skip to main content
DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information

This content will become publicly available on September 9, 2020

Title: Probing single-unit-cell resolved electronic structure modulations in oxide superlattices with standing-wave photoemission

Abstract

Control of structural coupling at complex-oxide interfaces is a powerful platform for creating ultrathin layers with electronic and magnetic properties unattainable in the bulk. Yet, with the capability to design and control the electronic structure of such buried layers and interfaces at a unit-cell level, a new challenge emerges to be able to probe these engineered emergent phenomena with depth-dependent atomic resolution as well as element- and orbital selectivity. In this work, we utilize a combination of core-level and valence-band soft x-ray standing-wave photoemission spectroscopy, in conjunction with scanning transmission electron microscopy, to probe the depth-dependent and single-unit-cell resolved electronic structure of an isovalent manganite superlattice [Eu 0.7Sr 0.3MnO 3/La 0.7Sr 0.3MnO 3]×15 wherein the electronic-structural properties are intentionally modulated with depth via engineered oxygen octahedra rotations/tilts and A-site displacements. Our unit-cell resolved measurements reveal significant transformations in the local chemical and electronic valence-band states, which are consistent with the layer-resolved first-principles theoretical calculations, hence opening the door for future depth-resolved studies of a wide variety of heteroengineered material systems.

Authors:
 [1];  [1];  [2];  [3];  [4];  [1];  [5];  [3];  [3];  [3];  [6];  [2];  [4];  [1]
  1. Temple Univ., Philadelphia, PA (United States)
  2. Northwestern Univ., Evanston, IL (United States)
  3. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
  4. Drexel Univ., Philadelphia, PA (United States)
  5. Paul Scherrer Inst. (PSI), Villigen (Switzerland); National Inst. of Materials Physics (Romania)
  6. Paul Scherrer Inst. (PSI), Villigen (Switzerland)
Publication Date:
Research Org.:
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Materials Sciences & Engineering Division; USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1572846
Alternate Identifier(s):
OSTI ID: 1560775
Grant/Contract Number:  
AC02-05CH11231; SC0012375; AC02-06CH11357; SC0019297
Resource Type:
Accepted Manuscript
Journal Name:
Physical Review B
Additional Journal Information:
Journal Volume: 100; Journal Issue: 12; Journal ID: ISSN 2469-9950
Publisher:
American Physical Society (APS)
Country of Publication:
United States
Language:
English
Subject:
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY

Citation Formats

Yang, W., Chandrasena, R. U., Gu, M., dos Reis, R. M. S., Moon, E. J., Arab, Arian, Husanu, M. -A., Nemšák, S., Gullikson, E. M., Ciston, J., Strocov, V. N., Rondinelli, J. M., May, S. J., and Gray, A. X. Probing single-unit-cell resolved electronic structure modulations in oxide superlattices with standing-wave photoemission. United States: N. p., 2019. Web. doi:10.1103/physrevb.100.125119.
Yang, W., Chandrasena, R. U., Gu, M., dos Reis, R. M. S., Moon, E. J., Arab, Arian, Husanu, M. -A., Nemšák, S., Gullikson, E. M., Ciston, J., Strocov, V. N., Rondinelli, J. M., May, S. J., & Gray, A. X. Probing single-unit-cell resolved electronic structure modulations in oxide superlattices with standing-wave photoemission. United States. doi:10.1103/physrevb.100.125119.
Yang, W., Chandrasena, R. U., Gu, M., dos Reis, R. M. S., Moon, E. J., Arab, Arian, Husanu, M. -A., Nemšák, S., Gullikson, E. M., Ciston, J., Strocov, V. N., Rondinelli, J. M., May, S. J., and Gray, A. X. Mon . "Probing single-unit-cell resolved electronic structure modulations in oxide superlattices with standing-wave photoemission". United States. doi:10.1103/physrevb.100.125119.
@article{osti_1572846,
title = {Probing single-unit-cell resolved electronic structure modulations in oxide superlattices with standing-wave photoemission},
author = {Yang, W. and Chandrasena, R. U. and Gu, M. and dos Reis, R. M. S. and Moon, E. J. and Arab, Arian and Husanu, M. -A. and Nemšák, S. and Gullikson, E. M. and Ciston, J. and Strocov, V. N. and Rondinelli, J. M. and May, S. J. and Gray, A. X.},
abstractNote = {Control of structural coupling at complex-oxide interfaces is a powerful platform for creating ultrathin layers with electronic and magnetic properties unattainable in the bulk. Yet, with the capability to design and control the electronic structure of such buried layers and interfaces at a unit-cell level, a new challenge emerges to be able to probe these engineered emergent phenomena with depth-dependent atomic resolution as well as element- and orbital selectivity. In this work, we utilize a combination of core-level and valence-band soft x-ray standing-wave photoemission spectroscopy, in conjunction with scanning transmission electron microscopy, to probe the depth-dependent and single-unit-cell resolved electronic structure of an isovalent manganite superlattice [Eu0.7Sr0.3MnO3/La0.7Sr0.3MnO3]×15 wherein the electronic-structural properties are intentionally modulated with depth via engineered oxygen octahedra rotations/tilts and A-site displacements. Our unit-cell resolved measurements reveal significant transformations in the local chemical and electronic valence-band states, which are consistent with the layer-resolved first-principles theoretical calculations, hence opening the door for future depth-resolved studies of a wide variety of heteroengineered material systems.},
doi = {10.1103/physrevb.100.125119},
journal = {Physical Review B},
number = 12,
volume = 100,
place = {United States},
year = {2019},
month = {9}
}

