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Title: Electron Doping of Proposed Kagome Quantum Spin Liquid Produces Localized States in the Band Gap

Carrier doping of quantum spin liquids is a long-proposed route to the emergence of high-temperature superconductivity. Electrochemical intercalation in kagome hydroxyl halide materials shows that samples remain insulating across a wide range of electron counts. In this work, we demonstrate through first-principles density-functional calculations, corrected for self-interaction, the mechanism by which electrons remain localized in various Zn-Cu hydroxyl halides, independent of the chemical identity of the dopant - the formation of polaronic states with attendant lattice displacements and a dramatic narrowing of bandwidth upon electron addition. The same theoretical method applied to electron doping in cuprate Nd 2CuO 4 correctly produces a metallic state when the initially formed polaron dissolves into an extended state. In conclusion, our general findings explain the insulating behavior in a wide range of 'doped' quantum magnets and demonstrate that new quantum spin liquid host materials are needed to realize metallicity borne of a spin liquid.
Authors:
 [1] ;  [2] ;  [3] ;  [3] ;  [3] ;  [4] ;  [5]
  1. Univ. of Colorado, Boulder, CO (United States); Southern University of Science and Technology, Shenzhen (China)
  2. Southern University of Science and Technology, Shenzhen (China)
  3. Johns Hopkins Univ., Baltimore, MD (United States)
  4. National Renewable Energy Lab. (NREL), Golden, CO (United States)
  5. Univ. of Colorado, Boulder, CO (United States)
Publication Date:
Report Number(s):
NREL/JA-5K00-72735
Journal ID: ISSN 0031-9007; PRLTAO
Grant/Contract Number:
AC36-08GO28308; SC0010467; FG02-08ER46544; AC02-05CH11231
Type:
Accepted Manuscript
Journal Name:
Physical Review Letters
Additional Journal Information:
Journal Volume: 121; Journal Issue: 18; Journal ID: ISSN 0031-9007
Publisher:
American Physical Society (APS)
Research Org:
National Renewable Energy Lab. (NREL), Golden, CO (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Materials Sciences & Engineering Division; USDOE Office of Energy Efficiency and Renewable Energy (EERE)
Country of Publication:
United States
Language:
English
Subject:
71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSICS; quantum material; density functional theory
OSTI Identifier:
1485568
Alternate Identifier(s):
OSTI ID: 1479856

Liu, Qihang, Yao, Qiushi, Kelly, Z. A., Pasco, C. M., McQueen, T. M., Lany, S., and Zunger, Alex. Electron Doping of Proposed Kagome Quantum Spin Liquid Produces Localized States in the Band Gap. United States: N. p., Web. doi:10.1103/PhysRevLett.121.186402.
Liu, Qihang, Yao, Qiushi, Kelly, Z. A., Pasco, C. M., McQueen, T. M., Lany, S., & Zunger, Alex. Electron Doping of Proposed Kagome Quantum Spin Liquid Produces Localized States in the Band Gap. United States. doi:10.1103/PhysRevLett.121.186402.
Liu, Qihang, Yao, Qiushi, Kelly, Z. A., Pasco, C. M., McQueen, T. M., Lany, S., and Zunger, Alex. 2018. "Electron Doping of Proposed Kagome Quantum Spin Liquid Produces Localized States in the Band Gap". United States. doi:10.1103/PhysRevLett.121.186402.
@article{osti_1485568,
title = {Electron Doping of Proposed Kagome Quantum Spin Liquid Produces Localized States in the Band Gap},
author = {Liu, Qihang and Yao, Qiushi and Kelly, Z. A. and Pasco, C. M. and McQueen, T. M. and Lany, S. and Zunger, Alex},
abstractNote = {Carrier doping of quantum spin liquids is a long-proposed route to the emergence of high-temperature superconductivity. Electrochemical intercalation in kagome hydroxyl halide materials shows that samples remain insulating across a wide range of electron counts. In this work, we demonstrate through first-principles density-functional calculations, corrected for self-interaction, the mechanism by which electrons remain localized in various Zn-Cu hydroxyl halides, independent of the chemical identity of the dopant - the formation of polaronic states with attendant lattice displacements and a dramatic narrowing of bandwidth upon electron addition. The same theoretical method applied to electron doping in cuprate Nd2CuO4 correctly produces a metallic state when the initially formed polaron dissolves into an extended state. In conclusion, our general findings explain the insulating behavior in a wide range of 'doped' quantum magnets and demonstrate that new quantum spin liquid host materials are needed to realize metallicity borne of a spin liquid.},
doi = {10.1103/PhysRevLett.121.186402},
journal = {Physical Review Letters},
number = 18,
volume = 121,
place = {United States},
year = {2018},
month = {10}
}

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