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

Title: Electron doping a kagome spin liquid

Abstract

Herbertsmithite, ZnCu3(OH)6Cl2, is a two-dimensional kagome lattice realization of a spin liquid, with evidence for fractionalized excitations and a gapped ground state. Such a quantum spin liquid has been proposed to underlie high-temperature superconductivity and is predicted to produce a wealth of new states, including a Dirac metal at 1/3 electron doping. Here, we report the topochemical synthesis of electron-doped ZnLixCu3(OH)6Cl2 from x=0 to x=1.8 (3/5 per Cu2+). Contrary to expectations, no metallicity or superconductivity is induced. Instead, we find a systematic suppression of magnetic behavior across the phase diagram. Lastly, our results demonstrate that significant theoretical work is needed to understand and predict the role of doping in magnetically frustrated narrow band insulators, particularly the interplay between local structural disorder and tendency toward electron localization, and pave the way for future studies of doped spin liquids.

Authors:
 [1];  [1];  [1]
  1. The Johns Hopkins Univ., Baltimore, MD (United States)
Publication Date:
Research Org.:
Johns Hopkins Univ., Baltimore, MD (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1361679
Grant/Contract Number:  
FG02-08ER46544
Resource Type:
Accepted Manuscript
Journal Name:
Physical Review. X
Additional Journal Information:
Journal Volume: 6; Journal Issue: 4; Journal ID: ISSN 2160-3308
Publisher:
American Physical Society
Country of Publication:
United States
Language:
English
Subject:
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY

Citation Formats

Kelly, Z. A., Gallagher, M. J., and McQueen, T. M. Electron doping a kagome spin liquid. United States: N. p., 2016. Web. doi:10.1103/PhysRevX.6.041007.
Kelly, Z. A., Gallagher, M. J., & McQueen, T. M. Electron doping a kagome spin liquid. United States. https://doi.org/10.1103/PhysRevX.6.041007
Kelly, Z. A., Gallagher, M. J., and McQueen, T. M. Thu . "Electron doping a kagome spin liquid". United States. https://doi.org/10.1103/PhysRevX.6.041007. https://www.osti.gov/servlets/purl/1361679.
@article{osti_1361679,
title = {Electron doping a kagome spin liquid},
author = {Kelly, Z. A. and Gallagher, M. J. and McQueen, T. M.},
abstractNote = {Herbertsmithite, ZnCu3(OH)6Cl2, is a two-dimensional kagome lattice realization of a spin liquid, with evidence for fractionalized excitations and a gapped ground state. Such a quantum spin liquid has been proposed to underlie high-temperature superconductivity and is predicted to produce a wealth of new states, including a Dirac metal at 1/3 electron doping. Here, we report the topochemical synthesis of electron-doped ZnLixCu3(OH)6Cl2 from x=0 to x=1.8 (3/5 per Cu2+). Contrary to expectations, no metallicity or superconductivity is induced. Instead, we find a systematic suppression of magnetic behavior across the phase diagram. Lastly, our results demonstrate that significant theoretical work is needed to understand and predict the role of doping in magnetically frustrated narrow band insulators, particularly the interplay between local structural disorder and tendency toward electron localization, and pave the way for future studies of doped spin liquids.},
doi = {10.1103/PhysRevX.6.041007},
journal = {Physical Review. X},
number = 4,
volume = 6,
place = {United States},
year = {Thu Oct 13 00:00:00 EDT 2016},
month = {Thu Oct 13 00:00:00 EDT 2016}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record

Citation Metrics:
Cited by: 49 works
Citation information provided by
Web of Science

Save / Share:

Works referenced in this record:

Resonating valence bonds: A new kind of insulator?
journal, February 1973


The Resonating Valence Bond State in La2CuO4 and Superconductivity
journal, March 1987


Evidence for a gapped spin-liquid ground state in a kagome Heisenberg antiferromagnet
journal, November 2015


Spin liquids in frustrated magnets
journal, March 2010


A Structurally Perfect S = 1 / 2 Kagomé Antiferromagnet
journal, October 2005

  • Shores, Matthew P.; Nytko, Emily A.; Bartlett, Bart M.
  • Journal of the American Chemical Society, Vol. 127, Issue 39
  • DOI: 10.1021/ja053891p

Site Specific X-ray Anomalous Dispersion of the Geometrically Frustrated Kagomé Magnet, Herbertsmithite, ZnCu 3 (OH) 6 Cl 2
journal, November 2010

  • Freedman, Danna E.; Han, Tianheng H.; Prodi, Andrea
  • Journal of the American Chemical Society, Vol. 132, Issue 45
  • DOI: 10.1021/ja1070398

A Cu 2+ ( S = 1 / 2 ) Kagomé Antiferromagnet: Mg x Cu 4− x (OH) 6 Cl 2
journal, April 2010

