Cl 2

Abstract

Here, single crystals of the van der Waals layered 5d transition-metal compound Os 0.55Cl 2 were grown and characterized by x-ray diffraction, magnetization and heat-capacity measurements, and atomic resolution electron microscopy. The crystals are stable in air and easily cleaved. The structure is derived from the CdCl 2 structure type, with triangular layers of transition metal sites coordinated by edge-sharing octahedra of Cl and separated by a van der Waals gap. On average, only 55% of the metal sites are occupied by Os, and evidence for short- and long-ranged vacancy orders is observed by diffraction and real-space imaging. Magnetization data indicate magnetocrystalline anisotropy due to spin-orbit coupling, antiferromagnetic correlations, and no sign of magnetic order or spin freezing down to 0.4 K. Heat-capacity measurements in applied magnetic fields show only a broad, field-dependent anomaly. The magnetic susceptibility and heat capacity obey power laws at low temperature and low field with exponents close to 0.5. The power law behaviors of the low-temperature heat capacity and magnetic susceptibility suggest gapless magnetic fluctuations prevent spin freezing or ordering in Os 0.55Cl 2. Divergence of the magnetic Gruneisen parameter indicates nearness to a magnetic quantum critical point. Similarities to behaviors of spin-liquid materials aremore » noted, and in total the findings suggest Os 0.55Cl 2 may be an example of a quantum spin liquid in the limit of strong chemical disorder.« less

Authors:
ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [1]
  1. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Materials Sciences & Engineering Division; USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1564209
Alternate Identifier(s):
OSTI ID: 1524115
Grant/Contract Number:  
AC05-00OR22725
Resource Type:
Accepted Manuscript
Journal Name:
Physical Review B
Additional Journal Information:
Journal Volume: 99; Journal Issue: 21; Journal ID: ISSN 2469-9950
Publisher:
American Physical Society (APS)
Country of Publication:
United States
Language:
English
Subject:
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY; 36 MATERIALS SCIENCE

Citation Formats

McGuire, Michael A., Zheng, Qiang, Yan, Jiaqiang, and Sales, Brian C. Chemical disorder and spin-liquid-like magnetism in the van der Waals layered 5d transition metal halide Os0.55Cl2. United States: N. p., 2019. Web. doi:10.1103/PhysRevB.99.214402.
McGuire, Michael A., Zheng, Qiang, Yan, Jiaqiang, & Sales, Brian C. Chemical disorder and spin-liquid-like magnetism in the van der Waals layered 5d transition metal halide Os0.55Cl2. United States. doi:10.1103/PhysRevB.99.214402.
McGuire, Michael A., Zheng, Qiang, Yan, Jiaqiang, and Sales, Brian C. Mon . "Chemical disorder and spin-liquid-like magnetism in the van der Waals layered 5d transition metal halide Os0.55Cl2". United States. doi:10.1103/PhysRevB.99.214402.
@article{osti_1564209,
title = {Chemical disorder and spin-liquid-like magnetism in the van der Waals layered 5d transition metal halide Os0.55Cl2},
author = {McGuire, Michael A. and Zheng, Qiang and Yan, Jiaqiang and Sales, Brian C.},
abstractNote = {Here, single crystals of the van der Waals layered 5d transition-metal compound Os0.55Cl2 were grown and characterized by x-ray diffraction, magnetization and heat-capacity measurements, and atomic resolution electron microscopy. The crystals are stable in air and easily cleaved. The structure is derived from the CdCl2 structure type, with triangular layers of transition metal sites coordinated by edge-sharing octahedra of Cl and separated by a van der Waals gap. On average, only 55% of the metal sites are occupied by Os, and evidence for short- and long-ranged vacancy orders is observed by diffraction and real-space imaging. Magnetization data indicate magnetocrystalline anisotropy due to spin-orbit coupling, antiferromagnetic correlations, and no sign of magnetic order or spin freezing down to 0.4 K. Heat-capacity measurements in applied magnetic fields show only a broad, field-dependent anomaly. The magnetic susceptibility and heat capacity obey power laws at low temperature and low field with exponents close to 0.5. The power law behaviors of the low-temperature heat capacity and magnetic susceptibility suggest gapless magnetic fluctuations prevent spin freezing or ordering in Os0.55Cl2. Divergence of the magnetic Gruneisen parameter indicates nearness to a magnetic quantum critical point. Similarities to behaviors of spin-liquid materials are noted, and in total the findings suggest Os0.55Cl2 may be an example of a quantum spin liquid in the limit of strong chemical disorder.},
doi = {10.1103/PhysRevB.99.214402},
journal = {Physical Review B},
number = 21,
volume = 99,
place = {United States},
year = {2019},
month = {6}
}

