Anionic substitution; Density-functional-theory; Energy efficient; Ferroelectric order; Ferroics; Magnetic orders; Multiferroics; Oxynitrides; Strong correlation; Thin-films; Chemistry (all); Materials Science (all); Condensed Matter Physics; Physics - Materials Science; Physics - Other; Electrochemistry; Biomaterials; Electronic, Optical and Magnetic Materials
Abstract :
[en] Multiferroics are a unique class of materials where magnetic and ferroelectric orders coexist. The research on multiferroics contributes significantly to the fundamental understanding of the strong correlations between different material degrees of freedom and provides an energy-efficient route toward the electrical control of magnetism. While multiple ABO3 oxide perovskites are identified as being multiferroic, their magnetoelectric coupling strength is often weak, necessitating the material search in different compounds. Here, the observation of room-temperature multiferroic orders in multi-anion SrNbO3−xNx thin films is reported. In these samples, the multi-anion state enables the room-temperature ferromagnetic ordering of the Nb d-electrons. Simultaneously, ferroelectric responses that originate from the structural symmetry breaking associated are found with both the off-center displacements of Nb and the geometric displacements of Sr, depending on the relative O-N arrangements within the Nb-centered octahedra. The findings not only diversify the available multiferroic material pool but also demonstrate a new multiferroism design strategy via multi-anion engineering.
Disciplines :
Physics
Author, co-author :
Garcia-Castro, Andres Camilo ; School of Physics, Universidad Industrial de Santander, Bucaramanga, Colombia
Ma, Yanjun; Department of Physics and Astronomy, West Virginia University, Morgantown, United States
Romestan, Zachary; Department of Physics and Astronomy, West Virginia University, Morgantown, United States
Bousquet, Eric ; Université de Liège - ULiège > Département de physique
Cen, Cheng ; Department of Physics and Astronomy, West Virginia University, Morgantown, United States
Romero, Aldo ; Université de Liège - ULiège > Département de physique > Physique des matériaux et nanostructures ; Department of Physics and Astronomy, West Virginia University, Morgantown, United States
Language :
English
Title :
Engineering of Ferroic Orders in Thin Films by Anionic Substitution
A.C.G.‐C. and Y.M., contributed equally to this work. This work has been supported by the grants NSF SI2‐SSE 1740112, DMREF‐NSF 1434897, DOE DE‐SC0016176 and DE‐SC0019491. The theoretical results were obtained thanks to the XSEDE facilities which are supported by the National Science Foundation under grant number ACI‐1053575. The authors also acknowledge the support from the Texas Advances Computer Center (with the Stampede2 and Bridges supercomputers), the OFFSPRING PRACE project (using the DECI resource BEM based in Poland at Wrocław) and on the CECI facilities funded by F.R.S‐FNRS (Grant No. 2.5020.1) and Tier‐1 supercomputer of the Fédération Wallonie‐Bruxelles funded by the Walloon Region (Grant No. 1117545). A.C.G.