- Letter
- Open Access
Orbital engineering in superlattices
Phys. Rev. B 104, L121102 – Published 1 September, 2021
DOI: https://doi.org/10.1103/PhysRevB.104.L121102
Abstract
Oxide heterostructures provide unique opportunities to modify the properties of quantum materials through a targeted manipulation of spin, charge, and orbital states. Here, we use resonant x-ray reflectometry to probe the electronic structure of thin slabs of embedded in a superlattice with . We extend the previously established methods of reflectometry analysis to a general form applicable to electron systems and extract quantitative depth-dependent x-ray linear dichroism profiles. Our data reveal an artificial, layered orbital polarization, where the average occupation of and orbitals in the interface planes next to is inverted compared to the central part of the slab. This phase is stable down to 30 K and the bulklike orbital ordering transitions are absent. We identify the key mechanism for the electronic reconstruction to be a combination of epitaxial strain and spatial confinement by the layers, in good agreement with predictions from ab initio theory.
Physics Subject Headings (PhySH)
- Electronic structure
- First-principles calculations
- Heterostructures
- Interfaces
- Mott insulators
- Multilayer thin films
- Strongly correlated systems
- Density functional calculations
- Resonant elastic x-ray scattering
- Scanning transmission electron microscopy
- X-ray absorption fine structure spectroscopy
- X-ray reflectivity
Article Text
Supplemental Material
References (54)
- J. Kanamori, J. Phys. Chem. Solids 10, 87 (1959).
- J. B. Goodenough, Phys. Rev. 100, 564 (1955).
- D. Gotfryd, E. M. Pärschke, J. Chaloupka, A. M. Oleś, and K. Wohlfeld, Phys. Rev. Research 2, 013353 (2020).
- V. Baltz, A. Manchon, M. Tsoi, T. Moriyama, T. Ono, and Y. Tserkovnyak, Rev. Mod. Phys. 90, 015005 (2018).
- M. Bibes and A. Barthelemy, IEEE Trans. Electron Devices 54, 1003 (2007).
- E. Assmann, P. Blaha, R. Laskowski, K. Held, S. Okamoto, and G. Sangiovanni, Phys. Rev. Lett. 110, 078701 (2013).
- S. Miyasaka, Y. Okimoto, M. Iwama, and Y. Tokura, Phys. Rev. B 68, 100406(R) (2003).
- G. R. Blake, T. T. M. Palstra, Y. Ren, A. A. Nugroho, and A. A. Menovsky, Phys. Rev. Lett. 87, 245501 (2001).
- Y. Ren, T. Palstra, D. Khomskii, E. Pellegrin, A. A. Nugroho, A. A. Menovsky, and G. A. Sawatzky, Nature (London) 396, 441 (1998).
- G. Khaliullin, P. Horsch, and A. M. Oleś, Phys. Rev. Lett. 86, 3879 (2001).
- S. Ishihara, Phys. Rev. B 69, 075118 (2004).
- D. J. Lovinger, M. Brahlek, P. Kissin, D. M. Kennes, A. J. Millis, R. Engel-Herbert, and R. D. Averitt, Phys. Rev. B 102, 115143 (2020).
- S. Miyasaka, J. Fujioka, M. Iwama, Y. Okimoto, and Y. Tokura, Phys. Rev. B 73, 224436 (2006).
- S. Sugai and K. Hirota, Phys. Rev. B 73, 020409(R) (2006).
- C. Ulrich, G. Khaliullin, J. Sirker, M. Reehuis, M. Ohl, S. Miyasaka, Y. Tokura, and B. Keimer, Phys. Rev. Lett. 91, 257202 (2003).
- E. Benckiser, R. Rückamp, T. Möller, T. Taetz, A. Möller, A. A. Nugroho, T. T. M. Palstra, G. S. Uhrig, and M. Grüninger, New J. Phys. 10, 053027 (2008).
- E. Benckiser, L. Fels, G. Ghiringhelli, M. Moretti Sala, T. Schmitt, J. Schlappa, V. N. Strocov, N. Mufti, G. R. Blake, A. A. Nugroho, T. T. M. Palstra, M. W. Haverkort, K. Wohlfeld, and M. Grüninger, Phys. Rev. B 88, 205115 (2013).