Journal Article:
Free Publicly Available Full Text
This content will become publicly available on June 3, 2020
Publisher's Version of Record

Citation Metrics:
Cited by: 2 works
Citation information provided by
Web of Science

Save / Share:

Works referenced in this record:

VI 3 —a New Layered Ferromagnetic Semiconductor
journal, March 2019

  • Kong, Tai; Stolze, Karoline; Timmons, Erik I.
  • Advanced Materials, Vol. 31, Issue 17
  • DOI: 10.1002/adma.201808074

Magnetic behavior and spin-lattice coupling in cleavable van der Waals layered CrCl 3 crystals
journal, June 2017


Proximate Kitaev quantum spin liquid behaviour in a honeycomb magnet
journal, April 2016

  • Banerjee, A.; Bridges, C. A.; Yan, J. -Q.
  • Nature Materials, Vol. 15, Issue 7
  • DOI: 10.1038/nmat4604

Oxide chlorides of osmium
journal, January 1968

  • Colton, R.; Farthing, Rh
  • Australian Journal of Chemistry, Vol. 21, Issue 3
  • DOI: 10.1071/CH9680589

High-temperature magnetostructural transition in van der Waals-layered α MoCl 3
journal, November 2017


Rearrangement of van der Waals stacking and formation of a singlet state at T = 90 K in a cluster magnet
journal, January 2017

  • Sheckelton, John P.; Plumb, Kemp W.; Trump, Benjamin A.
  • Inorganic Chemistry Frontiers, Vol. 4, Issue 3
  • DOI: 10.1039/C6QI00470A

Moessbauer spectroscopy and magnetization studies of .alpha.- and .beta.-ruthenium trichloride
journal, October 1992

  • Kobayashi, Y.; Okada, T.; Asai, K.
  • Inorganic Chemistry, Vol. 31, Issue 22
  • DOI: 10.1021/ic00048a025

Sc 2 Ga 2 CuO 7 : A possible quantum spin liquid near the percolation threshold
journal, November 2015


Novel J eff = 1 / 2 Mott State Induced by Relativistic Spin-Orbit Coupling in Sr 2 IrO 4
journal, August 2008


Diamagnetic Corrections and Pascal's Constants
journal, April 2008

  • Bain, Gordon A.; Berry, John F.
  • Journal of Chemical Education, Vol. 85, Issue 4
  • DOI: 10.1021/ed085p532

Universally Diverging Grüneisen Parameter and the Magnetocaloric Effect Close to Quantum Critical Points
journal, August 2003


EELS log-ratio technique for specimen-thickness measurement in the TEM
journal, February 1988

  • Malis, T.; Cheng, S. C.; Egerton, R. F.
  • Journal of Electron Microscopy Technique, Vol. 8, Issue 2
  • DOI: 10.1002/jemt.1060080206

Chloride und Oxidchloride des Osmiums
journal, April 1967


Hyperhoneycomb Iridate β Li 2 IrO 3 as a Platform for Kitaev Magnetism
journal, February 2015


Spin-glass behavior and vacancy order in van der Waals layered β MoCl 4
journal, July 2018


Gapless quantum spin liquid ground state in the two-dimensional spin-1/2 triangular antiferromagnet YbMgGaO4
journal, November 2015

  • Li, Yuesheng; Liao, Haijun; Zhang, Zhen
  • Scientific Reports, Vol. 5, Issue 1
  • DOI: 10.1038/srep16419

Novel magnetic state in d 4 Mott insulators
journal, February 2015


Investigation of the Polymorphism of Osmium Tetrachloride
journal, February 1969


Magnetism and electronic structure of La 2 ZnIrO 6 and La 2 MgIrO 6 : Candidate J eff = 1 2 Mott insulators
journal, April 2013


