DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Nanoengineering room temperature ferroelectricity into orthorhombic SmMnO3 films

Abstract

Orthorhombic RMnO3 (R = rare-earth cation) compounds are type-II multiferroics induced by inversion-symmetry-breaking of spin order. They hold promise for magneto-electric devices. However, no spontaneous room-temperature ferroic property has been observed to date in orthorhombic RMnO3. Here, using 3D straining in nanocomposite films of (SmMnO3)0.5((Bi,Sm)2O3)0.5, we demonstrate room temperature ferroelectricity and ferromagnetism with TC,FM ~ 90 K, matching exactly with theoretical predictions for the induced strain levels. Large in-plane compressive and out-of-plane tensile strains (-3.6% and +4.9%, respectively) were induced by the stiff (Bi,Sm)2O3 nanopillars embedded. The room temperature electric polarization is comparable to other spin-driven ferroelectric RMnO3 films. Also, while bulk SmMnO3 is antiferromagnetic, ferromagnetism was induced in the composite films. The Mn-O bond angles and lengths determined from density functional theory explain the origin of the ferroelectricity, i.e. modification of the exchange coupling. Our structural tuning method gives a route to designing multiferroics.

Authors:
ORCiD logo [1]; ORCiD logo [2];  [3]; ORCiD logo [4];  [5];  [6];  [6]; ORCiD logo [3];  [3];  [6]; ORCiD logo [5];  [3]
  1. Univ. of Cambridge (United Kingdom); Sungkyunkwan Univ. (SKKU), Suwon (South Korea). Center for Integrated Nanostructure Physics (CINAP), Inst. for Basic Science (IBS)
  2. Univ. of Cambridge (United Kingdom); Sungkyunkwan Univ. (SKKU), Suwon (South Korea). Center for Integrated Nanostructure Physics (CINAP), Inst. for Basic Science (IBS); Indian Inst. of Science Education and Research, Kerala (India)
  3. Univ. of Cambridge (United Kingdom)
  4. Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)
  5. Purdue Univ., West Lafayette, IN (United States)
  6. Pennsylvania State Univ., University Park, PA (United States)
Publication Date:
Research Org.:
Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)
Sponsoring Org.:
USDOE National Nuclear Security Administration (NNSA); Engineering and Physical Sciences Research Council (EPSRC)
OSTI Identifier:
1668354
Report Number(s):
SAND-2020-4894J
Journal ID: ISSN 2041-1723; 685972; TRN: US2203690
Grant/Contract Number:  
AC04-94AL85000; EP/L011700/1; EP/N004272/; SC0020145; NA0003525
Resource Type:
Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 11; Journal Issue: 1; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY; Condensed-matter physics; ferroelectrics and multiferroics; materials science

Citation Formats

Choi, Eun-Mi, Maity, Tuhin, Kursumovic, Ahmed, Lu, Ping, Bi, Zenxhing, Yu, Shukai, Park, Yoonsang, Zhu, Bonan, Wu, Rui, Gopalan, Venkatraman, Wang, Haiyan, and MacManus-Driscoll, Judith L. Nanoengineering room temperature ferroelectricity into orthorhombic SmMnO3 films. United States: N. p., 2020. Web. doi:10.1038/s41467-020-16101-2.
Choi, Eun-Mi, Maity, Tuhin, Kursumovic, Ahmed, Lu, Ping, Bi, Zenxhing, Yu, Shukai, Park, Yoonsang, Zhu, Bonan, Wu, Rui, Gopalan, Venkatraman, Wang, Haiyan, & MacManus-Driscoll, Judith L. Nanoengineering room temperature ferroelectricity into orthorhombic SmMnO3 films. United States. https://doi.org/10.1038/s41467-020-16101-2
Choi, Eun-Mi, Maity, Tuhin, Kursumovic, Ahmed, Lu, Ping, Bi, Zenxhing, Yu, Shukai, Park, Yoonsang, Zhu, Bonan, Wu, Rui, Gopalan, Venkatraman, Wang, Haiyan, and MacManus-Driscoll, Judith L. Tue . "Nanoengineering room temperature ferroelectricity into orthorhombic SmMnO3 films". United States. https://doi.org/10.1038/s41467-020-16101-2. https://www.osti.gov/servlets/purl/1668354.
@article{osti_1668354,
title = {Nanoengineering room temperature ferroelectricity into orthorhombic SmMnO3 films},
author = {Choi, Eun-Mi and Maity, Tuhin and Kursumovic, Ahmed and Lu, Ping and Bi, Zenxhing and Yu, Shukai and Park, Yoonsang and Zhu, Bonan and Wu, Rui and Gopalan, Venkatraman and Wang, Haiyan and MacManus-Driscoll, Judith L.},
abstractNote = {Orthorhombic RMnO3 (R = rare-earth cation) compounds are type-II multiferroics induced by inversion-symmetry-breaking of spin order. They hold promise for magneto-electric devices. However, no spontaneous room-temperature ferroic property has been observed to date in orthorhombic RMnO3. Here, using 3D straining in nanocomposite films of (SmMnO3)0.5((Bi,Sm)2O3)0.5, we demonstrate room temperature ferroelectricity and ferromagnetism with TC,FM ~ 90 K, matching exactly with theoretical predictions for the induced strain levels. Large in-plane compressive and out-of-plane tensile strains (-3.6% and +4.9%, respectively) were induced by the stiff (Bi,Sm)2O3 nanopillars embedded. The room temperature electric polarization is comparable to other spin-driven ferroelectric RMnO3 films. Also, while bulk SmMnO3 is antiferromagnetic, ferromagnetism was induced in the composite films. The Mn-O bond angles and lengths determined from density functional theory explain the origin of the ferroelectricity, i.e. modification of the exchange coupling. Our structural tuning method gives a route to designing multiferroics.},
doi = {10.1038/s41467-020-16101-2},
journal = {Nature Communications},
number = 1,
volume = 11,
place = {United States},
year = {Tue May 05 00:00:00 EDT 2020},
month = {Tue May 05 00:00:00 EDT 2020}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record

