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Title: Novel Electronic Behavior Driving NdNiO 3 Metal-Insulator Transition

Abstract

We present evidence that the metal-insulator transition (MIT) in a tensile-strained NdNiO3 (NNO) film is facilitated by a redistribution of electronic density and that it neither requires Ni charge disproportionation nor a symmetry change [U. Staub et al., Phys. Rev. Lett. 88, 126402 (2002); R. Jaramillo et al., Nat. Phys. 10, 304 (2014)]. Given that epitaxial tensile strain in thin NNO films induces preferential occupancy of the e(g) d(x2-y2) orbital we propose that the larger transfer integral of this orbital state with the O 2p orbital state mediates a redistribution of electronic density from the Ni atom. A decrease in the Ni d(x2-y2) orbital occupation is directly observed by resonant inelastic x-ray scattering below the MIT temperature. Furthermore, an increase in the Nd charge occupancy is measured by x-ray absorption at the Nd L-3 edge. Both spin-orbit coupling and crystal field effects combine to break the degeneracy of the Nd 5d states, shifting the energy of the Nd e(g) d(x2-y2) orbit towards the Fermi level, allowing the A site to become an active acceptor during the MIT. This work identifies the relocation of electrons from the Ni 3d to the Nd 5d orbitals across the MIT. We propose that themore » insulating gap opens between the Ni 3d and O 2p states, resulting from Ni 3d electron localization. The transition seems to be neither a purely Mott-Hubbard transition nor a simple charge transfer.« less

Authors:
; ; ; ; ; ; ; ;
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
Argonne National Laboratory - Advanced Photon Source; USDOE Office of Science (SC); University of Illinois - Chicago
OSTI Identifier:
1391765
DOE Contract Number:  
AC02-06CH11357
Resource Type:
Journal Article
Journal Name:
Physical Review Letters
Additional Journal Information:
Journal Volume: 115; Journal Issue: 3; Journal ID: ISSN 0031-9007
Publisher:
American Physical Society (APS)
Country of Publication:
United States
Language:
English

Citation Formats

Upton, M. H., Choi, Yongseong, Park, Hyowon, Liu, Jian, Meyers, D., Chakhalian, J., Middey, S., Kim, Jong-Woo, and Ryan, Philip J. Novel Electronic Behavior Driving NdNiO3 Metal-Insulator Transition. United States: N. p., 2015. Web. doi:10.1103/PhysRevLett.115.036401.
Upton, M. H., Choi, Yongseong, Park, Hyowon, Liu, Jian, Meyers, D., Chakhalian, J., Middey, S., Kim, Jong-Woo, & Ryan, Philip J. Novel Electronic Behavior Driving NdNiO3 Metal-Insulator Transition. United States. doi:10.1103/PhysRevLett.115.036401.
Upton, M. H., Choi, Yongseong, Park, Hyowon, Liu, Jian, Meyers, D., Chakhalian, J., Middey, S., Kim, Jong-Woo, and Ryan, Philip J. Wed . "Novel Electronic Behavior Driving NdNiO3 Metal-Insulator Transition". United States. doi:10.1103/PhysRevLett.115.036401.
@article{osti_1391765,
title = {Novel Electronic Behavior Driving NdNiO3 Metal-Insulator Transition},
author = {Upton, M. H. and Choi, Yongseong and Park, Hyowon and Liu, Jian and Meyers, D. and Chakhalian, J. and Middey, S. and Kim, Jong-Woo and Ryan, Philip J.},
abstractNote = {We present evidence that the metal-insulator transition (MIT) in a tensile-strained NdNiO3 (NNO) film is facilitated by a redistribution of electronic density and that it neither requires Ni charge disproportionation nor a symmetry change [U. Staub et al., Phys. Rev. Lett. 88, 126402 (2002); R. Jaramillo et al., Nat. Phys. 10, 304 (2014)]. Given that epitaxial tensile strain in thin NNO films induces preferential occupancy of the e(g) d(x2-y2) orbital we propose that the larger transfer integral of this orbital state with the O 2p orbital state mediates a redistribution of electronic density from the Ni atom. A decrease in the Ni d(x2-y2) orbital occupation is directly observed by resonant inelastic x-ray scattering below the MIT temperature. Furthermore, an increase in the Nd charge occupancy is measured by x-ray absorption at the Nd L-3 edge. Both spin-orbit coupling and crystal field effects combine to break the degeneracy of the Nd 5d states, shifting the energy of the Nd e(g) d(x2-y2) orbit towards the Fermi level, allowing the A site to become an active acceptor during the MIT. This work identifies the relocation of electrons from the Ni 3d to the Nd 5d orbitals across the MIT. We propose that the insulating gap opens between the Ni 3d and O 2p states, resulting from Ni 3d electron localization. The transition seems to be neither a purely Mott-Hubbard transition nor a simple charge transfer.},
doi = {10.1103/PhysRevLett.115.036401},
journal = {Physical Review Letters},
issn = {0031-9007},
number = 3,
volume = 115,
place = {United States},
year = {2015},
month = {7}
}

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