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Title: Electronic Structure of a Graphene-like Artificial Crystal of NdNiO3

Abstract

Artificial complex-oxide heterostructures containing ultrathin buried layers grown along the pseudocubic [111] direction have been predicted to host a plethora of exotic quantum states arising from the graphene-like lattice geometry and the interplay between strong electronic correlations and band topology. To date, however, electronic-structural investigations of such atomic layers remain an immense challenge due to the shortcomings of conventional surface-sensitive probes, with typical information depths of a few Ångstroms. Here, we use a combination of bulk-sensitive soft x-ray angle-resolved photoelectron spectroscopy (SX-ARPES), hard x-ray photoelectron spectroscopy (HAXPES) and state-of-the-art first-principles calculations to demonstrate a direct and robust method for extracting momentum-resolved and angle-integrated valence-band electronic structure of an ultrathin buckled graphene-like layer of NdNiO3 confined between two 4-unit cell-thick layers of insulating LaAlO3. The momentum-resolved dispersion of the buried Ni d states near the Fermi level obtained via SX-ARPES is in excellent agreement with the first-principles calculations and establishes the realization of an antiferro-orbital order in this artificial lattice. The HAXPES measurements reveal the presence of a valence-band (VB) bandgap of 265 meV. Lastly, our findings open a promising avenue for designing and investigating quantum states of matter with exotic order and topology in a few buried layers.

Authors:
 [1];  [2];  [3];  [1]; ORCiD logo [1]; ORCiD logo [4];  [2];  [4];  [5];  [6];  [7];  [8];  [9];  [10]; ORCiD logo [3];  [2];  [1]
  1. Temple Univ., Philadelphia, PA (United States)
  2. Rutgers Univ., Piscataway, NJ (United States)
  3. Univ. of Duisburg-Essen, Duisburg (Germany). Center for Nanointegration Duisburg-Essen (CENIDE)
  4. Indian Inst. of Science, Bengaluru (India)
  5. Paul Scherrer Inst. (PSI), Villigen (Switzerland). Swiss Light Source; National Inst. of Materials Physics, Magurele (Romania)
  6. Chinese Academy of Sciences (CAS), Beijing (China). Beijing National Lab. for Condensed-Matter Physics and Institute of Physics
  7. Chinese Academy of Sciences (CAS), Beijing (China). Beijing National Lab. for Condensed-Matter Physics and Institute of Physics; Collaborative Innovation Center of Quantum Matter, Beijing (China)
  8. Paul Scherrer Inst. (PSI), Villigen (Switzerland). Swiss Light Source
  9. Science and Technology Facilities Council (STFC), Oxford (United Kingdom). Diamond Light Source, Ltd.
  10. Univ. of West Bohemia, Pilsen (Czech Republic). New Technologies-Research Center
Publication Date:
Research Org.:
Temple Univ., Philadelphia, PA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1774776
Grant/Contract Number:  
SC0019297
Resource Type:
Accepted Manuscript
Journal Name:
Nano Letters
Additional Journal Information:
Journal Volume: 19; Journal Issue: 11; Journal ID: ISSN 1530-6984
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; Strongly correlated oxides; soft X-ray angle-resolved photoelectron spectroscopy; hard X-ray photoelectron spectroscopy; Band structure; Photoemission; Layers; Lattices; Colloids

Citation Formats

Arab, Arian, Liu, Xiaoran, Köksal, Okan, Yang, Weibing, Chandrasena, Ravini U., Middey, Srimanta, Kareev, Mikhail, Kumar, Siddharth, Husanu, Marius-Adrian, Yang, Zhenzhong, Gu, Lin, Strocov, Vladimir N., Lee, Tien-Lin, Minár, Jan, Pentcheva, Rossitza, Chakhalian, Jak, and Gray, Alexander X. Electronic Structure of a Graphene-like Artificial Crystal of NdNiO3. United States: N. p., 2019. Web. doi:10.1021/acs.nanolett.9b03962.
Arab, Arian, Liu, Xiaoran, Köksal, Okan, Yang, Weibing, Chandrasena, Ravini U., Middey, Srimanta, Kareev, Mikhail, Kumar, Siddharth, Husanu, Marius-Adrian, Yang, Zhenzhong, Gu, Lin, Strocov, Vladimir N., Lee, Tien-Lin, Minár, Jan, Pentcheva, Rossitza, Chakhalian, Jak, & Gray, Alexander X. Electronic Structure of a Graphene-like Artificial Crystal of NdNiO3. United States. https://doi.org/10.1021/acs.nanolett.9b03962
Arab, Arian, Liu, Xiaoran, Köksal, Okan, Yang, Weibing, Chandrasena, Ravini U., Middey, Srimanta, Kareev, Mikhail, Kumar, Siddharth, Husanu, Marius-Adrian, Yang, Zhenzhong, Gu, Lin, Strocov, Vladimir N., Lee, Tien-Lin, Minár, Jan, Pentcheva, Rossitza, Chakhalian, Jak, and Gray, Alexander X. Wed . "Electronic Structure of a Graphene-like Artificial Crystal of NdNiO3". United States. https://doi.org/10.1021/acs.nanolett.9b03962. https://www.osti.gov/servlets/purl/1774776.
@article{osti_1774776,
title = {Electronic Structure of a Graphene-like Artificial Crystal of NdNiO3},
author = {Arab, Arian and Liu, Xiaoran and Köksal, Okan and Yang, Weibing and Chandrasena, Ravini U. and Middey, Srimanta and Kareev, Mikhail and Kumar, Siddharth and Husanu, Marius-Adrian and Yang, Zhenzhong and Gu, Lin and Strocov, Vladimir N. and Lee, Tien-Lin and Minár, Jan and Pentcheva, Rossitza and Chakhalian, Jak and Gray, Alexander X.},
abstractNote = {Artificial complex-oxide heterostructures containing ultrathin buried layers grown along the pseudocubic [111] direction have been predicted to host a plethora of exotic quantum states arising from the graphene-like lattice geometry and the interplay between strong electronic correlations and band topology. To date, however, electronic-structural investigations of such atomic layers remain an immense challenge due to the shortcomings of conventional surface-sensitive probes, with typical information depths of a few Ångstroms. Here, we use a combination of bulk-sensitive soft x-ray angle-resolved photoelectron spectroscopy (SX-ARPES), hard x-ray photoelectron spectroscopy (HAXPES) and state-of-the-art first-principles calculations to demonstrate a direct and robust method for extracting momentum-resolved and angle-integrated valence-band electronic structure of an ultrathin buckled graphene-like layer of NdNiO3 confined between two 4-unit cell-thick layers of insulating LaAlO3. The momentum-resolved dispersion of the buried Ni d states near the Fermi level obtained via SX-ARPES is in excellent agreement with the first-principles calculations and establishes the realization of an antiferro-orbital order in this artificial lattice. The HAXPES measurements reveal the presence of a valence-band (VB) bandgap of 265 meV. Lastly, our findings open a promising avenue for designing and investigating quantum states of matter with exotic order and topology in a few buried layers.},
doi = {10.1021/acs.nanolett.9b03962},
journal = {Nano Letters},
number = 11,
volume = 19,
place = {United States},
year = {Wed Oct 23 00:00:00 EDT 2019},
month = {Wed Oct 23 00:00:00 EDT 2019}
}

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