Electronic and structural response to pressure in the hyperkagome-lattice Na3Ir3O8

Sun, F.; Zheng, H.; Liu, Y.; Sandoval, E. D.; Xu, C.; Xu, J.; Jin, C. Q.; Sun, C. J.; Yang, W. G.; Mao, H. K.; Mitchell, J. F.; Kolmogorov, A. N.; Haskel, D.

doi:10.1103/PhysRevB.98.085131

Electronic and structural response to pressure in the hyperkagome-lattice ${Na}_{3} {Ir}_{3} O_{8}$

Journal Article · Mon Aug 20 00:00:00 EDT 2018 · Physical Review B

DOI:https://doi.org/10.1103/PhysRevB.98.085131· OSTI ID:1472084

Sun, F. ^[1]; Zheng, H. ^[2]; Liu, Y. ^[3]; Sandoval, E. D. ^[4]; Xu, C. ^[5]; Xu, J. ^[6]; Jin, C. Q. ^[7]; Sun, C. J. ^[2]; Yang, W. G. ^[8]; Mao, H. K. ^[8]; Mitchell, J. F. ^[2]; Kolmogorov, A. N. ^[4]; Haskel, D. ^[2]

Center for High Pressure Science and Technology Advanced Research (HPSTAR), Beijing (China); Argonne National Lab. (ANL), Argonne, IL (United States); Chinese Academy of Sciences (CAS), Beijing (China)
Argonne National Lab. (ANL), Argonne, IL (United States)
Chinese Academy of Sciences (CAS), Beijing (China); Xi'an Modern Chemistry Research Institute, Xi'an (China)
Binghamton Univ., State Univ. of New York, Binghamton, NY (United States)
Center for High Pressure Science and Technology Advanced Research (HPSTAR), Beijing (China)
Argonne National Lab. (ANL), Argonne, IL (United States); Northern Illinois Univ., DeKalb, IL (United States)
Chinese Academy of Sciences (CAS), Beijing (China); Collaborative Innovation Center of Quantum Matter, Beijing (China)
Center for High Pressure Science and Technology Advanced Research (HPSTAR), Beijing (China); Carnegie Inst. of Washington, Argonne, IL (United States)

Here, the hyper-kagome lattice iridate Na₃Ir₃O₈, closely related to spin liquid candidate Na₄Ir₃O₈, is unusual in that spin-orbit interactions acting on the 1/3-filled J_eff = 1/2 state lead to a semimetallic ground state, in contrast to the conventional insulating Mott state stabilized by S-O interactions in the 1/2-filled J_eff = 1/2 state of other iridates including Na₄Ir₃O₈. We have studied the evolution of crystal structure, electronic structure, and transport in Na₃Ir₃O₈ under high pressure using x-ray diffraction, x-ray absorption near edge structure, and electrical resistance measurements in a diamond anvil cell. The study was augmented by the use of ab initio calculations, which provided insight into pressure-induced changes in crystal and electronic structure. We found that Na₃Ir₃O₈ transforms from a semimetal to an insulator under pressure, with an estimated energy gap that increases to about 130 meV at P similar to 9 GPa. At approximately 10 GPa, a cubic-to-monoclinic structural transition takes place between two insulating phases. This structural transition features a sizable volume collapse and a high-pressure phase characterized by apparent dimerization of Ir-Ir distances, wide dispersion of Ir-O-Ir bond angles, and an increase in the occupation of 5d states. Although the energy gap is reduced in the high-pressure phase, insulating behavior remains to the highest pressures similar to 1 Mbar. The strongly pressure-dependent insulating gap shows a positive correlation with the expectation value of the angular part of the S-O interaction, < L • S >, which may indicate an active role of S-O interactions in stabilizing the insulating state that emerges in the compressed Na₃Ir₃O₈ structure.

View Accepted Manuscript (DOE)

Research Organization:: Argonne National Lab. (ANL), Argonne, IL (United States)

Sponsoring Organization:: USDOE National Nuclear Security Administration (NNSA)

Grant/Contract Number:: AC02-06CH11357; FG02-99ER45775; NA0001974

OSTI ID:: 1472084

Alternate ID(s):: OSTI ID: 1465243

Journal Information:: Physical Review B, Journal Name: Physical Review B Journal Issue: 8 Vol. 98; ISSN 2469-9950; ISSN PRBMDO

Publisher:: American Physical Society (APS)Copyright Statement

Country of Publication:: United States

Language:: English

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