Orbital Ordering of the Mobile and Localized Electrons at Oxygen-Deficient LaAlO3/SrTiO3 If Interfaces

被引:37
作者
Chikina, Alla [1 ]
Lechermann, Frank [2 ]
Husanu, Marius-Adrian [1 ,3 ]
Caputo, Marco [1 ]
Cancellieri, Claudia [1 ,4 ]
Wang, Xiaoqiang [1 ]
Schmitt, Thorsten [1 ]
Radovic, Milan [1 ]
Strocov, Vladimir N. [1 ]
机构
[1] Paul Scherrer Inst, Swiss Light Source, CH-5232 Villigen, Switzerland
[2] Univ Hamburg, Inst Theoret Phys, Jungiusstr 9, DE-20355 Hamburg, Germany
[3] Natl Inst Mat Phys, Atomistilor 405A, RO-077125 Magurele, Romania
[4] Empa, Swiss Fed Labs Mat Sci & Technol, Ueberlandstr 129, CH-8600 Dubendorf, Switzerland
基金
瑞士国家科学基金会;
关键词
LaAlO3/SrTiO3; interface; oxide interfaces; resonant photoemission; two-dimensional electron gas; oxygen vacancies; RESOLVED RESONANT PHOTOEMISSION; BEAMLINE; ADRESS; SOLVER; GAS;
D O I
10.1021/acsnano.8b02335
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
Interfacing different transition-metal oxides opens a route to functionalizing their rich interplay of electron, spin, orbital, and lattice degrees of freedom for electronic and spintronic devices. Electronic and magnetic properties of SrTiO3-based interfaces hosting a mobile two-dimensional electron system (2DES) are strongly influenced by oxygen vacancies, which form an electronic dichotomy, where strongly correlated localized electrons in the in-gap states (IGSs) coexist with noncorrelated delocalized 2DES. Here, we use resonant soft-X-ray photoelectron spectroscopy to prove the e(g) character of the IGSs, as opposed to the t(2g) character of the 2DES in the paradigmatic LaAlO3/SrTiO3 interface. We furthermore separate the d(xy) and d(xz)/d(xz) orbital contributions based on deeper consideration of the resonant photoexcitation process in terms of orbital and momentum selectivity. Supported by a self-consistent combination of density functional theory and dynamical mean field theory calculations, this experiment identifies local orbital reconstruction that goes beyond the conventional e(g)-vs-t(2g) band ordering. A hallmark of oxygen-deficient LaAlO3/SrTiO3 is a significant hybridization of the e(g) and t(2g) orbitals. Our findings provide routes for tuning the electronic and magnetic properties of oxide interfaces through "defect engineering" with oxygen vacancies.
引用
收藏
页码:7927 / 7935
页数:9
相关论文
共 53 条
[1]   Electronic phase separation at the LaAlO3/SrTiO3 interface [J].
Ariando ;
Wang, X. ;
Baskaran, G. ;
Liu, Z. Q. ;
Huijben, J. ;
Yi, J. B. ;
Annadi, A. ;
Barman, A. Roy ;
Rusydi, A. ;
Dhar, S. ;
Feng, Y. P. ;
Ding, J. ;
Hilgenkamp, H. ;
Venkatesan, T. .
NATURE COMMUNICATIONS, 2011, 2
[2]   Hubbard band versus oxygen vacancy states in the correlated electron metal SrVO3 [J].
Backes, S. ;
Rodel, T. C. ;
Fortuna, F. ;
Frantzeskakis, E. ;
Le Fevre, P. ;
Bertran, F. ;
Kobayashi, M. ;
Yukawa, R. ;
Mitsuhashi, T. ;
Kitamura, M. ;
Horiba, K. ;
Kumigashira, H. ;
Saint-Martin, R. ;
Fouchet, A. ;
Berini, B. ;
Dumont, Y. ;
Kim, A. J. ;
Lechermann, F. ;
Jeschke, H. O. ;
Rozenberg, M. J. ;
Valenti, R. ;
Santander-Syro, A. F. .
PHYSICAL REVIEW B, 2016, 94 (24)
[3]   Interface exchange processes in LaAlO3/SrTiO3 induced by oxygen vacancies [J].
Behrmann, Malte ;
Lechermann, Frank .
PHYSICAL REVIEW B, 2015, 92 (12)
[4]   Direct k-Space Mapping of the Electronic Structure in an Oxide-Oxide Interface [J].
Berner, G. ;
Sing, M. ;
Fujiwara, H. ;
Yasui, A. ;
Saitoh, Y. ;
Yamasaki, A. ;
Nishitani, Y. ;
Sekiyama, A. ;
Pavlenko, N. ;
Kopp, T. ;
Richter, C. ;
Mannhart, J. ;
Suga, S. ;
Claessen, R. .
PHYSICAL REVIEW LETTERS, 2013, 110 (24)
[5]   Magnetic effects at the interface between non-magnetic oxides [J].
Brinkman, A. ;
Huijben, M. ;
Van Zalk, M. ;
Huijben, J. ;
Zeitler, U. ;
Maan, J. C. ;
Van der Wiel, W. G. ;
Rijnders, G. ;
Blank, D. H. A. ;
Hilgenkamp, H. .
NATURE MATERIALS, 2007, 6 (07) :493-496
[6]   Polaronic metal state at the LaAlO3/SrTiO3 interface [J].
Cancellieri, C. ;
Mishchenko, A. S. ;
Aschauer, U. ;
Filippetti, A. ;
Faber, C. ;
Barisic, O. S. ;
Rogalev, V. A. ;
Schmitt, T. ;
Nagaosa, N. ;
Strocov, V. N. .
NATURE COMMUNICATIONS, 2016, 7
[7]   Doping-dependent band structure of LaAlO3/SrTiO3 interfaces by soft x-ray polarization-controlled resonant angle-resolved photoemission [J].
Cancellieri, C. ;
Reinle-Schmitt, M. L. ;
Kobayashi, M. ;
Strocov, V. N. ;
Willmott, P. R. ;
Fontaine, D. ;
Ghosez, Ph ;
Filippetti, A. ;
Delugas, P. ;
Fiorentini, V. .
PHYSICAL REVIEW B, 2014, 89 (12)
[8]   Anomalous orbital structure in a spinel-perovskite interface [J].
Cao, Yanwei ;
Liu, Xiaoran ;
Shafer, Padraic ;
Middey, Srimanta ;
Meyers, Derek ;
Kareev, Mikhail ;
Zhong, Zhicheng ;
Kim, Jong-Woo ;
Ryan, Philip J. ;
Arenholz, Elke ;
Chakhalian, Jak .
NPJ QUANTUM MATERIALS, 2016, 1
[9]   Observation of a two-dimensional liquid of Frohlich polarons at the bare SrTiO3 surface [J].
Chen, Chaoyu ;
Avila, Jose ;
Frantzeskakis, Emmanouil ;
Levy, Anna ;
Asensio, Maria C. .
NATURE COMMUNICATIONS, 2015, 6
[10]   Spontaneous 2-Dimensional Carrier Confinement at the n-Type SrTiO3/LaAlO3 Interface [J].
Delugas, Pietro ;
Filippetti, Alessio ;
Fiorentini, Vincenzo ;
Bilc, Daniel I. ;
Fontaine, Denis ;
Ghosez, Philippe .
PHYSICAL REVIEW LETTERS, 2011, 106 (16)