Title: Size‐Induced Ferroelectricity in Antiferroelectric Oxide Membranes

Abstract

Despite extensive studies on size effects in ferroelectrics, how structures and properties evolve in antiferroelectrics with reduced dimensions still remains elusive. Given the enormous potential of utilizing antiferroelectrics for high-energy-density storage applications, understanding their size effects will provide key information for optimizing device performances at small scales. Here, the fundamental intrinsic size dependence of antiferroelectricity in lead-free NaNbO₃ membranes is investigated. Via a wide range of experimental and theoretical approaches, an intriguing antiferroelectric-to-ferroelectric transition upon reducing membrane thickness is probed. This size effect leads to a ferroelectric single-phase below 40 nm, as well as a mixed-phase state with ferroelectric and antiferroelectric orders coexisting above this critical thickness. Furthermore, it is shown that the antiferroelectric and ferroelectric orders are electrically switchable. First-principle calculations further reveal that the observed transition is driven by the structural distortion arising from the membrane surface. This work provides direct experimental evidence for intrinsic size-driven scaling in antiferroelectrics and demonstrates enormous potential of utilizing size effects to drive emergent properties in environmentally benign lead-free oxides with the membrane platform.

Authors:

Xu, Ruijuan  ^[1];

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Crust, Kevin J. ^[2]; Harbola, Varun ^[2]; Arras, Rémi ^[3]; Patel, Kinnary Y. ^[4]; Prosandeev, Sergey ^[4]; Cao, Hui ^[5]; Shao, Yu‐Tsun ^[6]; Behera, Piush ^[7]; Caretta, Lucas ^[8]; Kim, Woo Jin ^[9]; Khandelwal, Aarushi ^[9]; Acharya, Megha ^[10]; Wang, Melody M. ^[11]; Liu, Yin ^[12]; Barnard, Edward S. ^[13]; Raja, Archana ^[13]; Martin, Lane W. ^[10]; Gu, X. Wendy ^[14]; Zhou, Hua ^[15] more »; Ramesh, Ramamoorthy ^[16]; Muller, David A. ^[17]; Bellaiche, Laurent ^[4]; Hwang, Harold Y. ^[9] « less

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+ Show Author Affiliations

1. Department of Applied Physics Stanford University Stanford CA 94305 USA, Stanford Institute for Materials and Energy Sciences SLAC National Accelerator Laboratory Menlo Park CA 94025 USA, Department of Materials Science and Engineering North Carolina State University Raleigh NC 27606 USA
2. Stanford Institute for Materials and Energy Sciences SLAC National Accelerator Laboratory Menlo Park CA 94025 USA, Department of Physics Stanford University Stanford CA 94305 USA
3. CEMES Université de Toulouse CNRS UPS, 29 rue Jeanne Marvig F‐31055 Toulouse France
4. Physics Department and Institute for Nanoscience and Engineering University of Arkansas Fayetteville AR 72701 USA
5. Materials Science Division Argonne National Laboratory Lemont IL 60439 USA
6. Department of Applied and Engineering Physics Cornell University Ithaca NY 14853 USA, Mork Family Department of Chemical Engineering and Materials Science University of Southern California Los Angeles CA 90089 USA
7. Department of Materials Science and Engineering University of California Berkeley Berkeley CA 94720 USA
8. Department of Materials Science and Engineering University of California Berkeley Berkeley CA 94720 USA, School of Engineering Brown University Providence RI 02912 USA
9. Department of Applied Physics Stanford University Stanford CA 94305 USA, Stanford Institute for Materials and Energy Sciences SLAC National Accelerator Laboratory Menlo Park CA 94025 USA
10. Department of Materials Science and Engineering University of California Berkeley Berkeley CA 94720 USA, Materials Sciences Division Lawrence Berkeley National Laboratory Berkeley CA 94720 USA
11. Department of Materials Science and Engineering Stanford University Stanford CA 94305 USA
12. Department of Materials Science and Engineering North Carolina State University Raleigh NC 27606 USA
13. The Molecular Foundry Lawrence Berkeley National Laboratory 1 Cyclotron Road Berkeley CA 94720 USA
14. Department of Mechanical Engineering Stanford University Stanford CA 94305 USA
15. X‐ray Science Division Advanced Photon Source Argonne National Laboratory Lemont IL 60439 USA
16. Department of Materials Science and Nanoengineering Department of Physics and Astronomy Rice University Houston TX 77251 USA
17. Department of Applied and Engineering Physics Cornell University Ithaca NY 14853 USA

Publication Date:

Sun Mar 19 00:00:00 EDT 2023

Research Org.:

Argonne National Laboratory (ANL), Argonne, IL (United States). Advanced Photon Source (APS); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). Molecular Foundry; SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)

Sponsoring Org.:

USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division (MSE); National Science Foundation (NSF); US Army Research Office (ARO); USDOD; US Department of the Navy, Office of Naval Research (ONR); US Air Force Office of Scientific Research (AFOSR); North Carolina State University; University of California System; USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF); Vannevar Bush Faculty Fellowship (VBFF); USDOE Office of Science (SC), Basic Energy Sciences (BES)

OSTI Identifier:

1962461

Alternate Identifier(s):

OSTI ID: 1962463; OSTI ID: 1988274; OSTI ID: 2000755; OSTI ID: 2228946; OSTI ID: 2305345

Grant/Contract Number:  

DE‐AC02‐76SF00515; DE‐AC02‐05CH11231; DE‐AC02‐05‐CH11231; DE‐SC0021075; DE‐AC02‐06CH11357; AC02-06CH11357; AC02-76SF00515; AC02-05CH11231; SC0021075; ECCS-1542152; W911NF-21-2-0162; N00014-20-1-2834; N00014-21-1-2086; FA9550-18-1-0480; W911NF-21-1-0118; DGE-1656518

Resource Type:

Published Article

Journal Name:

Advanced Materials

Additional Journal Information:

Journal Name: Advanced Materials Journal Volume: 35 Journal Issue: 17; Journal ID: ISSN 0935-9648

Publisher:

Wiley Blackwell (John Wiley & Sons)

Country of Publication:

Germany

Language:

English

Subject:

36 MATERIALS SCIENCE; antiferroelectric materials; membranes; phase transition; size effects; sodium niobate; membrane; antiferroelectric