- M. Brahlek, L. Zhang, J. Lapano, H.-T. Zhang, R. Engel-Herbert, N. Shukla, S. Datta, H. Paik, and D. G. Schlom, MRS Commun. 7, 27 (2017).
- A. David, R. Frésard, P. Boullay, W. Prellier, U. Lüders, and P.-E. Janolin, Appl. Phys. Lett. 98, 212106 (2011).
- H. Rotella, O. Copie, A. Pautrat, P. Boullay, A. David, D. Pelloquin, C. Labbé, C. Frilay, and W. Prellier, J. Phys.: Condens. Matter 27, 095603 (2015).
- D. Kumar, A. David, A. Fouchet, A. Pautrat, J. Varignon, C. U. Jung, U. Lüders, B. Domengès, O. Copie, P. Ghosez, and W. Prellier, Phys. Rev. B 99, 224405 (2019).
- G. Fabbris, D. Meyers, J. Okamoto, J. Pelliciari, A. S. Disa, Y. Huang, Z.-Y. Chen, W. B. Wu, C. T. Chen, S. Ismail-Beigi, C. H. Ahn, F. J. Walker, D. J. Huang, T. Schmitt, and M. P. M. Dean, Phys. Rev. Lett. 117, 147401 (2016).
- M. Wu, E. Benckiser, M. W. Haverkort, A. Frano, Y. Lu, U. Nwankwo, S. Brück, P. Audehm, E. Goering, S. Macke, V. Hinkov, P. Wochner, G. Christiani, S. Heinze, G. Logvenov, H.-U. Habermeier, and B. Keimer, Phys. Rev. B 88, 125124 (2013).
- F. Wrobel, B. Geisler, Y. Wang, G. Christiani, G. Logvenov, M. Bluschke, E. Schierle, P. A. van Aken, B. Keimer, R. Pentcheva, and E. Benckiser, Phys. Rev. Materials 2, 035001 (2018).
- P. Chen, Z. Huang, M. Li, X. Yu, X. Wu, C. Li, N. Bao, S. Zeng, P. Yang, L. Qu, J. Chen, J. Ding, S. J. Pennycook, W. Wu, T. V. Venkatesan, A. Ariando, and G. M. Chow, Adv. Funct. Mater. 30, 1909536 (2020).
- B. Geisler and R. Pentcheva, Phys. Rev. Applied 11, 044047 (2019).
- D. Doennig, W. E. Pickett, and R. Pentcheva, Phys. Rev. B 89, 121110(R) (2014).
- B. Geisler and R. Pentcheva, Phys. Rev. B 102, 020502(R) (2020).
- Ş. Smadici, P. Abbamonte, A. Bhattacharya, X. Zhai, B. Jiang, A. Rusydi, J. N. Eckstein, S. D. Bader, and J.-M. Zuo, Phys. Rev. Lett. 99, 196404 (2007).
- J. Park, B.-G. Cho, K. D. Kim, J. Koo, H. Jang, K.-T. Ko, J.-H. Park, K.-B. Lee, J.-Y. Kim, D. R. Lee, C. A. Burns, S. S. A. Seo, and H. N. Lee, Phys. Rev. Lett. 110, 017401 (2013).
- H. Wadati, D. G. Hawthorn, J. Geck, T. Higuchi, Y. Hikita, H. Y. Hwang, L. F. Kourkoutis, D. A. Muller, S.-W. Huang, D. J. Huang, H.-J. Lin, C. Schüßler-Langeheine, H.-H. Wu, E. Schierle, E. Weschke, N. J. C. Ingle, and G. A. Sawatzky, J. Appl. Phys. 106, 083705 (2009).
- E. Benckiser, M. W. Haverkort, S. Brück, E. Goering, S. Macke, A. Frano, X. Yang, O. K. Andersen, G. Cristiani, H. U. Habermeier, A. V. Boris, I. Zegkinoglou, P. Wochner, H. J. Kim, V. Hinkov, and B. Keimer, Nat. Mater. 10, 189 (2011).
