Out-of-plane ferroelectricity and robust magnetoelectricity in quasi-two-dimensional materials

Lu, Xue-Zeng; Zhang, Hui-Min; Zhou, Ying; Zhu, Tong; Xiang, Hongjun; Dong, Shuai; Kageyama, Hiroshi; Rondinelli, James M.

doi:10.1126/sciadv.adi0138

Out-of-plane ferroelectricity and robust magnetoelectricity in quasi-two-dimensional materials

Journal Article · Tue Nov 21 23:00:00 EST 2023 · Science Advances

DOI:https://doi.org/10.1126/sciadv.adi0138· OSTI ID:2471906

^[1]; ^[2]; ^[2]; Zhu, Tong ^[3]; ^[4]; ^[2]; ^[3]; ^[5]

Southeast University, Nanjing (China); Northwestern Univ., Evanston, IL (United States)
Southeast University, Nanjing (China)
Kyoto University (Japan)
Fudan University, Shanghai (China); Shanghai Qi Zhi Institute (China)
Northwestern University, Evanston, IL (United States)

Thin-film ferroelectrics have been pursued for capacitive and nonvolatile memory devices. They rely on polarizations that are oriented in an out-of-plane direction to facilitate integration and addressability with complementary metal-oxide semiconductor architectures. The internal depolarization field, however, formed by surface charges can suppress the out-of-plane polarization in ultrathin ferroelectric films that could otherwise exhibit lower coercive fields and operate with lower power. Here, we unveil stabilization of a polar longitudinal optical (LO) mode in the n = 2 Ruddlesden–Popper family that produces out-of-plane ferroelectricity, persists under open-circuit boundary conditions, and is distinct from hyperferroelectricity. Our first-principles calculations show the stabilization of the LO mode is ubiquitous in chalcogenides and halides and relies on anharmonic trilinear mode coupling. We further show that the out-of-plane ferroelectricity can be predicted with a crystallographic tolerance factor, and we use these insights to design a room-temperature multiferroic with strong magnetoelectric coupling suitable for magneto-electric spin-orbit transistors.

View Accepted Manuscript (DOE)

Research Organization:: Kansas State University, Manhattan, KS (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); Defense Advanced Research Projects Agency (DARPA); National Science Foundation (NSF); Japan Society for the Promotion of Science (JSPS)

Grant/Contract Number:: FG02-86ER13491; AC02-06CH11357

OSTI ID:: 2471906

Journal Information:: Science Advances, Journal Name: Science Advances Journal Issue: 47 Vol. 9; ISSN 2375-2548

Publisher:: AAASCopyright Statement

Country of Publication:: United States

Language:: English

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