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Title: Charge partitioning and anomalous hole doping in Rh-doped Sr 2 IrO 4

The simultaneous presence of sizable spin-orbit interactions and electron correlations in iridium oxides has led to predictions of novel ground states including Dirac semimetals, Kitaev spin liquids, and superconductivity. Electron and hole doping studies of spin-orbit assisted Mott insulator Sr 2IrO 4 are being intensively pursued due to extensive parallels with the La 2CuO 4 parent compound of cuprate superconductors. In particular, the mechanism of charge doping associated with replacement of Ir with Rh ions remains controversial with profound consequences for the interpretation of electronic structure and transport data. Using x-ray absorption near edge structure measurements at the Rh L, K, and Ir L edges we observe anomalous evolution of charge partitioning between Rh and Ir with Rh doping. The partitioning of charge between Rh and Ir sites progresses in a way that holes are initially doped into the J eff = 1/2 band at low x only to be removed from it at higher x values. Furthermore, this anomalous hole doping naturally explains the reentrant insulating phase in the phase diagram of Sr 2Ir 1–xRh xO 4 and ought to be considered when searching for superconductivity and other emergent phenomena in iridates doped with 4d elements.
 [1] ;  [2] ;  [3] ;  [3] ;  [4] ;  [5]
  1. Argonne National Lab. (ANL), Argonne, IL (United States); Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
  2. Argonne National Lab. (ANL), Argonne, IL (United States); Washington Univ., St. Louis, MO (United States); Brookhaven National Lab. (BNL), Upton, NY (United States)
  3. Univ. of Colorado, Boulder, CO (United States)
  4. Univ. zu Koln, Koln (Germany)
  5. Argonne National Lab. (ANL), Argonne, IL (United States)
Publication Date:
Report Number(s):
BNL-113512-2017-JA; LA-UR-17-30769
Journal ID: ISSN 2469-9950; PRBMDO; R&D Project: PO011; KC0201060; TRN: US1700712
Grant/Contract Number:
SC0012704; AC02-06CH11357; AC52-06NA25396
Accepted Manuscript
Journal Name:
Physical Review B
Additional Journal Information:
Journal Volume: 95; Journal Issue: 6; Journal ID: ISSN 2469-9950
American Physical Society (APS)
Research Org:
Brookhaven National Laboratory (BNL), Upton, NY (United States); Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Country of Publication:
United States
OSTI Identifier:
Alternate Identifier(s):
OSTI ID: 1344005; OSTI ID: 1431080