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Title: Polarity compensation in ultra-thin films of complex oxides: The case of a perovskite nickelate

Abstract

In this study, we address the fundamental issue of growth of perovskite ultra-thin films under the condition of a strong polar mismatch at the heterointerface exemplified by the growth of a correlated metal LaNiO 3 on the band insulator SrTiO 3 along the pseudo cubic [111] direction. While in general the metallic LaNiO 3 film can effectively screen this polarity mismatch, we establish that in the ultra-thin limit, films are insulating in nature and require additional chemical and structural reconstruction to compensate for such mismatch. A combination of in-situ reflection high-energy electron diffraction recorded during the growth, X-ray diffraction, and synchrotron based resonant X-ray spectroscopy reveal the formation of a chemical phase La 2Ni 2O 5 (Ni 2+) for a few unit-cell thick films. First-principles layer-resolved calculations of the potential energy across the nominal LaNiO 3/SrTiO 3 interface confirm that the oxygen vacancies can efficiently reduce the electric field at the interface.

Authors:
 [1];  [1];  [1];  [1];  [1];  [1];  [2];  [1];  [1]
  1. University of Arkansas, Fayetteville, AR (United States). Dept. of Physics.
  2. Argonne National Lab. (ANL), Argonne, IL (United States)
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1221158
Alternate Identifier(s):
OSTI ID: 1241336
Grant/Contract Number:  
AC02-06CH11357
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Scientific Reports
Additional Journal Information:
Journal Volume: 4; Journal ID: ISSN 2045-2322
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; electronic properties and materials; surfaces; interfaces and thin films; surfaces, interfaces and thin films

Citation Formats

Middey, S., Rivero, P., Meyers, D., Kareev, M., Liu, X., Cao, Y., Freeland, J. W., Barraza-Lopez, S., and Chakhalian, J.. Polarity compensation in ultra-thin films of complex oxides: The case of a perovskite nickelate. United States: N. p., 2014. Web. doi:10.1038/srep06819.
Middey, S., Rivero, P., Meyers, D., Kareev, M., Liu, X., Cao, Y., Freeland, J. W., Barraza-Lopez, S., & Chakhalian, J.. Polarity compensation in ultra-thin films of complex oxides: The case of a perovskite nickelate. United States. https://doi.org/10.1038/srep06819
Middey, S., Rivero, P., Meyers, D., Kareev, M., Liu, X., Cao, Y., Freeland, J. W., Barraza-Lopez, S., and Chakhalian, J.. Wed . "Polarity compensation in ultra-thin films of complex oxides: The case of a perovskite nickelate". United States. https://doi.org/10.1038/srep06819. https://www.osti.gov/servlets/purl/1221158.
@article{osti_1221158,
title = {Polarity compensation in ultra-thin films of complex oxides: The case of a perovskite nickelate},
author = {Middey, S. and Rivero, P. and Meyers, D. and Kareev, M. and Liu, X. and Cao, Y. and Freeland, J. W. and Barraza-Lopez, S. and Chakhalian, J.},
abstractNote = {In this study, we address the fundamental issue of growth of perovskite ultra-thin films under the condition of a strong polar mismatch at the heterointerface exemplified by the growth of a correlated metal LaNiO3 on the band insulator SrTiO3 along the pseudo cubic [111] direction. While in general the metallic LaNiO3 film can effectively screen this polarity mismatch, we establish that in the ultra-thin limit, films are insulating in nature and require additional chemical and structural reconstruction to compensate for such mismatch. A combination of in-situ reflection high-energy electron diffraction recorded during the growth, X-ray diffraction, and synchrotron based resonant X-ray spectroscopy reveal the formation of a chemical phase La2Ni2O5 (Ni2+) for a few unit-cell thick films. First-principles layer-resolved calculations of the potential energy across the nominal LaNiO3/SrTiO3 interface confirm that the oxygen vacancies can efficiently reduce the electric field at the interface.},
doi = {10.1038/srep06819},
url = {https://www.osti.gov/biblio/1221158}, journal = {Scientific Reports},
issn = {2045-2322},
number = ,
volume = 4,
place = {United States},
year = {2014},
month = {10}
}

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Cited by: 25 works
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Works referenced in this record:

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    Works referencing / citing this record:

    Tuning Bifunctional Oxygen Electrocatalysts by Changing the A-Site Rare-Earth Element in Perovskite Nickelates
    journal, August 2018


    A Coherently Strained Monoclinic [111]PbTiO 3 Film Exhibiting Zero Poisson's Ratio State
    journal, June 2019


    Interfacial Charge Engineering in Ferroelectric-Controlled Mott Transistors
    journal, June 2017


    Polar metals by geometric design
    journal, April 2016


    Hybridization-controlled charge transfer and induced magnetism at correlated oxide interfaces
    journal, January 2016


    Charge transfer-induced magnetic exchange bias and electron localization in (111)- and (001)-oriented LaNiO 3 /LaMnO 3 superlattices
    journal, March 2017


    Carrier localization in perovskite nickelates from oxygen vacancies
    journal, October 2019


    Rare-earth nickelates R NiO 3 : thin films and heterostructures
    journal, February 2018


    Design of n - and p -type oxide thermoelectrics in LaNiO 3 / SrTiO 3 ( 001 ) superlattices exploiting interface polarity
    journal, March 2017


    Manipulating the polar mismatch at the LaNi O 3 / SrTi O 3 (111) interface
    journal, April 2017


    Epitaxial strain modulated electronic properties of interface controlled nickelate superlattices
    journal, July 2018


    Design of a Mott Multiferroic from a Nonmagnetic Polar Metal
    journal, August 2015


    Mott Electrons in an Artificial Graphenelike Crystal of Rare-Earth Nickelate
    journal, February 2016


    Disentangled Cooperative Orderings in Artificial Rare-Earth Nickelates
    journal, April 2018


    Hybridization-Switching Induced Mott Transition in A B O 3 Perovskites
    journal, January 2019


    Role of polar compensation in interfacial ferromagnetism of LaNiO 3 / CaMnO 3 superlattices
    journal, July 2017


    Polarity-driven oxygen vacancy formation in ultrathin LaNiO 3 films on SrTiO 3
    journal, October 2017