Interface properties and built-in potential profile of a LaCrO3/SrTiO3 superlattice determined by standing-wave excited photoemission spectroscopy

Lin, S. -C.; Kuo, C. -T.; Comes, R. B.; Rault, J. E.; Rueff, J. -P.; Nemšák, S.; Taleb, A.; Kortright, J. B.; Meyer-Ilse, J.; Gullikson, E.; Sushko, P. V.; Spurgeon, S. R.; Gehlmann, M.; Bowden, M. E.; Plucinski, L.; Chambers, S. A.; Fadley, C. S.

doi:10.1103/PhysRevB.98.165124

Interface properties and built-in potential profile of a $LaCr O_{3} / SrTi O_{3}$ superlattice determined by standing-wave excited photoemission spectroscopy

Journal Article · Mon Oct 01 04:00:00 EDT 2018 · Physical Review B

DOI:https://doi.org/10.1103/PhysRevB.98.165124· OSTI ID:1489034

Lin, S. -C.; Kuo, C. -T.; Comes, R. B.; Rault, J. E.; Rueff, J. -P.; Nemšák, S.; Taleb, A.; Kortright, J. B.; Meyer-Ilse, J.; Gullikson, E.; Sushko, P. V.; Spurgeon, S. R.; Gehlmann, M.; Bowden, M. E.; Plucinski, L.; Chambers, S. A.; Fadley, C. S.

LaCrO₃ (LCO) / SrTiO₃ (STO) heterojunctions are intriguing due to a polar discontinuity along (001), two distinct and controllable interface structures [(LaO)⁺/(TiO₂)0 and (SrO)⁰/(CrO₂)^– ], and interface-induced ferroelectricity. In this study, we have used soft- and hard-x-ray standing-wave excited photoemission spectroscopy (SW-XPS) to generate a non-destructive determination of the elemental depth profile of the two interfaces, the layer-resolved valence electronic structure, and the depth distribution of interface-induced built-in potentials in the two constituent oxides. From the determined sample structure, an alternating charged interface configuration is observed: a positive charged 2-Å-thick (LaO)⁺/(TiO₂)⁰ intermediate layer at the LCO_top/STO_bottom interface and a negative charged 2-Å-thick (SrO)⁰/(CrO₂)^– intermediate layer at the STO_top/LCO_bottom interface. SW-XPS also enabled us to deconvolute the LCO-contributed and STO-contributed matrix-element-weighted density of states (MEWDOSs) from the valence band (VB) spectra for the LCO/STO SL. Monitoring the VB edges of the deconvoluted MEWDOS shift with a change in probing profile, the alternating charged-induced built-in potentials are observed in both constituent oxides. Finally, with a two-step simulation, the built-in potentials across the SL are resolved in detail and represented by the depth distribution of VB edges.

Research Organization:: Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)

DOE Contract Number:: AC05-76RL01830

OSTI ID:: 1489034

Report Number(s):: PNNL-SA-131974

Journal Information:: Physical Review B, Journal Name: Physical Review B Journal Issue: 16 Vol. 98; ISSN 2469-9950; ISSN PRBMDO

Publisher:: American Physical Society (APS)

Country of Publication:: United States

Language:: English

References (40)