Journal Article:
Free Publicly Available Full Text
This content will become publicly available on September 9, 2020
Publisher's Version of Record

Save / Share:

Works referenced in this record:

Commentary: The Materials Project: A materials genome approach to accelerating materials innovation
journal, July 2013

  • Jain, Anubhav; Ong, Shyue Ping; Hautier, Geoffroy
  • APL Materials, Vol. 1, Issue 1
  • DOI: 10.1063/1.4812323

Research Update: Towards designed functionalities in oxide-based electronic materials
journal, August 2015

  • Rondinelli, James M.; Poeppelmeier, Kenneth R.; Zunger, Alex
  • APL Materials, Vol. 3, Issue 8
  • DOI: 10.1063/1.4928289

Towards properties on demand in quantum materials
journal, October 2017

  • Basov, D. N.; Averitt, R. D.; Hsieh, D.
  • Nature Materials, Vol. 16, Issue 11
  • DOI: 10.1038/nmat5017

Inverse design in search of materials with target functionalities
journal, March 2018


Predictions of new AB O 3 perovskite compounds by combining machine learning and density functional theory
journal, April 2018


Enhancement of ferroelectricity at metal–oxide interfaces
journal, April 2009

  • Stengel, Massimiliano; Vanderbilt, David; Spaldin, Nicola A.
  • Nature Materials, Vol. 8, Issue 5
  • DOI: 10.1038/nmat2429

Oxide Interfaces--An Opportunity for Electronics
journal, March 2010


Interface Physics in Complex Oxide Heterostructures
journal, March 2011


Coexistence of magnetic order and two-dimensional superconductivity at LaAlO3/SrTiO3 interfaces
journal, September 2011

  • Li, Lu; Richter, C.; Mannhart, J.
  • Nature Physics, Vol. 7, Issue 10, p. 762-766
  • DOI: 10.1038/nphys2080

Whither the oxide interface
journal, January 2012

  • Chakhalian, J.; Millis, A. J.; Rondinelli, J.
  • Nature Materials, Vol. 11, Issue 2
  • DOI: 10.1038/nmat3225

Emergent phenomena at oxide interfaces
journal, January 2012

  • Hwang, H. Y.; Iwasa, Y.; Kawasaki, M.
  • Nature Materials, Vol. 11, Issue 2
  • DOI: 10.1038/nmat3223

Interfacial Ferromagnetism in LaNiO 3 / CaMnO 3 Superlattices
journal, August 2013


Generalized Gradient Approximation Made Simple
journal, October 1996

  • Perdew, John P.; Burke, Kieron; Ernzerhof, Matthias
  • Physical Review Letters, Vol. 77, Issue 18, p. 3865-3868
  • DOI: 10.1103/PhysRevLett.77.3865

Dynamical mean-field theory of strongly correlated fermion systems and the limit of infinite dimensions
journal, January 1996

  • Georges, Antoine; Kotliar, Gabriel; Krauth, Werner
  • Reviews of Modern Physics, Vol. 68, Issue 1
  • DOI: 10.1103/RevModPhys.68.13

Control of octahedral connectivity in perovskite oxide heterostructures: An emerging route to multifunctional materials discovery
journal, March 2012

  • Rondinelli, James M.; May, Steven J.; Freeland, John W.
  • MRS Bulletin, Vol. 37, Issue 3
  • DOI: 10.1557/mrs.2012.49

Atomically engineered ferroic layers yield a room-temperature magnetoelectric multiferroic
journal, September 2016

  • Mundy, Julia A.; Brooks, Charles M.; Holtz, Megan E.
  • Nature, Vol. 537, Issue 7621
  • DOI: 10.1038/nature19343

Interface-engineered oxygen octahedral coupling in manganite heterostructures
journal, December 2017

  • Huijben, M.; Koster, G.; Liao, Z. L.
  • Applied Physics Reviews, Vol. 4, Issue 4
  • DOI: 10.1063/1.4985770

Spatial control of functional properties via octahedral modulations in complex oxide superlattices
journal, December 2014

  • Moon, E. J.; Colby, R.; Wang, Q.
  • Nature Communications, Vol. 5, Issue 1
  • DOI: 10.1038/ncomms6710

