Abstract
The topochemical transformation of single crystals of Sr3Ir2O7 into Sr3Ir2O7F2 is reported via fluorine insertion. Characterization of the newly formed Sr3Ir2O7F2 phase shows a nearly complete oxidation of Ir4+ cations into Ir5+ that in turn drives the system from an antiferromagnetic Mott insulator with a half-filled Jeff=1/2 band into a nonmagnetic J=0 band insulator. First principles calculations reveal a remarkably flat insertion energy that locally drives the fluorination process to completion. Band structure calculations support the formation of a band insulator whose charge gap relies on the strong spin-orbit coupling inherent in the Ir metal ions of this compound.
| Original language | English |
|---|---|
| Article number | 155128 |
| Journal | Physical Review B |
| Volume | 98 |
| Issue number | 15 |
| DOIs | |
| State | Published - Oct 16 2018 |
Funding
This work was supported primarily by ARO Award No. W911NF-16-1-0361 (S.D.W., C.P., Z.P.). M.W.S. was supported by the MRSEC Program of the National Science Foundation under Award No. DMR-1121053. The MRL Shared Experimental Facilities are supported by the MRSEC Program of the NSF under Award No. DMR 1720256, a member of the NSF-funded Materials Research Facilities Network. The work at HYU was supported by the Basic Science Research Program through the National Research Foundation of Korea (NRF) funded by the Ministry of Science, ICT and Future Planning (Grant No. 2017R1A2B4009413). The work at ORNL's HFIR was sponsored by the Scientific User Facilities Division, Office of Science, Basic Energy Sciences, US Department of Energy. Research conducted at CHESS is supported by the NSF under Award No. DMR-1332208.