‐C. acknowledge the grant No. 2489 entitled “Investigación y predicción de propiedades ferroeléctricas, magnéticas y magnetoeléctricas de oxinitruros tipo Sr(Nb,Ta)ON” and the grant No. 2677 entitled “‘Quiralidad y Ordenamiento Magnético en Sistemas Cristalinos: Estudio Teórico desde Primeros Principios”’ both supported by the VIE – UIS. Also, the authors thank the support from the GridUIS‐2 experimental testbed, developed under the Universidad Industrial de Santander (SC3‐UIS) High Performance and Scientific Computing Centre, with support from UIS Vicerrectoría de Investigación y Extensión (VIE‐UIS) and several UIS research groups as well as other funding resources. 3− x xA.C.G.-C. and Y.M., contributed equally to this work. This work has been supported by the grants NSF SI2-SSE 1740112, DMREF-NSF 1434897, DOE DE-SC0016176 and DE-SC0019491. The theoretical results were obtained thanks to the XSEDE facilities which are supported by the National Science Foundation under grant number ACI-1053575. The authors also acknowledge the support from the Texas Advances Computer Center (with the Stampede2 and Bridges supercomputers), the OFFSPRING PRACE project (using the DECI resource BEM based in Poland at Wroc?aw) and on the CECI facilities funded by F.R.S-FNRS (Grant No. 2.5020.1) and Tier-1 supercomputer of the F?d?ration Wallonie-Bruxelles funded by the Walloon Region (Grant No. 1117545). A.C.G.-C. acknowledge the grant No. 2489 entitled ?Investigaci?n y predicci?n de propiedades ferroel?ctricas, magn?ticas y magnetoel?ctricas de oxinitruros tipo Sr(Nb,Ta)O3?xNx? and the grant No. 2677 entitled ??Quiralidad y Ordenamiento Magn?tico en Sistemas Cristalinos: Estudio Te?rico desde Primeros Principios?? both supported by the VIE ? UIS. Also, the authors thank the support from the GridUIS-2 experimental testbed, developed under the Universidad Industrial de Santander (SC3-UIS) High Performance and Scientific Computing Centre, with support from UIS Vicerrector?a de Investigaci?n y Extensi?n (VIE-UIS) and several UIS research groups as well as other funding resources.
R. Ramesh, L. W. Martin, La Rivista del Nuovo Cimento 2021, 44, 251.
N. A. Hill, J. Phys. Chem. B 2000, 104, 6694.
Y. Zhang, J. Wang, P. Ghosez, Phys. Rev. Lett. 2020, 125, 157601.
N. A. Benedek, C. J. Fennie, Phys. Rev. Lett. 2011, 106, 107204.
A. C. Garcia-Castro, W. Ibarra-Hernandez, E. Bousquet, A. H. Romero, Phys. Rev. Lett. 2018, 121, 117601.
M. J. Pitcher, P. Mandal, M. S. Dyer, J. Alaria, P. Borisov, H. Niu, J. B. Claridge, M. J. Rosseinsky, Science 2015, 347, 420.
R. Ramesh, N. A. Spaldin, Nat. Mater. 2007, 6, 21.
M. Fiebig, T. Lottermoser, D. Meier, M. Trassin, Nat. Rev. Mater. 2016, 1, 16046.
N. A. Spaldin, R. Ramesh, Nat. Mater. 2019, 18, 203.
J. Wang, Science 2003, 299, 1719.
B. B. Van Aken, T. T. M. Palstra, A. Filippetti, N. A. Spaldin, Nat. Mater. 2004, 3, 164.
N. Ikeda, H. Ohsumi, K. Ohwada, K. Ishii, T. Inami, K. Kakurai, Y. Murakami, K. Yoshii, S. Mori, Y. Horibe, H. Kitô, Nature 2005, 436, 1136.
A. C. Garcia-Castro, N. A. Spaldin, A. H. Romero, E. Bousquet, Phys. Rev. B 2014, 89, 104107.
A. C. Garcia-Castro, A. H. Romero, E. Bousquet, Phys. Rev. Lett. 2016, 116, 117202.
M. Yang, Amit KC, A. C. Garcia-Castro, P. Borisov, E. Bousquet, D. Lederman, A. H. Romero, C. Cen, Sci. Rep. 2017, 7, 1.
K. Page, M. W. Stoltzfus, Y.-I.l Kim, T. Proffen, P. M. Woodward, A. K. Cheetham, R. Seshadri, Chem. Mater. 2007, 19, 4037.
