Skip to main content
OSTI.GOVU.S. Department of Energy Office of Scientific and Technical Information
U.S. Department of Energy
Office of Scientific and Technical Information
 

Phonon dynamics in quantum spin liquid and valence bond crystal states in the barlowite family of kagome magnets

Journal Article · · Physical Review. B
 [1];  [2];  [3];  [1];  [4];  [2];  [1]
  1. SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States); Stanford Univ., CA (United States)
  2. SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)
  3. Brookhaven National Laboratory (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)
  4. SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States); Stanford Univ., CA (United States); National Renewable Energy Laboratory (NREL), Golden, CO (United States)
+ Show Author Affiliations
The barlowite [Cu4⁢(OD)6⁢FBr] family of materials is characterized by antiferromagnetic spin-1/2 kagome layers and are believed to host interesting ground states of quantum magnetism. Substituting the interlayer sites with zinc ions yields Zn-barlowite (Zn𝑥⁢Cu4−𝑥⁢(OD)6⁢FBr, 𝑥 ≈ 0.80) which is a strong candidate to have a quantum spin liquid (QSL) state. Experimentally distinguishing between valence bond crystal (VBC) and QSL states in the absence of magnetic ordering can prove challenging as both states exhibit similar average spin-spin correlations. Using high-resolution inelastic x-ray scattering with 1.4 meV energy resolution, we probe acoustic phonons in these structurally similar materials at various temperatures. Our measurements uncover robust differences possibly driven by different spin-phonon physics in VBC and QSL states, particularly at the 𝑀-point Brillouin zone boundary. Over a large 𝑇=[15,200]⁢ K temperature range, where neither material undergoes magnetic ordering nor a structural transition, we observe phonon softening in Zn-barlowite in contrast to a hardening of the same phonon in barlowite. Further, these results indicate that acoustic phonons in the barlowite system can be used to study and possibly distinguish between QSL and disordered VBC states in quantum magnets.
Research Organization:
Brookhaven National Laboratory (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)
Sponsoring Organization:
National Science Foundation (NSF); Swiss National Science Foundation (SNSF); USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division (MSE); USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF)
Grant/Contract Number:
AC02-76SF00515; SC0012704
OSTI ID:
2569439
Report Number(s):
BNL--228236-2025-JAAM
Journal Information:
Physical Review. B, Journal Name: Physical Review. B Journal Issue: 9 Vol. 111; ISSN 2469-9969; ISSN 2469-9950
Publisher:
American Physical Society (APS)Copyright Statement
Country of Publication:
United States
Language:
English

References (46)

