Heterogeneous Integration of Freestanding Bilayer Oxide Membrane for Multiferroicity

Kang, Kyeong Tae; Corey, Zachary John; Hwang, Jaejin; Sharma, Yogesh; Paudel, Binod; Roy, Pinku; Collins, Liam; Wang, Xueijing; Lee, Joon Woo; Oh, Yoon Seok; Kim, Yeonhoo; Yoo, Jinkyoung; Lee, Jaekwang; Htoon, Han; Jia, Quanxi; Chen, Aiping

doi:10.1002/advs.202207481

Heterogeneous Integration of Freestanding Bilayer Oxide Membrane for Multiferroicity

Journal Article · Mon Apr 03 00:00:00 EDT 2023 · Advanced Science

DOI:https://doi.org/10.1002/advs.202207481· OSTI ID:1968681

Kang, Kyeong Tae ^[1]; Corey, Zachary John ^[2]; Hwang, Jaejin ^[3]; Sharma, Yogesh ^[4]; Paudel, Binod ^[4]; ^[2]; ^[5]; ^[4]; Lee, Joon Woo ^[6]; Oh, Yoon Seok ^[7]; ^[8]; ^[4]; Lee, Jaekwang ^[9]; ^[4]; Jia, Quanxi ^[10]; ^[4]

Los Alamos National Laboratory (LANL), Los Alamos, NM (United States). Center for Integrated Nanotechnologies (CINT); Kyungpook National University, Daegu (Korea, Republic of)
Los Alamos National Laboratory (LANL), Los Alamos, NM (United States). Center for Integrated Nanotechnologies (CINT); State University of New York (SUNY), Buffalo, NY (United States)
Department of Physics Pusan National University Busan 46241 South Korea; Pusan National University, Busan (Korea, Republic of)
Los Alamos National Laboratory (LANL), Los Alamos, NM (United States). Center for Integrated Nanotechnologies (CINT)
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS)
Pusan National University, Busan (Korea, Republic of); Ulsan National Institute of Science and Technology (UNIST), Ulsan (Korea, Republic of)
Ulsan National Institute of Science and Technology (UNIST), Ulsan (Korea, Republic of)
Los Alamos National Laboratory (LANL), Los Alamos, NM (United States). Center for Integrated Nanotechnologies (CINT); Korea Research Institue of Standards and Science, Daejeon (Korea, Republic of)
Pusan National Univ., Busan (Korea, Republic of)
State University of New York (SUNY), Buffalo, NY (United States)

Transition metal oxides exhibit a plethora of electrical and magnetic properties described by their order parameters. In particular, ferroic orderings offer access to a rich spectrum of fundamental physics phenomena, in addition to a range of technological applications. The heterogeneous integration of ferroelectric and ferromagnetic materials is a fruitful way to design multiferroic oxides. The realization of freestanding heterogeneous membranes of multiferroic oxides is highly desirable. In this study, epitaxial BaTiO₃/La_0.7Sr_0.3MnO₃ freestanding bilayer membranes are fabricated using pulsed laser epitaxy. The membrane displays ferroelectricity and ferromagnetism above room temperature accompanying the finite magnetoelectric coupling constant. Further, this study reveals that a freestanding heterostructure can be used to manipulate the structural and emergent properties of the membrane. In the absence of the strain caused by the substrate, the change in orbital occupancy of the magnetic layer leads to the reorientation of the magnetic easy-axis, that is, perpendicular magnetic anisotropy. These results of designing multiferroic oxide membranes open new avenues to integrate such flexible membranes for electronic applications.

View Accepted Manuscript (DOE)

Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Science (CNMS)

Sponsoring Organization:: USDOE National Nuclear Security Administration (NNSA); USDOE Laboratory Directed Research and Development (LDRD) Program; USDOE Office of Science (SC); National Science Foundation (NSF); National Research Foundation of Korea (NRF)

Grant/Contract Number:: AC05-00OR22725; 89233218CNA000001

OSTI ID:: 1968681

Alternate ID(s):: OSTI ID: 1972125

Journal Information:: Advanced Science, Journal Name: Advanced Science Journal Issue: 15 Vol. 10; ISSN 2198-3844

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

References (64)