Some future perspectives in soft- and hard- X-ray photoemission Fadley, Charles S.; Nemšák, Slavomir Journal of Electron Spectroscopy and Related Phenomena, Vol. 195 https://doi.org/10.1016/j.elspec.2014.06.004	journal	August 2014
Energetic, spatial, and momentum character of the electronic structure at a buried interface: The two-dimensional electron gas between two metal oxides Nemšák, S.; Conti, G.; Gray, A. X. Physical Review B, Vol. 93, Issue 24 https://doi.org/10.1103/PhysRevB.93.245103	journal	June 2016
Origin of the light green color and electronic ground state of La Cr O 3 Ong, Khuong P.; Blaha, Peter; Wu, Ping Physical Review B, Vol. 77, Issue 7 https://doi.org/10.1103/PhysRevB.77.073102	journal	February 2008
Ab initio molecular-dynamics simulation of the liquid-metal–amorphous-semiconductor transition in germanium Kresse, G.; Hafner, J. Physical Review B, Vol. 49, Issue 20, p. 14251-14269 https://doi.org/10.1103/PhysRevB.49.14251	journal	May 1994
Precise Determination of the Valence-Band Edge in X-Ray Photoemission Spectra: Application to Measurement of Semiconductor Interface Potentials Kraut, E. A.; Grant, R. W.; Waldrop, J. R. Physical Review Letters, Vol. 44, Issue 24 https://doi.org/10.1103/PhysRevLett.44.1620	journal	June 1980
Band alignment of epitaxial SrTiO3 thin films with (LaAlO3)0.3-(Sr2AlTaO6)0.7 (001) Comes, Ryan B.; Xu, Peng; Jalan, Bharat Applied Physics Letters, Vol. 107, Issue 13 https://doi.org/10.1063/1.4932063	journal	September 2015
Suppression of Near-Fermi Level Electronic States at the Interface in a LaNiO 3 / SrTiO 3 Superlattice Kaiser, A. M.; Gray, A. X.; Conti, G. Physical Review Letters, Vol. 107, Issue 11 https://doi.org/10.1103/PhysRevLett.107.116402	journal	September 2011
Electronic structure of AlFeN films exhibiting crystallographic orientation change from c- to a-axis with Fe concentrations and annealing effect Tatemizo, Nobuyuki; Imada, Saki; Okahara, Kizuna Scientific Reports, Vol. 10, Issue 1 https://doi.org/10.1038/s41598-020-58835-5	journal	February 2020
Surface-interface coupling in an oxide heterostructure: Impact of adsorbates on LaAlO 3 / SrTiO 3 Scheiderer, P.; Pfaff, F.; Gabel, J. Physical Review B, Vol. 92, Issue 19 https://doi.org/10.1103/PhysRevB.92.195422	journal	November 2015
Multiband Optical Absorption Controlled by Lattice Strain in Thin-Film LaCrO 3 Sushko, Peter V.; Qiao, Liang; Bowden, Mark Physical Review Letters, Vol. 110, Issue 7 https://doi.org/10.1103/PhysRevLett.110.077401	journal	February 2013
Charge transfer and interfacial magnetism in (LaNiO 3 ) n /(LaMnO 3 ) 2 superlattices Hoffman, J.; Tung, I. C.; Nelson-Cheeseman, B. B. Physical Review B, Vol. 88, Issue 14 https://doi.org/10.1103/PhysRevB.88.144411	journal	October 2013
The multicomponent structure of the 4d orbital in X-ray photoelectron spectra of the lanthanum(III) ion Howng, Wei-Yean; Thorn, R. J. Chemical Physics Letters, Vol. 56, Issue 3 https://doi.org/10.1016/0009-2614(78)89016-2	journal	June 1978
Impact of built-in potential across LaFeO3/SrTiO3 heterojunctions on photocatalytic activity Nakamura, Kentarou; Mashiko, Hisanori; Yoshimatsu, Kohei Applied Physics Letters, Vol. 108, Issue 21 https://doi.org/10.1063/1.4952736	journal	May 2016
Projector augmented-wave method Blöchl, P. E. Physical Review B, Vol. 50, Issue 24, p. 17953-17979 https://doi.org/10.1103/PhysRevB.50.17953	journal	December 1994
Determination of layer-resolved composition, magnetization, and electronic structure of an Fe/MgO tunnel junction by standing-wave core and valence photoemission Yang, See-Hun; Balke, Benjamin; Papp, Christian Physical Review B, Vol. 84, Issue 18 https://doi.org/10.1103/PhysRevB.84.184410	journal	November 2011
Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set Kresse, G.; Furthmüller, J. Physical Review B, Vol. 54, Issue 16, p. 11169-11186 https://doi.org/10.1103/PhysRevB.54.11169	journal	October 1996
Interface Structure, Band Alignment, and Built-In Potentials at LaFeO 3 / n − SrTiO 3 Heterojunctions Comes, Ryan; Chambers, Scott Physical Review Letters, Vol. 117, Issue 22 https://doi.org/10.1103/PhysRevLett.117.226802	journal	November 2016
Making use of x-ray optical effects in photoelectron-, Auger electron-, and x-ray emission spectroscopies: Total reflection, standing-wave excitation, and resonant effects Yang, S. -H.; Gray, A. X.; Kaiser, A. M. Journal of Applied Physics, Vol. 113, Issue 7 https://doi.org/10.1063/1.4790171	journal	February 2013
Restoring the Density-Gradient Expansion for Exchange in Solids and Surfaces Perdew, John P.; Ruzsinszky, Adrienn; Csonka, Gábor I. Physical Review Letters, Vol. 100, Issue 13 https://doi.org/10.1103/PhysRevLett.100.136406	journal	April 2008
Observation of polar vortices in oxide superlattices Yadav, A. K.; Nelson, C. T.; Hsu, S. L. Nature, Vol. 530, Issue 7589 https://doi.org/10.1038/nature16463	journal	January 2016