RVB description of the low-energy singlets of the spin 1/2 kagomé antiferromagnet journal October 2000
Resonating valence bonds: A new kind of insulator? journal February 1973
Fault-tolerant quantum computation by anyons journal January 2003
Quantum kagome frustrated antiferromagnets: One route to quantum spin liquids journal March 2016
Site Specific X-ray Anomalous Dispersion of the Geometrically Frustrated Kagomé Magnet, Herbertsmithite, ZnCu 3 (OH) 6 Cl 2 journal November 2010
Fractionalized excitations in the spin-liquid state of a kagome-lattice antiferromagnet journal December 2012
Identifying topological order by entanglement entropy journal November 2012
Giant phonon anomalies in the proximate Kitaev quantum spin liquid α-RuCl3 journal June 2021
From magnetic order to quantum disorder in the Zn-barlowite series of S = 1/2 kagomé antiferromagnets journal October 2020
Materializing rival ground states in the barlowite family of kagome magnets: quantum spin liquid, spin ordered, and valence bond crystal states journal April 2020
Emergence of the spin polarized domains in the kagome lattice Heisenberg antiferromagnet Zn-barlowite (Zn0.95Cu0.05)Cu3(OD)6FBr journal December 2022
Emergence of spin singlets with inhomogeneous gaps in the kagome lattice Heisenberg antiferromagnets Zn-barlowite and herbertsmithite journal August 2021
The observation of quantum fluctuations in a kagome Heisenberg antiferromagnet journal November 2022
Quantum spin liquids: a review journal November 2016
Gapped Spin-1/2 Spinon Excitations in a New Kagome Quantum Spin Liquid Compound Cu 3 Zn(OH) 6 FBr journal June 2017
From Claringbullite to a New Spin Liquid Candidate Cu 3 Zn(OH) 6 FCl journal December 2018
Infrared phonons as a probe of spin-liquid states in herbertsmithite ZnCu 3 (OH) 6 Cl 2 journal January 2017
The Ultrahigh Resolution IXS Beamline of NSLS-II: Recent Advances and Scientific Opportunities journal March 2013
Heat transport of the kagome Heisenberg quantum spin liquid candidate YCu3(OH)6.5Br2.5 : Localized magnetic excitations and a putative spin gap journal December 2022
High-energy spin excitations in the quantum spin liquid candidate Zn-substituted barlowite probed by resonant inelastic x-ray scattering journal February 2023
Spin-phonon interactions on the kagome lattice: Dirac spin liquid versus valence-bond solids journal April 2024
A new theory of the spin-Peierls transition with special relevance to the experiments on TTFCuBDT journal January 1979
Topology of the resonating valence-bond state: Solitons and high- T c superconductivity journal June 1987
X-ray scattering study of the spin-Peierls transition and soft phonon behavior in TiOCl journal December 2007
Barlowite as a canted antiferromagnet: Theory and experiment journal September 2015
Correlated impurities and intrinsic spin-liquid physics in the kagome material herbertsmithite journal August 2016
O 17 NMR Study of the Intrinsic Magnetic Susceptibility and Spin Dynamics of the Quantum Kagome Antiferromagnet ZnCu 3 ( OH ) 6 Cl 2 journal February 2008
Density Matrix Renormalization Group Numerical Study of the Kagome Antiferromagnet journal September 2008
Scale-Free Antiferromagnetic Fluctuations in the s = 1 / 2 Kagome Antiferromagnet Herbertsmithite journal December 2009
Barlowite: A Spin- 1 / 2 Antiferromagnet with a Geometrically Perfect Kagome Motif journal November 2014
Freezing of the Lattice in the Kagome Lattice Heisenberg Antiferromagnet Zn-Barlowite ZnCu3(OD)6FBr journal April 2022
Solitons in Polyacetylene journal June 1979
Density matrix formulation for quantum renormalization groups journal November 1992
Probing Spin Correlations with Phonons in the Strongly Frustrated Magnet ZnCr 2 O 4 journal April 2005
Magnetically Induced Phonon Anisotropy in ZnCr 2 O 4 from First Principles journal May 2006
Spin Dynamics of the Spin- 1 / 2 Kagome Lattice Antiferromagnet ZnCu 3 ( OH ) 6 Cl 2 journal March 2007
Single-crystal growth of C u 4 ( OH ) 6 BrF and universal behavior in quantum spin liquid candidates synthetic barlowite and herbertsmithite journal April 2018
Site-specific structure at multiple length scales in kagome quantum spin liquid candidates journal December 2020
Combinatorial exploration of quantum spin liquid candidates in the herbertsmithite material family journal June 2023
Extraordinary π -electron superconductivity emerging from a quantum spin liquid journal July 2021
Toward exact predictions of spin-phonon relaxation times: An ab initio implementation of open quantum systems theory journal August 2022
Spin-Liquid Ground State of the S = 1/2 Kagome Heisenberg Antiferromagnet journal April 2011
The Resonating Valence Bond State in La2CuO4 and Superconductivity journal March 1987
The Relationship Between High-Temperature Superconductivity and the Fractional Quantum Hall Effect journal October 1988
Evidence for a gapped spin-liquid ground state in a kagome Heisenberg antiferromagnet journal November 2015
Quantum spin liquids journal January 2020

Similar Records

Related Subjects

75 CONDENSED MATTER PHYSICS
SUPERCONDUCTIVITY AND SUPERFLUIDITY
Frustrated magnetism
Kagome lattice
Quantum spin liquid
Valence bond solid