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Chin. Phys. B, 2021, Vol. 30(4): 046102    DOI: 10.1088/1674-1056/abe0c8

X-ray absorption investigation of the site occupancies of the copper element in nominal Cu3Zn(OH)6FBr

Ruitang Wang(王瑞塘)1,2, Xiaoting Li(李效亭)3, Xin Han(韩鑫)1,2, Jiaqi Lin(林佳琪)1,2, Yong Wang(王勇)4, Tian Qian(钱天)1,5, Hong Ding(丁洪)1,5, Youguo Shi(石友国)1,2, and Xuerong Liu(柳学榕)3,†
1 Beijing National Laboratory for Condensed Matter Physics and Institute of Physics, Chinese Academy of Sciences, Beijing 100190, China; 2 University of Chinese Academy of Sciences, Beijing 100049, China; 3 School of Physical Science and Technology, ShanghaiTech University, Shanghai 201210, China; 4 Shanghai Synchrotron Radiation Facility, Shanghai Institute of Applied Physics, Chinese Academy of Sciences, Shanghai 201800, China; 5 Songshan Lake Materials Laboratory, Dongguan 250100, China
Abstract  With Zn substitution to the three-dimensional antiferromagnetically ordered barlowite Cu4(OH)6FBr, Cu3Zn(OH)6FBr shows no magnetic phase transition down to 50 mK, and the system is suggested to be a two-dimensional kagomé quantum spin liquid [Chin. Phys. Lett. 34 077502 (2017)]. A key issue to identify such phase diagram is the exact chemical formula of the substituted compound. With Cu L-edge x-ray absorption spectrum (XAS) combined with the MultiX XAS calculations, we evaluate the Cu concentration in a nominal Cu3Zn(OH)6FBr sample. Our results show that although the Cu concentration is 2.80, close to the expected value, there is 34% residual Cu occupation in intersite layers between kagomé layers. Thus the Zn substitution of the intersite layers is not complete, and likely it intrudes the kagomé layers.
Keywords:  x-ray absorption spectrum      barlowite spin liquid candidate      chemical occupations  
Received:  30 December 2020      Revised:  22 January 2021      Accepted manuscript online:  28 January 2021
PACS:  61.05.cj (X-ray absorption spectroscopy: EXAFS, NEXAFS, XANES, etc.)  
  75.10.Kt (Quantum spin liquids, valence bond phases and related phenomena)  
  71.15.Mb (Density functional theory, local density approximation, gradient and other corrections)  
  61.50.Nw (Crystal stoichiometry)  
Fund: Project supported by the National Natural Science Foundation of China (Grant Nos. 11934017 and 11774399), the Key Research and Development Program of China (Grant No. 2016YFA0401000), the Chinese Academy of Sciences (Grant No. 112111KYSB20170059), and the K. C. Wong Education Foundation (Grant No. GJTD-2018-01).
Corresponding Authors:  Corresponding author. E-mail:   

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Ruitang Wang(王瑞塘), Xiaoting Li(李效亭), Xin Han(韩鑫), Jiaqi Lin(林佳琪), Yong Wang(王勇), Tian Qian(钱天), Hong Ding(丁洪), Youguo Shi(石友国), and Xuerong Liu(柳学榕) X-ray absorption investigation of the site occupancies of the copper element in nominal Cu3Zn(OH)6FBr 2021 Chin. Phys. B 30 046102

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