Electrical Manipulation of Orbital Occupancy and Magnetic Anisotropy in Manganites Cui, Bin; Song, Cheng; Gehring, Gillian A. Advanced Functional Materials, Vol. 25, Issue 6 https://doi.org/10.1002/adfm.201403370	journal	December 2014
Ultraflexible and Malleable Fe/BaTiO ₃ Multiferroic Heterostructures for Functional Devices Zhao, Yanan; Peng, Renci; Guo, Yunting Advanced Functional Materials, Vol. 31, Issue 16 https://doi.org/10.1002/adfm.202009376	journal	January 2021
Flexible Ferroelectric Devices: Status and Applications Jia, Xiaotong; Guo, Rui; Tay, Beng Kang Advanced Functional Materials, Vol. 32, Issue 45 https://doi.org/10.1002/adfm.202205933	journal	September 2022
Epitaxial Lift-Off of Centimeter-Scaled Spinel Ferrite Oxide Thin Films for Flexible Electronics Shen, Lvkang; Wu, Liang; Sheng, Quan Advanced Materials, Vol. 29, Issue 33 https://doi.org/10.1002/adma.201702411	journal	June 2017
Metal Oxide Nanocomposites: A Perspective from Strain, Defect, and Interface Chen, Aiping; Su, Qing; Han, Hyungkyu Advanced Materials, Vol. 31, Issue 4 https://doi.org/10.1002/adma.201803241	journal	October 2018
A Room‐Temperature Ferroelectric Ferromagnet in a 1D Tetrahedral Chain Network Kang, Kyeong Tae; Roh, Chang Jae; Lim, Jinyoung Advanced Materials https://doi.org/10.1002/adma.201808104	journal	April 2019
Beyond Substrates: Strain Engineering of Ferroelectric Membranes Pesquera, David; Parsonnet, Eric; Qualls, Alexander Advanced Materials, Vol. 32, Issue 43 https://doi.org/10.1002/adma.202003780	journal	September 2020
Competing Interface and Bulk Effect–Driven Magnetoelectric Coupling in Vertically Aligned Nanocomposites Chen, Aiping; Dai, Yaomin; Eshghinejad, Ahmad Advanced Science, Vol. 6, Issue 19 https://doi.org/10.1002/advs.201901000	journal	August 2019
Flexible Magnetoelectric Nanocomposites with Tunable Properties Alnassar, Mohammed Y.; Ivanov, Yurii P.; Kosel, Jürgen Advanced Electronic Materials, Vol. 2, Issue 6 https://doi.org/10.1002/aelm.201600081	journal	April 2016
Freestanding Perovskite Oxide Films: Synthesis, Challenges, and Properties Chiabrera, Francesco M.; Yun, Shinhee; Li, Ying Annalen der Physik, Vol. 534, Issue 9 https://doi.org/10.1002/andp.202200084	journal	June 2022
Highly Flexible Freestanding BaTiO ₃ ‐CoFe ₂ O ₄ Heteroepitaxial Nanostructure Self‐Assembled with Room‐Temperature Multiferroicity Zhong, Gaokuo; An, Feng; Qu, Ke Small, Vol. 18, Issue 3 https://doi.org/10.1002/smll.202104213	journal	November 2021
Perpendicular magnetic anisotropy in compressive strained La0.67Sr0.33MnO3 films Xiao, Zhengyu; Zhang, Fei; Farrukh, Muhammad Akhyar Journal of Materials Science, Vol. 54, Issue 12 https://doi.org/10.1007/s10853-019-03517-5	journal	March 2019
Evolution of the charge- and strain-mediated magnetoelectric coupling effect in the La0.7Sr0.3MnO3/BaTiO3 bilayer Li, Tingxian; Zhang, Feipeng; Li, Kuoshe Journal of Alloys and Compounds, Vol. 638 https://doi.org/10.1016/j.jallcom.2015.03.121	journal	July 2015
Driving mechanism for magnetoelectric effect in CoFe2O4–BaTiO3 multiferroic composite Duong, Giap V.; Groessinger, R.; Sato Turtelli, R. Journal of Magnetism and Magnetic Materials, Vol. 310, Issue 2 https://doi.org/10.1016/j.jmmm.2006.10.333	journal	March 2007
Thickness dependence of dynamic and static magnetic properties of pulsed laser deposited La0.7Sr0.3MnO3 films on SrTiO3(001) Monsen, Åsmund; Boschker, Jos E.; Macià, Ferran Journal of Magnetism and Magnetic Materials, Vol. 369 https://doi.org/10.1016/j.jmmm.2014.06.038	journal	November 2014