- M. Wu, E. Benckiser, P. Audehm, E. Goering, P. Wochner, G. Christiani, G. Logvenov, H.-U. Habermeier, and B. Keimer, Phys. Rev. B 91, 195130 (2015).
- S. Macke, A. Radi, J. E. Hamann-Borrero, A. Verna, M. Bluschke, S. Brück, E. Goering, R. Sutarto, F. He, G. Cristiani, M. Wu, E. Benckiser, H.-U. Habermeier, G. Logvenov, N. Gauquelin, G. A. Botton, A. P. Kajdos, S. Stemmer, G. A. Sawatzky, M. W. Haverkort, Adv. Mater. 26, 6554 (2014).
- See Supplemental Material at http://link.aps.org/supplemental/10.1103/PhysRevB.104.L121102 for further details of XRD used to verify the structure of inside the SL, the description of scattering factor models, uniqueness of XLD profiles, and sensitivity of x-ray reflectometry, which includes Refs. [50, 51, 52, 53, 54].
- S. Brück, S. Bauknecht, B. Ludescher, E. Goering, and G. Schütz, Rev. Sci. Instrum. 79, 083109 (2008).
- M. W. Haverkort, M. Zwierzycki, and O. K. Andersen, Phys. Rev. B 85, 165113 (2012).
- Y. Lu, M. Höppner, O. Gunnarsson, and M. W. Haverkort, Phys. Rev. B 90, 085102 (2014).
- M. W. Haverkort, G. Sangiovanni, P. Hansmann, A. Toschi, Y. Lu, and S. Macke, Europhys. Lett. 108, 57004 (2014).
- W. Kohn and L. J. Sham, Phys. Rev. 140, A1133 (1965).
- P. Giannozzi, S. Baroni, N. Bonini, M. Calandra, R. Car, C. Cavazzoni, D. Ceresoli, G. L. Chiarotti, M. Cococcioni, I. Dabo, A. Dal Corso, S. de Gironcoli, S. Fabris, G. Fratesi, R. Gebauer, U. Gerstmann, C. Gougoussis, A. Kokalj, M. Lazzeri, L. Martin-Samos et al., J. Phys.: Condens. Matter 21, 395502 (2009).
- J. P. Perdew, K. Burke, and M. Ernzerhof, Phys. Rev. Lett. 77, 3865 (1996).
- M. Cococcioni and S. de Gironcoli, Phys. Rev. B 71, 035105 (2005).
- L. F. Kourkoutis, Y. Hotta, T. Susaki, H. Y. Hwang, and D. A. Muller, Phys. Rev. Lett. 97, 256803 (2006).
- M. Kasuya, Y. Tokura, T. Arima, H. Eisaki, and S. Uchida, Phys. Rev. B 47, 6197 (1993).
- N. Hollmann, Ph.D. thesis, University of Cologne, 2010.
- Since and are proportional to and , respectively, where refers to the holes residing in a given orbital [48, 49].
- B. T. Thole, P. Carra, F. Sette, and G. van der Laan, Phys. Rev. Lett. 68, 1943 (1992).
- P. Carra, H. König, B. Thole, and M. Altarelli, Phys. B: Condens. Matter 192, 182 (1993).
- A. Vailionis, H. Boschker, W. Siemons, E. P. Houwman, D. H. A. Blank, G. Rijnders, and G. Koster, Phys. Rev. B 83, 064101 (2011).
- C. T. Chantler, J. Phys. Chem. Ref. Data 29, 597 (2000).
- R. Nakajima, J. Stöhr, and Y. U. Idzerda, Phys. Rev. B 59, 6421 (1999).
- A. Ruosi, C. Raisch, A. Verna, R. Werner, B. A. Davidson, J. Fujii, R. Kleiner, and D. Koelle, Phys. Rev. B 90, 125120 (2014).
- J. Hwang, J. Son, J. Y. Zhang, A. Janotti, C. G. Van de Walle, and S. Stemmer, Phys. Rev. B 87, 060101(R) (2013).