Resolution of a Racemic Pteridine during Paper Chromatography
journal, September 1963

  • Albert, Adrien; Serjeant, E. P.
  • Nature, Vol. 199, Issue 4898
  • DOI: 10.1038/1991098a0

Continuous excitations of the triangular-lattice quantum spin liquid YbMgGaO4
journal, December 2016

  • Paddison, Joseph A. M.; Daum, Marcus; Dun, Zhiling
  • Nature Physics, Vol. 13, Issue 2
  • DOI: 10.1038/nphys3971

Coupling of Crystal Structure and Magnetism in the Layered, Ferromagnetic Insulator CrI 3
journal, January 2015

  • McGuire, Michael A.; Dixit, Hemant; Cooper, Valentino R.
  • Chemistry of Materials, Vol. 27, Issue 2
  • DOI: 10.1021/cm504242t

Spin-Orbit-Coupling Effects in Transition-Metal Compounds
journal, July 1968


Bulk properties of the van der Waals hard ferromagnet VI 3
journal, January 2019


Ferromagnetic van der Waals Crystal VI 3
journal, March 2019

  • Tian, Shangjie; Zhang, Jian-Feng; Li, Chenghe
  • Journal of the American Chemical Society, Vol. 141, Issue 13
  • DOI: 10.1021/jacs.8b13584

Crystal and Magnetic Structures in Layered, Transition Metal Dihalides and Trihalides
journal, April 2017


Spin Liquid State in the S = 1 / 2 Triangular Lattice Ba 3 CuSb 2 O 9
journal, April 2011


Anisotropic Ru 3 +   4 d 5 magnetism in the α RuCl 3 honeycomb system: Susceptibility, specific heat, and zero-field NMR
journal, May 2015


Excitonic Magnetism in Van Vleck–type d 4 Mott Insulators
journal, November 2013


α RuCl 3 : A spin-orbit assisted Mott insulator on a honeycomb lattice
journal, July 2014


Layer-dependent ferromagnetism in a van der Waals crystal down to the monolayer limit
journal, June 2017

  • Huang, Bevin; Clark, Genevieve; Navarro-Moratalla, Efrén
  • Nature, Vol. 546, Issue 7657
  • DOI: 10.1038/nature22391

Detuning the Honeycomb of the α-RuCl 3 Kitaev Lattice: A Case of Cr 3+ Dopant
journal, May 2019


Antiferromagnetic Mott insulating state in single crystals of the honeycomb lattice material Na 2 IrO 3
journal, August 2010


Ba 2 YIrO 6 : A cubic double perovskite material with Ir 5 + ions
journal, January 2016


Destabilization of Magnetic Order in a Dilute Kitaev Spin Liquid Candidate
journal, December 2017


X-Ray, infrared, and magnetic studies of α- and β-ruthenium trichloride
journal, January 1967

  • Fletcher, J. M.; Gardner, W. E.; Fox, A. C.
  • J. Chem. Soc. A, Vol. 0, Issue 0
  • DOI: 10.1039/J19670001038

Li 2 RhO 3 : A spin-glassy relativistic Mott insulator
journal, April 2013


Spin Dynamics of the Spin- 1 / 2 Kagome Lattice Antiferromagnet ZnCu 3 ( OH ) 6 Cl 2
journal, March 2007


Structure of the high-temperature form of osmium(IV) chloride
journal, August 1977

  • Cotton, F. Albert.; Rice, Catherine E.
  • Inorganic Chemistry, Vol. 16, Issue 8
  • DOI: 10.1021/ic50174a008

Divergence of the Grüneisen Parameter and Magnetocaloric Effect at Heavy Fermion Quantum Critical Points
journal, July 2010

  • Gegenwart, P.; Tokiwa, Y.; Donath, J. G.
  • Journal of Low Temperature Physics, Vol. 161, Issue 1-2
  • DOI: 10.1007/s10909-010-0197-0

Effect of nonmagnetic dilution in the honeycomb-lattice iridates Na 2 IrO 3 and Li 2 IrO 3
journal, June 2014


Flux growth in a horizontal configuration: An analog to vapor transport growth
journal, July 2017