Influence of clamping effect in BaTiO3 film on the magnetoelectric behavior of layered multiferroic heterostructures Li, Tingxian; Wang, Hongwei; Ma, Dongwei Materials Research Bulletin, Vol. 115 https://doi.org/10.1016/j.materresbull.2019.03.026	journal	July 2019
Freestanding Oxide Ferroelectric Tunnel Junction Memories Transferred onto Silicon Lu, Di; Crossley, Sam; Xu, Ruijuan Nano Letters, Vol. 19, Issue 6 https://doi.org/10.1021/acs.nanolett.9b01327	journal	April 2019
Flexible Memristors Based on Single-Crystalline Ferroelectric Tunnel Junctions Luo, Zheng-Dong; Peters, Jonathan J. P.; Sanchez, Ana M. ACS Applied Materials & Interfaces, Vol. 11, Issue 26 https://doi.org/10.1021/acsami.9b04738	journal	June 2019
Flexible Quasi-Two-Dimensional CoFe ₂ O ₄ Epitaxial Thin Films for Continuous Strain Tuning of Magnetic Properties Zhang, Yong; Shen, Lvkang; Liu, Ming ACS Nano, Vol. 11, Issue 8 https://doi.org/10.1021/acsnano.7b02637	journal	June 2017
Deterministic switching of ferromagnetism at room temperature using an electric field Heron, J. T.; Bosse, J. L.; He, Q. Nature, Vol. 516, Issue 7531 https://doi.org/10.1038/nature14004	journal	December 2014
Synthesis of freestanding single-crystal perovskite films and heterostructures by etching of sacrificial water-soluble layers Lu, Di; Baek, David J.; Hong, Seung Sae Nature Materials, Vol. 15, Issue 12 https://doi.org/10.1038/nmat4749	journal	September 2016
Emergent functions of quantum materials Tokura, Yoshinori; Kawasaki, Masashi; Nagaosa, Naoto Nature Physics, Vol. 13, Issue 11 https://doi.org/10.1038/nphys4274	journal	September 2017
Advances in magnetoelectric multiferroics Spaldin, N. A.; Ramesh, R. Nature Materials, Vol. 18, Issue 3 https://doi.org/10.1038/s41563-018-0275-2	journal	February 2019
Freestanding crystalline oxide perovskites down to the monolayer limit Ji, Dianxiang; Cai, Songhua; Paudel, Tula R. Nature, Vol. 570, Issue 7759 https://doi.org/10.1038/s41586-019-1255-7	journal	June 2019
Heterogeneous integration of single-crystalline complex-oxide membranes Kum, Hyun S.; Lee, Hyungwoo; Kim, Sungkyu Nature, Vol. 578, Issue 7793 https://doi.org/10.1038/s41586-020-1939-z	journal	February 2020
Epitaxial lift-off of freestanding (011) and (111) SrRuO3 thin films using a water sacrificial layer Le, Phu T. P.; ten Elshof, Johan E.; Koster, Gertjan Scientific Reports, Vol. 11, Issue 1 https://doi.org/10.1038/s41598-021-91848-2	journal	June 2021
Oxygen Vacancy-Tuned Physical Properties in Perovskite Thin Films with Multiple B-site Valance States Enriquez, Erik; Chen, Aiping; Harrell, Zach Scientific Reports, Vol. 7, Issue 1 https://doi.org/10.1038/srep46184	journal	April 2017
Direct fabrication of BiFeO₃ thin films on polyimide substrates for flexible electronics Tomczyk, Monika; Bretos, Iñigo; Jiménez, Ricardo Journal of Materials Chemistry C, Vol. 5, Issue 47 https://doi.org/10.1039/C7TC04571A	journal	January 2017
Thickness evolution of the twin structure and shear strain in LSMO films Santiso, José; Balcells, Lluis; Konstantinovic, Zorica CrystEngComm, Vol. 15, Issue 19 https://doi.org/10.1039/c3ce40085a	journal	January 2013
Tuning the growth and strain relaxation of ferroelectric BaTiO₃ thin films on SrRuO₃ electrode: influence on electrical properties Aidoud, Amina; Maroutian, Thomas; Matzen, Sylvia The European Physical Journal Applied Physics, Vol. 80, Issue 3 https://doi.org/10.1051/epjap/2017170314	journal	December 2017
The role of strain in magnetic anisotropy of manganite thin films Suzuki, Y.; Hwang, H. Y.; Cheong, S-W. Applied Physics Letters, Vol. 71, Issue 1 https://doi.org/10.1063/1.119454	journal	July 1997