N. Vonrüti, U. Aschauer, Phys. Rev. Lett. 2018, 120, 046001.
M. Yang, J. Oró-Solé, A. Kusmartseva, A. Fuertes, J. P. Attfield, J. Am. Chem. Soc. 2010, 132, 4822.
M. Yang, J. Oró-Solé, J. A. Rodgers, A. B. Jorge, A. Fuertes, J. P. Attfield, Nat. Chem. 2011, 3, 47.
N. Charles, R. J. Saballos, J. M. Rondinelli, Chem. Mater. 2018, 30, 3528.
G. Gou, M. Zhao, J. Shi, J. K. Harada, J. M. Rondinelli, Chem. Mater. 2020, 32, 2815.
K. Fukutani, H. Daimon, S. Ino, Jpn. J. Appl. Phys. 1992, 31, 3429.
H. Y. Sun, Z. W. Mao, T. W. Zhang, L. Han, T. T. Zhang, X. B. Cai, X. Guo, Y. F. Li, Y. P. Zang, W. Guo, J. H. Song, D. X. Ji, C. Y. Gu, C. Tang, Z. B. Gu, N. Wang, Y. Zhu, D. G. Schlom, Y. F. Nie, X. Q. Pan, Nat. Commun. 2018, 9, 2965.
J. H. Haeni, C. D. Theis, D. G. Schlom, J. Electroceram. 2000, 4, 385.
J. H. Neave, B. A. Joyce, P. J. Dobson, N. Norton, Appl. Phys. A 1983, 31, 1.
T. Kawamura, P. A. Maksym, Surf. Sci. 1985, 161, 12.
C. S. Lent, P. I. Cohen, Surf. Sci. 1984, 139, 121.
D. Oka, Y. Hirose, S. Nakao, T. Fukumura, T. Hasegawa, Phys. Rev. B 2015, 92, 205102.
H. Hannerz, G. Svensson, S. Y.a. Istomin, O. G. D'yachenko, J. Solid State Chem. 1999, 147, 421.
A. M. Glazer, Acta Crystallogr., Sect. B: Struct. Crystallogr. Cryst. Chem. 1972, 28, 3384.
S. G. Ebbinghaus, A. Weidenkaff, A. Rachel, A. Reller, Acta Crystallogr., Sect. C: Struct. Chem. 2004, 60, i91.
S. Maintz, V. L. Deringer, A. L. Tchougréeff, R. Dronskowski, J. Comput. Chem. 2016, 37, 1030.
V. L. Deringer, A. L. Tchougréeff, R. Dronskowski, J. Phys. Chem. A 2011, 115, 5461.
S. Maintz, V. L. Deringer, A. L. Tchougréeff, R. Dronskowski, J. Comput. Chem. 2013, 34, 2557.
R. Dronskowski, P. E. Blochl, J. Phys. Chem. 1993, 978617.
G. A. Landrum, R. Dronskowski, Angew. Chem., Int. Ed. 2000, 39, 1560.
D. Oka, Y. Hirose, H. Kamisaka, T. Fukumura, K. Sasa, S. Ishii, H. Matsuzaki, Y. Sato, Y. Ikuhara, T. Hasegawa, Sci. Rep. 2014, 4, 4987.
J. S. Gelves-Badillo, A. H. Romero, A. C. Garcia-Castro, Phys. Chem. Chem. Phys. 2021, 23, 17142.
Y. Wang, X. Liu, J. D. Burton, S. S. Jaswal, E. Y. Tsymbal, Phys. Rev. Lett. 2012, 109, 247601.
H. Djani, A. C. Garcia-Castro, W.-Y.i Tong, P. Barone, E. Bousquet, S. Picozzi, P. Ghosez, npj Quantum Mater. 2019, 4, 51.