Interface properties of magnetic tunnel junction La 0.7 Sr 0.3 MnO 3 / SrTiO 3 superlattices studied by standing-wave excited photoemission spectroscopy Gray, A. X.; Papp, C.; Balke, B. Physical Review B, Vol. 82, Issue 20 https://doi.org/10.1103/PhysRevB.82.205116	journal	November 2010
Two-Dimensional Electron Gases at Complex Oxide Interfaces Stemmer, Susanne; James Allen, S. Annual Review of Materials Research, Vol. 44, Issue 1 https://doi.org/10.1146/annurev-matsci-070813-113552	journal	July 2014
Probing the Origin of Interfacial Carriers in SrTiO ₃ –LaCrO ₃ Superlattices Comes, Ryan B.; Spurgeon, Steven R.; Kepaptsoglou, Despoina M. Chemistry of Materials, Vol. 29, Issue 3 https://doi.org/10.1021/acs.chemmater.6b04329	journal	January 2017
Concentration and chemical-state profiles at heterogeneous interfaces with sub-nm accuracy from standing-wave ambient-pressure photoemission Nemšák, Slavomír; Shavorskiy, Andrey; Karslioglu, Osman Nature Communications, Vol. 5, Issue 1 https://doi.org/10.1038/ncomms6441	journal	November 2014
Interface-Induced Polarization in SrTiO ₃ -LaCrO ₃ Superlattices Comes, Ryan B.; Spurgeon, Steven R.; Heald, Steve M. Advanced Materials Interfaces, Vol. 3, Issue 10 https://doi.org/10.1002/admi.201500779	journal	February 2016
X-ray standing-wave investigations of valence electronic structure Woicik, J. C.; Nelson, E. J.; Heskett, D. Physical Review B, Vol. 64, Issue 12 https://doi.org/10.1103/PhysRevB.64.125115	journal	September 2001
Direct Measurement of Valence-Charge Asymmetry by X-Ray Standing Waves Woicik, J. C.; Nelson, E. J.; Pianetta, P. Physical Review Letters, Vol. 84, Issue 4 https://doi.org/10.1103/PhysRevLett.84.773	journal	January 2000
Band Alignment, Built-In Potential, and the Absence of Conductivity at the LaCrO 3 / SrTiO 3 ( 001 ) Heterojunction Chambers, S. A.; Qiao, L.; Droubay, T. C. Physical Review Letters, Vol. 107, Issue 20 https://doi.org/10.1103/PhysRevLett.107.206802	journal	November 2011
Spontaneous Polarization and Bulk Photovoltaic Effect Driven by Polar Discontinuity in LaFeO 3 / SrTiO 3 Heterojunctions Nakamura, M.; Kagawa, F.; Tanigaki, T. Physical Review Letters, Vol. 116, Issue 15 https://doi.org/10.1103/PhysRevLett.116.156801	journal	April 2016
Electron-energy-loss spectra and the structural stability of nickel oxide: An LSDA+U study Dudarev, S. L.; Botton, G. A.; Savrasov, S. Y. Physical Review B, Vol. 57, Issue 3, p. 1505-1509 https://doi.org/10.1103/PhysRevB.57.1505	journal	January 1998
Resonant photoemission of La and Yb at the 3d absorption edge Lagarde, P.; Flank, A. -M.; Ogasawara, H. Journal of Electron Spectroscopy and Related Phenomena, Vol. 128, Issue 2-3 https://doi.org/10.1016/S0368-2048(02)00283-9	journal	February 2003
Band-Gap Reduction and Dopant Interaction in Epitaxial La,Cr Co-doped SrTiO ₃ Thin Films Comes, Ryan B.; Sushko, Peter V.; Heald, Steve M. Chemistry of Materials, Vol. 26, Issue 24 https://doi.org/10.1021/cm503541u	journal	December 2014
RHEED Intensity Oscillations for the Stoichiometric Growth of SrTiO₃ Thin Films by Reactive Molecular Beam Epitaxy Haeni, J. H.; Theis, C. D.; Schlom, D. G. Journal of Electroceramics, Vol. 4, Issue 2/3, p. 385-391 https://doi.org/10.1023/A:1009947517710	journal	January 2000
Atomically engineered ferroic layers yield a room-temperature magnetoelectric multiferroic Mundy, Julia A.; Brooks, Charles M.; Holtz, Megan E. Nature, Vol. 537, Issue 7621 https://doi.org/10.1038/nature19343	journal	September 2016
Voltage- and time-dependent valence state transition in cobalt oxide catalysts during the oxygen evolution reaction Zhou, Jing; Zhang, Linjuan; Huang, Yu-Cheng Nature Communications, Vol. 11, Issue 1 https://doi.org/10.1038/s41467-020-15925-2	journal	April 2020
Theoretical study of Schottky-barrier formation at epitaxial rare-earth-metal/semiconductor interfaces Delaney, Kris T.; Spaldin, Nicola A.; Van de Walle, Chris G. Physical Review B, Vol. 81, Issue 16 https://doi.org/10.1103/PhysRevB.81.165312	journal	April 2010
Dynamic interface rearrangement in LaFeO 3 / n − SrTiO 3 heterojunctions Spurgeon, Steven R.; Sushko, Peter V.; Chambers, Scott A. Physical Review Materials, Vol. 1, Issue 6 https://doi.org/10.1103/PhysRevMaterials.1.063401	journal	November 2017
Interface-induced Polarization in SrTiO$_3$-LaCrO$_3$ Superlattices Comes, Ryan B.; Spurgeon, Steven R.; Heald, Steve M. arXiv https://doi.org/10.48550/arxiv.1604.02434	text	January 2016
Ultralow Contact Resistance at an Epitaxial Metal/Oxide Heterojunction Through Interstitial Site Doping Chambers, Scott A.; Gu, Meng; Sushko, Peter V. Advanced Materials, Vol. 25, Issue 29 https://doi.org/10.1002/adma.201301030	journal	May 2013
Atomic subshell photoionization cross sections and asymmetry parameters: 1 ⩽ Z ⩽ 103 Yeh, J. J.; Lindau, I. Atomic Data and Nuclear Data Tables, Vol. 32, Issue 1 https://doi.org/10.1016/0092-640X(85)90016-6	journal	January 1985