Magnetic anisotropy of ferromagnetic La0.7(Sr, Ca)0.3MnO3 epitaxial films Steenbeck, K.; Hiergeist, R. Applied Physics Letters, Vol. 75, Issue 12 https://doi.org/10.1063/1.124817	journal	September 1999
Strain-dependent magnetic phase diagram of epitaxial La0.67Sr0.33MnO3 thin films Tsui, F.; Smoak, M. C.; Nath, T. K. Applied Physics Letters, Vol. 76, Issue 17 https://doi.org/10.1063/1.126363	journal	April 2000
Strain modification of epitaxial perovskite oxide thin films using structural transitions of ferroelectric BaTiO3 substrate Lee, M. K.; Nath, T. K.; Eom, C. B. Applied Physics Letters, Vol. 77, Issue 22 https://doi.org/10.1063/1.1328762	journal	November 2000
Step-induced uniaxial magnetic anisotropy of La0:67Sr0:33MnO3 thin films Mathews, Mercy; Postma, Ferry M.; Lodder, J. Cock Applied Physics Letters, Vol. 87, Issue 24 https://doi.org/10.1063/1.2143136	journal	December 2005
Synthesis of ordered arrays of multiferroic NiFe2O4-Pb(Zr0.52Ti0.48)O3 core-shell nanowires Liu, Ming; Li, Xin; Imrane, Hassan Applied Physics Letters, Vol. 90, Issue 15 https://doi.org/10.1063/1.2722043	journal	April 2007
Quantitative determination of anisotropic magnetoelectric coupling in BiFeO3–CoFe2O4 nanostructures Oh, Yoon Seok; Crane, S.; Zheng, H. Applied Physics Letters, Vol. 97, Issue 5 https://doi.org/10.1063/1.3475420	journal	August 2010
Multiferroics: Past, present, and future Spaldin, Nicola A.; Cheong, Sang-Wook; Ramesh, Ramamoorthy Physics Today, Vol. 63, Issue 10 https://doi.org/10.1063/1.3502547	journal	October 2010
Tailoring magnetic anisotropy in epitaxial half metallic La _0.7 Sr _0.3 MnO ₃ thin films Perna, P.; Rodrigo, C.; Jiménez, E. Journal of Applied Physics, Vol. 110, Issue 1 https://doi.org/10.1063/1.3605542	journal	July 2011
Magnetic properties of BaTiO₃/La_0.7Sr_0.3MnO₃ thin films integrated on Si(100) Singamaneni, Srinivasa Rao; Fan, Wu; Prater, J. T. Journal of Applied Physics, Vol. 116, Issue 22 https://doi.org/10.1063/1.4903322	journal	December 2014
Synthesis of single-crystal La_0.67Sr_0.33MnO₃ freestanding films with different crystal-orientation Lu, Zengxing; Liu, Jingwu; Feng, Jiatai APL Materials, Vol. 8, Issue 5 https://doi.org/10.1063/1.5145029	journal	May 2020
Anisotropic domains and antiferrodistortive-transition controlled magnetization in epitaxial manganite films on vicinal SrTiO ₃ substrates Paudel, Binod; Zhang, Bruce; Sharma, Yogesh Applied Physics Letters, Vol. 117, Issue 8 https://doi.org/10.1063/5.0016371	journal	August 2020
Freestanding La _0.7 Sr _0.3 MnO ₃ :NiO vertically aligned nanocomposite thin films for flexible perpendicular interfacial exchange coupling Huang, Jijie; Zhang, Di; Liu, Juncheng Materials Research Letters, Vol. 10, Issue 4 https://doi.org/10.1080/21663831.2022.2041502	journal	March 2022
Effect of misfit strain on multiferroic and magnetoelectric properties of epitaxial La_0.7Sr_0.3MnO₃/BaTiO₃ bilayer Li, T. X.; Zhang, M.; Yu, F. J. Journal of Physics D: Applied Physics, Vol. 45, Issue 8 https://doi.org/10.1088/0022-3727/45/8/085002	journal	February 2012
Multiferroics of spin origin Tokura, Yoshinori; Seki, Shinichiro; Nagaosa, Naoto Reports on Progress in Physics, Vol. 77, Issue 7 https://doi.org/10.1088/0034-4885/77/7/076501	journal	July 2014
Ab initiomolecular dynamics for liquid metals Kresse, G.; Hafner, J. Physical Review B, Vol. 47, Issue 1, p. 558-561 https://doi.org/10.1103/PhysRevB.47.558	journal	January 1993
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