P. Sharma, F.-.X. Xiang, D.-F.u Shao, D. Zhang, E. Y. Tsymbal, A. R. Hamilton, J. Seidel, Sci. Adv. 2019, 5, eaax5080.
A. Zabalo, M. Stengel, Phys. Rev. Lett. 2021, 126, 127601.
Z. Fei, W. Zhao, T. A. Palomaki, B. Sun, M. K. Miller, Z. Zhao, J. Yan, X. Xu, D. H. Cobden, Nature 2018, 560, 336.
P. Hohenberg, W. Kohn, Phys. Rev. 1964, 136, B864.
W. Kohn, L. J. Sham, Phys. Rev. 1965, 140, A1133.
G. Kresse, J. Furthmüller, Phys. Rev. B: Condens. Matter Mater. Phys. 1996, 54, 11169.
G. Kresse, D. Joubert, Phys. Rev. B: Condens. Matter Mater. Phys. 1999, 59, 1758.
P. E. Blöchl, Phys. Rev. B 1994, 50, 17953.
J. P. Perdew, A. Ruzsinszky, G. I. Csonka, O. A. Vydrov, G. E. Scuseria, L. A. Constantin, X. Zhou, K. Burke, Phys. Rev. Lett. 2008, 100, 136406.
A. I. Liechtenstein, V. I. Anisimov, J. Zaanen, Phys. Rev. B 1995, 52, R5467.
R. Grau-Crespo, S. Hamad, C. R. A. Catlow, N. H. Leeuw, J. Phys.: Condens. Matter 2007, 19, 256201.
X. He, N. Helding, M. J. Verstraete, E. Bousquet, Mater. Sci. 2021, 264, 107938.
A. I. Liechtenstein, M. I. Katsnelson, V. P. Antropov, V. A. Gubanov, J. Magn. Magn. Mater. 1987, 67, 65.
D.m. M. Korotin, V. V. Mazurenko, V. I. Anisimov, S. V. Streltsov, Phys. Rev. B: Condens. Matter Mater. Phys. 2015, 91, 224405.
G. Pizzi, et al., J. Phys.: Condens. Matter 2020, 32, 165902.
X. Gonze, B. Amadon, G. Antonius, F. Arnardi, L. Baguet, J.-M. Beuken, J. Bieder, F. Bottin, J. Bouchet, E. Bousquet, N. Brouwer, F. Bruneval, G. Brunin, T. Cavignac, J.-.B. Charraud, W. Chen, M. Côté, S. Cottenier, J. Denier, G. Geneste, P. Ghosez, M. Giantomassi, Y. Gillet, O. Gingras, D. R. Hamann, G. Hautier, X.u He, N. Helbig, N. Holzwarth, Y. Jia, F. Jollet, W. Lafargue-Dit-Hauret, K. Lejaeghere, M. A. L. Marques, A. Martin, C. Martins, H. P. C. Miranda, F. Naccarato, K. Persson, G. Petretto, V. Planes, Y. Pouillon, S. Prokhorenko, F. Ricci, G.-M. Rignanese, A. H. Romero, M. M. Schmitt, M. Torrent, M. J. Van Setten, B. Van Troeye, M. J. Verstraete, G. Zérah, J. W. Zwanziger, Comput. Phys. Commun. 2020, 248, 107042.
A. H. Romero, D. C. Allan, B. Amadon, G. Antonius, T. Applencourt, L. Baguet, J. Bieder, F. Bottin, J. Bouchet, E. Bousquet, F. Bruneval, G. Brunin, D. Caliste, M. Côté, J. Denier, C. Dreyer, P. Ghosez, M. Giantomassi, Y. Gillet, O. Gingras, D. R. Hamann, G. Hautier, F. Jollet, G. Jomard, A. Martin, H. P. C. Miranda, F. Naccarato, G. Petretto, N. A. Pike, V. Planes, S. Prokhorenko, T. Rangel, F. Ricci, G.-M. Rignanese, M. Royo, M. Stengel, M. Torrent, M. J. Van Setten, B. Van Troeye, M. J. Verstraete, J. Wiktor, J. W. Zwanziger, X. Gonze, J. Chem. Phys. 2020, 152, 124102.
F. Bruneval, C. Varvenne, J.-P. Crocombette, E. Clouet, Phys. Rev. B 2015, 91, 024107.