Towards 3D Mapping of BO 6 Octahedron Rotations at Perovskite Heterointerfaces, Unit Cell by Unit Cell
journal, July 2015


Structural “ δ Doping” to Control Local Magnetization in Isovalent Oxide Heterostructures
journal, November 2017


Epitaxial growth and properties of thin film oxides
journal, August 2000


Oxide nano-engineering using MBE
journal, December 2001


Symmetry Lowering in Extreme-Electron-Density Perovskite Quantum Wells
journal, June 2013


Tuning the Structure of Nickelates to Achieve Two-Dimensional Electron Conduction
journal, February 2014

  • Kumah, Divine P.; Disa, Ankit S.; Ngai, Joseph H.
  • Advanced Materials, Vol. 26, Issue 12
  • DOI: 10.1002/adma.201304256

Depth-resolved photoemission spectroscopy with soft X-ray standing waves
journal, March 2001


Momentum-resolved electronic structure at a buried interface from soft X-ray standing-wave angle-resolved photoemission
journal, October 2013


Future directions in standing-wave photoemission
journal, August 2014


Atomic scale imaging of competing polar states in a Ruddlesden–Popper layered oxide
journal, August 2016

  • Stone, Greg; Ophus, Colin; Birol, Turan
  • Nature Communications, Vol. 7, Issue 1
  • DOI: 10.1038/ncomms12572

A fast image simulation algorithm for scanning transmission electron microscopy
journal, May 2017


A streaming multi-GPU implementation of image simulation algorithms for scanning transmission electron microscopy
journal, October 2017

  • Pryor, Alan; Ophus, Colin; Miao, Jianwei
  • Advanced Structural and Chemical Imaging, Vol. 3, Issue 1
  • DOI: 10.1186/s40679-017-0048-z

Efficiency of ab-initio total energy calculations for metals and semiconductors using a plane-wave basis set
journal, July 1996


From ultrasoft pseudopotentials to the projector augmented-wave method
journal, January 1999


Projector augmented-wave method
journal, December 1994


Electron-energy-loss spectra and the structural stability of nickel oxide: An LSDA+U study
journal, January 1998

  • Dudarev, S. L.; Botton, G. A.; Savrasov, S. Y.
  • Physical Review B, Vol. 57, Issue 3, p. 1505-1509
  • DOI: 10.1103/PhysRevB.57.1505

Structural effects on the magnetic and transport properties of perovskite A 1 x A x MnO 3 ( x = 0.25 , 0.30)
journal, October 1997


Suppression of Octahedral Tilts and Associated Changes in Electronic Properties at Epitaxial Oxide Heterostructure Interfaces
journal, August 2010


Control of Structural Distortions in Transition-Metal Oxide Films through Oxygen Displacement at the Heterointerface
journal, April 2014

  • Aso, Ryotaro; Kan, Daisuke; Shimakawa, Yuichi
  • Advanced Functional Materials, Vol. 24, Issue 33
  • DOI: 10.1002/adfm.201303521

Soft-X-ray ARPES facility at the ADRESS beamline of the SLS: concepts, technical realisation and scientific applications
journal, November 2013


Simulation of electron spectra for surface analysis (SESSA): a novel software tool for quantitative Auger-electron spectroscopy and X-ray photoelectron spectroscopy
journal, January 2005

  • Smekal, Werner; Werner, Wolfgang S. M.; Powell, Cedric J.
  • Surface and Interface Analysis, Vol. 37, Issue 11
  • DOI: 10.1002/sia.2097

Calculations of electron inelastic mean free paths. IX. Data for 41 elemental solids over the 50 eV to 30 keV range
journal, February 2011

  • Tanuma, S.; Powell, C. J.; Penn, D. R.
  • Surface and Interface Analysis, Vol. 43, Issue 3
  • DOI: 10.1002/sia.3522

Depth-resolved charge reconstruction at the LaNi O 3 / CaMn O 3 interface
journal, October 2018


Surface-interface coupling in an oxide heterostructure: Impact of adsorbates on LaAlO 3 / SrTiO 3
journal, November 2015


Suppression of Near-Fermi Level Electronic States at the Interface in a LaNiO 3 / SrTiO 3 Superlattice
journal, September 2011


Atomic-resolution chemical imaging of oxygen local bonding environments by electron energy loss spectroscopy
journal, July 2012

  • Mundy, Julia A.; Mao, Qingyun; Brooks, Charles M.
  • Applied Physics Letters, Vol. 101, Issue 4
  • DOI: 10.1063/1.4737208

STEM-EELS imaging of complex oxides and interfaces
journal, January 2012

  • Varela, Maria; Gazquez, Jaume; Pennycook, Stephen J.
  • MRS Bulletin, Vol. 37, Issue 01, p. 29-35
  • DOI: 10.1557/mrs.2011.330