Dynamical correlations leading to site and orbital selective Mott insulator transition in hydrogen doped SmNiO3

Bhat, Soumya S.; Singh, Vijay; Herath, Uthpala; Varughese, Bilvin; Sankaranarayanan, Subramanian K. R. S.; Park, Hyowon; Romero, Aldo H.

doi:10.1103/PhysRevB.109.205124

Dynamical correlations leading to site and orbital selective Mott insulator transition in hydrogen doped SmNiO₃

Journal Article · Thu May 09 00:00:00 EDT 2024 · Physical Review. B

DOI:https://doi.org/10.1103/PhysRevB.109.205124· OSTI ID:2571539

^[1]; ^[2]; ^[1]; Varughese, Bilvin ^[3]; Sankaranarayanan, Subramanian K. R. S. ^[4]; Park, Hyowon ^[4]; ^[1]

West Virginia Univ., Morgantown, WV (United States)
GITAM School of Science, Bangalore (India)
Univ. of Illinois, Chicago, IL (United States)
Univ. of Illinois, Chicago, IL (United States); Argonne National Laboratory (ANL), Argonne, IL (United States)

Electron doping induces metal -to -insulator transition (MIT) in SmNiO₃ as realized by experiments. While earlier density functional theory (DFT) studies with static correlations fell short of explaining the recent MIT observations at lower hydrogen concentrations, we present a comprehensive computational investigation employing an advanced approach. We combine DFT with dynamical mean field theory (DFT + DMFT) to efficiently analyze the insulating behavior of hydrogen -doped SmNiO₃. In contrast to previous theoretical works, our calculations predict an insulator transition occurring at a reduced doping level of H:Ni = 0.5:1. Specifically, while the DFT + U method reveals a gap opening between p-to-d orbitals, the DMFT approach highlights a gap opening between d-to-d orbitals. Our findings uncover a selective Mott transition in site and orbital characteristics, with the Ni ions proximate to the doped hydrogen exhibiting Mott -like traits. Notably, DMFT calculations highlight a pronounced dependence on Hund's parameter J, implying the presence of Hundness in the Mott insulator. Finally, this study underscores the necessity of accounting for dynamical correlations to accurately describe the electronic structure of strongly correlated electron-doped rare-earth nickelates.

View Accepted Manuscript (DOE)

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

Sponsoring Organization:: National Science Foundation (NSF); USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF)

Grant/Contract Number:: AC02-06CH11357; SC0021375

OSTI ID:: 2571539

Alternate ID(s):: OSTI ID: 2356861

Journal Information:: Physical Review. B, Journal Name: Physical Review. B Journal Issue: 20 Vol. 109; ISSN 2469-9969; ISSN 2469-9950

Publisher:: American Physical Society (APS)Copyright Statement

Country of Publication:: United States

Language:: English

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Related Subjects

75 CONDENSED MATTER PHYSICS
SUPERCONDUCTIVITY AND SUPERFLUIDITY
dynamical mean field theory
electronic structure
first-principles calculations
metal-insulator transition
nickelates
strongly correlated systems