Non-volatile electric-field control of inversion symmetry

Lucas Caretta; Yu-Tsun Shao; Jia Yu; Antonio B Mei; Bastien F Grosso; Cheng Dai; Piush Behera; Daehun Lee; Margaret McCarter; Eric Parsonnet; Harikrishnan K P; Fei Xue; Xiangwei Guo; Edward S Barnard; Steffen Ganschow; Zijian Hong; Archana Raja; Lane W Martin; Long-Qing Chen; Manfred Fiebig; Keji Lai; Nicola A Spaldin; David A Muller; Darrell G Schlom; Ramamoorthy Ramesh

doi:10.1038/s41563-022-01412-0

Non-volatile electric-field control of inversion symmetry

Nat Mater. 2023 Feb;22(2):207-215. doi: 10.1038/s41563-022-01412-0. Epub 2022 Dec 19.

Authors

Lucas Caretta^#^{1

2}, Yu-Tsun Shao^#^{3

4}, Jia Yu⁵, Antonio B Mei⁶, Bastien F Grosso⁷, Cheng Dai⁸, Piush Behera⁹, Daehun Lee⁵, Margaret McCarter¹⁰, Eric Parsonnet¹⁰, Harikrishnan K P³, Fei Xue⁸, Xiangwei Guo^{11

12}, Edward S Barnard¹³, Steffen Ganschow¹⁴, Zijian Hong¹¹, Archana Raja¹³, Lane W Martin^{9

15}, Long-Qing Chen⁸, Manfred Fiebig⁷, Keji Lai⁵, Nicola A Spaldin⁷, David A Muller^{3

16}, Darrell G Schlom^{6

14

16}, Ramamoorthy Ramesh^{17

18

19}

Affiliations

¹ Department of Materials Science and Engineering, University of California, Berkeley, CA, USA. lucas_caretta@brown.edu.
² School of Engineering, Brown University, Providence, RI, USA. lucas_caretta@brown.edu.
³ School of Applied and Engineering Physics, Cornell University, Ithaca, NY, USA.
⁴ Mork Family Department of Chemical Engineering and Materials Science, University of Southern California, Los Angeles, CA, USA.
⁵ Department of Physics, University of Texas, Austin, TX, USA.
⁶ Department of Materials Science and Engineering, Cornell University, Ithaca, NY, USA.
⁷ Department of Materials, ETH Zurich, Zurich, Switzerland.
⁸ Department of Materials Science and Engineering, The Pennsylvania State University, University Park, PA, USA.
⁹ Department of Materials Science and Engineering, University of California, Berkeley, CA, USA.
¹⁰ Department of Physics, University of California, Berkeley, CA, USA.
¹¹ State Key Laboratory of Silicon Materials, School of Materials Science and Engineering, Zhejiang University, Hangzhou, China.
¹² Hangzhou Global Scientific and Technological Innovation Center, Zhejiang University, Hangzhou, China.
¹³ Molecular Foundry, Lawrence Berkeley National Laboratory, Berkeley, CA, USA.
¹⁴ Leibniz-Institut für Kristallzüchtung, Berlin, Germany.
¹⁵ Materials Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, CA, USA.
¹⁶ Kavli Institute at Cornell for Nanoscale Science, Ithaca, NY, USA.
¹⁷ Department of Materials Science and Engineering, University of California, Berkeley, CA, USA. rramesh@berkeley.edu.
¹⁸ Department of Physics, University of California, Berkeley, CA, USA. rramesh@berkeley.edu.
¹⁹ Materials Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, CA, USA. rramesh@berkeley.edu.

^# Contributed equally.

PMID: 36536139
DOI: 10.1038/s41563-022-01412-0

Abstract

Competition between ground states at phase boundaries can lead to significant changes in properties under stimuli, particularly when these ground states have different crystal symmetries. A key challenge is to stabilize and control the coexistence of symmetry-distinct phases. Using BiFeO₃ layers confined between layers of dielectric TbScO₃ as a model system, we stabilize the mixed-phase coexistence of centrosymmetric and non-centrosymmetric BiFeO₃ phases at room temperature with antipolar, insulating and polar semiconducting behaviour, respectively. Application of orthogonal in-plane electric (polar) fields results in reversible non-volatile interconversion between the two phases, hence removing and introducing centrosymmetry. Counterintuitively, we find that an electric field 'erases' polarization, resulting from the anisotropy in octahedral tilts introduced by the interweaving TbScO₃ layers. Consequently, this interconversion between centrosymmetric and non-centrosymmetric phases generates changes in the non-linear optical response of over three orders of magnitude, resistivity of over five orders of magnitude and control of microscopic polar order. Our work establishes a platform for cross-functional devices that take advantage of changes in optical, electrical and ferroic responses, and demonstrates octahedral tilts as an important order parameter in materials interface design.

Grants and funding

ETHOS MURI W911NF-21-2-0162/United States Department of Defense | United States Army | U.S. Army Research, Development and Engineering Command | Army Research Office (ARO)