Figures / Tables:

Fig. 1 Fig. 1: Electron microscopy images of thick SMO:BSO VAN film grown on STO (001). a Cross-sectional STEM-HAADF image showing clear pillars of BSO embedded in SMO. The BSO grows faster than SMO as observed by the pillars being thicker than the SMO. b BSO and SMO showing domain matching epitaxymore » of 7 unit cells of SMO matching with 5 unit cells of BSO. d Plan-view STEM-HAADF image shows a VAN structure over a wide area. A regular pattern of connected BSO pillars in an SMO matrix is observed. e A region of SMO enclosed by laterally connected BSO pillars is shown. c, f EDS maps and line profiles of across the VAN film, showing that SMO contains only very minor Bi and that BSO has a -1:1 Bi:Sm ratio. Scale bar: 10 nm.« less

Save / Share:

Works referenced in this record:

Evidence for large electric polarization from collinear magnetism in TmMnO 3
journal, April 2009


Effects of strain on ferroelectric polarization and magnetism in orthorhombic HoMnO 3
journal, January 2013


Emergence of ferromagnetism in antiferromagnetic TbMnO3 by epitaxial strain
journal, May 2010

  • Marti, X.; Skumryev, V.; Ferrater, C.
  • Applied Physics Letters, Vol. 96, Issue 22
  • DOI: 10.1063/1.3443714

Nanoscale domain evolution in thin films of multiferroic TbMnO 3
journal, December 2009


Ferroelectric Sm-Doped BiMnO 3 Thin Films with Ferromagnetic Transition Temperature Enhanced to 140 K
journal, August 2014

  • Choi, Eun-Mi; Kursumovic, Ahmed; Lee, Oon Jew
  • ACS Applied Materials & Interfaces, Vol. 6, Issue 17
  • DOI: 10.1021/am501351c

Magnetic control of ferroelectric polarization
journal, November 2003


Magnetically induced ferroelectricity in orthorhombic manganites: Microscopic origin and chemical trends
journal, July 2008


Abnormal magnetic ordering and ferromagnetism in perovskite ScMnO 3 film
journal, June 2015

  • Wang, F.; Zhang, Y. Q.; Liu, W.
  • Applied Physics Letters, Vol. 106, Issue 23
  • DOI: 10.1063/1.4922727

Extensive Series of Hexagonal and Orthorhombic RMnO 3 (R = Y, La, Sm, Tb, Yb, Lu) Thin Films by Atomic Layer Deposition
journal, April 2011

  • Uusi-Esko, Kristina; Karppinen, Maarit
  • Chemistry of Materials, Vol. 23, Issue 7
  • DOI: 10.1021/cm103480d

New strain states and radical property tuning of metal oxides using a nanocomposite thin film approach
journal, June 2015

  • MacManus-Driscoll, Judith; Suwardi, Ady; Kursumovic, Ahmed
  • APL Materials, Vol. 3, Issue 6
  • DOI: 10.1063/1.4919059