Cited By (2)

Probing energy landscapes in multilayer heterostructures: Challenges and opportunities Chambers, Scott A.; Sushko, Peter V. APL Materials, Vol. 7, Issue 11 https://doi.org/10.1063/1.5129155	journal	November 2019
Polarization-dependent electric potential distribution across nanoscale ferroelectric Hf _0.5 Zr _0.5 O ₂ in functional memory capacitors Matveyev, Yury; Mikheev, Vitalii; Negrov, Dmitry Nanoscale, Vol. 11, Issue 42 https://doi.org/10.1039/c9nr05904k	journal	January 2019

Similar Records

Interface properties and built-in potential profile of a

LaCr O_{3} / SrTi O_{3}

superlattice determined by standing-wave excited photoemission spectroscopy

Journal Article · Sun Oct 14 20:00:00 EDT 2018 · Physical Review B · OSTI ID:1563966

Dynamic interface rearrangement in

{LaFeO}_{3} / n - {SrTiO}_{3}

heterojunctions

Journal Article · Sun Nov 05 19:00:00 EST 2017 · Physical Review Materials · OSTI ID:1430717

Stoichiometry dependence of potential screening at

La_{(1 - δ)} Al_{(1 + δ)} O_{3} / SrTiO_{3}

interfaces

Journal Article · Thu Apr 02 20:00:00 EDT 2015 · Physical Review. B, Condensed Matter and Materials Physics · OSTI ID:1177475

Related Subjects

metal-oxide heterostructure
standing-wave excited photoemission spectroscopy
STEM-EELS composition map
built-in potential