Pressure effects on the magnetoresistance in doped manganese perovskites Hwang, H. Y.; Palstra, T. T. M.; Cheong, S- W. Physical Review B, Vol. 52, Issue 21 https://doi.org/10.1103/PhysRevB.52.15046	journal	December 1995
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
Generalized gradient approximation for the exchange-correlation hole of a many-electron system Perdew, John P.; Burke, Kieron; Wang, Yue Physical Review B, Vol. 54, Issue 23 https://doi.org/10.1103/PhysRevB.54.16533	journal	December 1996
Fully unconstrained noncollinear magnetism within the projector augmented-wave method Hobbs, D.; Kresse, G.; Hafner, J. Physical Review B, Vol. 62, Issue 17 https://doi.org/10.1103/PhysRevB.62.11556	journal	November 2000
Broken symmetries in the crystalline and magnetic structures of γ -iron Marsman, M.; Hafner, J. Physical Review B, Vol. 66, Issue 22 https://doi.org/10.1103/PhysRevB.66.224409	journal	December 2002
Strong uniaxial in-plane magnetic anisotropy of (001)- and (011)-oriented La 0.67 Sr 0.33 MnO 3 thin films on NdGaO 3 substrates Boschker, H.; Mathews, M.; Houwman, E. P. Physical Review B, Vol. 79, Issue 21 https://doi.org/10.1103/PhysRevB.79.214425	journal	June 2009
Large Magnetovolume Effect in Yttrium Doped La-Ca-Mn-O Perovskite Ibarra, M. R.; Algarabel, P. A.; Marquina, C. Physical Review Letters, Vol. 75, Issue 19 https://doi.org/10.1103/PhysRevLett.75.3541	journal	November 1995
Freestanding crystalline YB a 2 C u 3 O 7 − x heterostructure membranes Chen, Zhuoyu; Wang, Bai Yang; Goodge, Berit H. Physical Review Materials, Vol. 3, Issue 6 https://doi.org/10.1103/PhysRevMaterials.3.060801	journal	June 2019
Role of scaffold network in controlling strain and functionalities of nanocomposite films Chen, Aiping; Hu, Jia-Mian; Lu, Ping Science Advances, Vol. 2, Issue 6 https://doi.org/10.1126/sciadv.1600245	journal	June 2016
Phase transition enhanced superior elasticity in freestanding single-crystalline multiferroic BiFeO ₃ membranes Peng, Bin; Peng, Ren-Ci; Zhang, Yong-Qiang Science Advances, Vol. 6, Issue 34 https://doi.org/10.1126/sciadv.aba5847	journal	August 2020
Epitaxial BiFeO₃ Multiferroic Thin Film Heterostructures Wang, J.; Neaton, J. B.; Zheng, H. Science, Vol. 299, Issue 5613, p. 1719-1722 https://doi.org/10.1126/science.1080615	journal	March 2003
Multiferroic BaTiO3-CoFe2O4 Nanostructures Zheng, H. Science, Vol. 303, Issue 5658 https://doi.org/10.1126/science.1094207	journal	January 2004
Extreme tensile strain states in La _0.7 Ca _0.3 MnO ₃ membranes Hong, Seung Sae; Gu, Mingqiang; Verma, Manish Science, Vol. 368, Issue 6486 https://doi.org/10.1126/science.aax9753	journal	April 2020
Super-elastic ferroelectric single-crystal membrane with continuous electric dipole rotation Dong, Guohua; Li, Suzhi; Yao, Mouteng Science, Vol. 366, Issue 6464 https://doi.org/10.1126/science.aay7221	journal	October 2019
Substrate clamping effect onto magnetoelectric coupling in multiferroic BaTiO ₃ -CoFe ₂ O ₄ core-shell nanofibers via coaxial electrospinning Fu, Bi; Lu, Ruie; Gao, Kun EPL (Europhysics Letters), Vol. 112, Issue 2 https://doi.org/10.1209/0295-5075/112/27002	journal	October 2015
Surface-Step-Induced Magnetic Anisotropy in Epitaxial LSMO Deposited on Engineered STO Surfaces Pawlak, Jakub; Żywczak, Antoni; Kanak, Jarosław Materials, Vol. 13, Issue 18 https://doi.org/10.3390/ma13184148	journal	September 2020
The path to flexible ferroelectrics: Approaches and progress Chang, Lei; You, Lu; Wang, Junling Japanese Journal of Applied Physics, Vol. 57, Issue 9 https://doi.org/10.7567/JJAP.57.0902A3	journal	June 2018

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