Interfacial charge transfer and its impact on transport properties of LaNiO3/LaFeO3 superlattices

Wang, Le; Yang, Zhifei; Koirala, Krishna Prasad; Bowden, Mark E.; Freeland, John W.; Sushko, Peter V.; Kuo, Cheng-Tai; Chambers, Scott A.; Wang, Chongmin; Jalan, Bharat; Du, Yingge

doi:10.1126/sciadv.adq6687

Interfacial charge transfer and its impact on transport properties of LaNiO₃/LaFeO₃ superlattices

Journal Article · Wed Dec 18 00:00:00 EST 2024 · Science Advances

DOI:https://doi.org/10.1126/sciadv.adq6687· OSTI ID:2483607

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Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)
Univ. of Minnesota, Minneapolis, MN (United States)
Argonne National Laboratory (ANL), Argonne, IL (United States). Advanced Photon Source (APS)
SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States). Stanford Synchrotron Radiation Lightsource (SSRL)
Pacific Northwest National Laboratory (PNNL), Richland, WA (United States). Environmental Molecular Sciences Laboratory (EMSL)

Charge transfer or redistribution at oxide heterointerfaces is a critical phenomenon, often leading to remarkable properties such as two-dimensional electron gas and interfacial ferromagnetism. Despite studies on LaNiO₃/LaFeO₃ superlattices and heterostructures, the direction and magnitude of the charge transfer remain debated, with some suggesting no charge transfer due to the high stability of Fe³⁺ (3d⁵). Here, we synthesized a series of epitaxial LaNiO₃/LaFeO₃ superlattices and demonstrated partial (up to ~0.5 e^-/interface unit cell) charge transfer from Fe to Ni near the interface, supported by density functional theory simulations and spectroscopic evidence of changes in Ni and Fe oxidation states. The electron transfer from LaFeO₃ to LaNiO₃ and the subsequent rearrangement of the Fe 3d band create an unexpected metallic ground state within the LaFeO₃ layer, strongly influencing the in-plane transport properties across the superlattice. Moreover, we establish a direct correlation between interfacial charge transfer and in-plane electrical transport properties, providing insights for designing functional oxide heterostructures with emerging properties.

View Accepted Manuscript (DOE)

Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States). Advanced Photon Source (APS); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). National Energy Research Scientific Computing Center (NERSC); Pacific Northwest National Laboratory (PNNL), Richland, WA (United States); SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States); SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States). Stanford Synchrotron Radiation Lightsource (SSRL)

Sponsoring Organization:: National Research Foundation of Korea (NRF); National Science Foundation (NSF); US Air Force Office of Scientific Research (AFOSR); USDOE Office of Science (SC), Basic Energy Sciences (BES)

Contributing Organization:: Argonne National Laboratory (ANL); Lawrence Berkeley National Laboratory (LBNL); Pacific Northwest National Laboratory (PNNL)

Grant/Contract Number:: AC02-05CH11231; AC02-76SF00515; AC05-76RL01830

OSTI ID:: 2483607

Alternate ID(s):: OSTI ID: 2497905

Report Number(s):: PNNL-SA--198926

Journal Information:: Science Advances, Journal Name: Science Advances Journal Issue: 51 Vol. 10; ISSN 2375-2548

Publisher:: AAASCopyright Statement

Country of Publication:: United States

Language:: English

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