  • Chu, Shaoyan; McQueen, Tyrel M.; Chisnell, Robin
  • Journal of the American Chemical Society, Vol. 132, Issue 16
  • DOI: 10.1021/ja1008322

Fractionalized excitations in the spin-liquid state of a kagome-lattice antiferromagnet
journal, December 2012

  • Han, Tian-Heng; Helton, Joel S.; Chu, Shaoyan
  • Nature, Vol. 492, Issue 7429
  • DOI: 10.1038/nature11659

Theoretical prediction of a strongly correlated Dirac metal
journal, July 2014

  • Mazin, I. I.; Jeschke, Harald O.; Lechermann, Frank
  • Nature Communications, Vol. 5, Issue 1
  • DOI: 10.1038/ncomms5261

Prospect of quantum anomalous Hall and quantum spin Hall effect in doped kagome lattice Mott insulators
journal, May 2016

  • Guterding, Daniel; Jeschke, Harald O.; Valentí, Roser
  • Scientific Reports, Vol. 6, Issue 1
  • DOI: 10.1038/srep25988

The Hydride Anion in an Extended Transition Metal Oxide Array: LaSrCoO3H0.7
journal, March 2002


Infinite-layer iron oxide with a square-planar coordination
journal, December 2007

  • Tsujimoto, Y.; Tassel, C.; Hayashi, N.
  • Nature, Vol. 450, Issue 7172, p. 1062-1065
  • DOI: 10.1038/nature06382

Structural and electronic properties of sodium-intercalated C60
journal, April 1992

  • Rosseinsky, M. J.; Murphy, D. W.; Fleming, R. M.
  • Nature, Vol. 356, Issue 6368
  • DOI: 10.1038/356416a0

Mixed-valence-driven heavy-fermion behavior and superconductivity in KNi 2 Se 2
journal, August 2012


A ternary phase in Cu–Li–Mg system
journal, June 2007


X-ray photoelectron studies on some oxides and hydroxides of cobalt, nickel, and copper
journal, November 1975

  • McIntyre, N. S.; Cook, M. G.
  • Analytical Chemistry, Vol. 47, Issue 13
  • DOI: 10.1021/ac60363a034

Mixed valence: origins and developments
journal, September 2007

  • Day, Peter; Hush, Noel S.; Clark, Robin J. H.
  • Philosophical Transactions of the Royal Society A: Mathematical, Physical and Engineering Sciences, Vol. 366, Issue 1862
  • DOI: 10.1098/rsta.2007.2135

X-ray photoelectron spectroscopy of copper(II), copper(I), and mixed valence systems
journal, January 1976


Auger lines in x-ray photoelectron spectrometry
journal, May 1972


The stability of CuO and Cu2O surfaces during argon sputtering studied by XPS and AES
journal, March 1985


Triplet and singlet excitations in the valence bond crystal phase of the kagome lattice Heisenberg model
journal, April 2008


Absence of Diffusion in Certain Random Lattices
journal, March 1958


Electronic tunability of the frustrated triangular-lattice cluster magnet LiZn 2−x Mo 3 O 8
journal, January 2015

  • Sheckelton, John P.; Neilson, James R.; McQueen, Tyrel M.
  • Materials Horizons, Vol. 2, Issue 1
  • DOI: 10.1039/C4MH00166D

Mott Transition from a Spin Liquid to a Fermi Liquid in the Spin-Frustrated Organic Conductor κ ( ET ) 2 Cu 2 ( CN ) 3
journal, October 2005


Large enhancement of the thermopower in NaxCoO2 at high Na doping
journal, June 2006

  • Lee, Minhyea; Viciu, Liliana; Li, Lu
  • Nature Materials, Vol. 5, Issue 7
  • DOI: 10.1038/nmat1669

Spin-Liquid State in the S = 1 / 2 Hyperkagome Antiferromagnet Na 4 Ir 3 O 8
journal, September 2007


Spin-orbit coupling in the metallic and spin-liquid phases of Na 4 Ir 3 O 8
journal, February 2011


EXPGUI , a graphical user interface for GSAS
journal, April 2001


Works referencing / citing this record:

Frustration and quantum criticality
journal, May 2018


Local study of the insulating quantum kagome antiferromagnets YCu 3 ( OH ) 6 O x Cl 3 x ( x = 0 , 1 / 3 )
journal, July 2019


Quantum spin liquids
journal, January 2020


Thermodynamic, Dynamic, and Transport Properties of Quantum Spin Liquid in Herbertsmithite from an Experimental and Theoretical Point of View
journal, August 2019

  • Shaginyan, Vasily R.; Msezane, Alfred Z.; Amusia, Miron Ya.
  • Condensed Matter, Vol. 4, Issue 3
  • DOI: 10.3390/condmat4030075

Quantum Spin Liquids
text, January 2019