Distorted perovskite with e g 1 configuration as a frustrated spin system
journal, August 2003


Epitaxial TbMnO 3 thin films on SrTiO 3 substrates: a structural study
journal, March 2009


Dielectric and AC-Calorimetry Measurements of SmMnO 3 under High Pressure
journal, January 2012

  • Aoyama, Takuya; Miyake, Atsushi; Shimizu, Katsuya
  • Journal of the Physical Society of Japan, Vol. 81, Issue Suppl.B
  • DOI: 10.1143/JPSJS.81SB.SB036

Thick lead-free ferroelectric films with high Curie temperatures through nanocomposite-induced strain
journal, July 2011

  • Harrington, Sophie A.; Zhai, Junyi; Denev, Sava
  • Nature Nanotechnology, Vol. 6, Issue 8
  • DOI: 10.1038/nnano.2011.98

Ab Initio Study on Structure, Elastic, and Mechanical Properties of Lanthanide Sesquioxides
journal, February 2018

  • Pathak, Arup Kumar; Vazhappilly, Tijo
  • physica status solidi (b), Vol. 255, Issue 6
  • DOI: 10.1002/pssb.201700668

Composite epitaxial thin films: A new platform for tuning, probing, and exploiting mesoscale oxides
journal, November 2015

  • MacManus-Driscoll, J. L.; Suwardi, A.; Wang, H.
  • MRS Bulletin, Vol. 40, Issue 11
  • DOI: 10.1557/mrs.2015.258

β B i 2 O 3 under compression: Optical and elastic properties and electron density topology analysis
journal, June 2016


Ferroelectricity and Giant Magnetocapacitance in Perovskite Rare-Earth Manganites
journal, June 2004


Microscopic model and phase diagrams of the multiferroic perovskite manganites
journal, October 2009


Turning antiferromagnetic Sm 0.34 Sr 0.66 MnO 3 into a 140 K ferromagnet using a nanocomposite strain tuning approach
journal, January 2016

  • Suwardi, Ady; Prasad, Bhagwati; Lee, Shinbuhm
  • Nanoscale, Vol. 8, Issue 15
  • DOI: 10.1039/C6NR01037G

Artificial chemical and magnetic structure at the domain walls of an epitaxial oxide
journal, November 2014

  • Farokhipoor, S.; Magén, C.; Venkatesan, S.
  • Nature, Vol. 515, Issue 7527
  • DOI: 10.1038/nature13918

Tunnel junctions with multiferroic barriers
journal, March 2007

  • Gajek, Martin; Bibes, Manuel; Fusil, Stéphane
  • Nature Materials, Vol. 6, Issue 4
  • DOI: 10.1038/nmat1860

Room-temperature multiferroic magnetoelectrics
journal, November 2013


Ab initio Modeling of Elastic and Optical Properties of Sb and Bi Sesquioxides
journal, June 2018


Relationship between crystal structure and multiferroic orders in orthorhombic perovskite manganites
journal, October 2018


Mixed-valence manganites
journal, March 1999


Multiferroics: a magnetic twist for ferroelectricity
journal, January 2007

  • Cheong, Sang-Wook; Mostovoy, Maxim
  • Nature Materials, Vol. 6, Issue 1
  • DOI: 10.1038/nmat1804

Giant spin-driven ferroelectric polarization in TbMnO3 under high pressure
journal, September 2014

  • Aoyama, T.; Yamauchi, K.; Iyama, A.
  • Nature Communications, Vol. 5, Issue 1
  • DOI: 10.1038/ncomms5927

Multiferroic properties and magnetic structure of Sm 1 x Y x MnO 3
journal, May 2011


Magnetoelectric phase diagrams of orthorhombic R MnO 3 ( R = Gd , Tb, and Dy)
journal, June 2005


Lattice dynamics of manganites R MnO 3 ( R  =Sm, Eu or Gd): instabilities and coexistence of orthorhombic and hexagonal phases
journal, July 2009


A new technique based on current measurement for nanoscale ferroelectricity assessment: Nano-positive up negative down
journal, February 2017

  • Martin, Simon; Baboux, Nicolas; Albertini, David
  • Review of Scientific Instruments, Vol. 88, Issue 2
  • DOI: 10.1063/1.4974953

Materials Data on SmMnO3 (SG:62) by Materials Project
dataset, January 2016

  • Available, None
  • LBNL Materials Project; Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
  • DOI: 10.17188/1200426

Figures/Tables have been extracted from DOE-funded journal article accepted manuscripts.