Tunable quadruple-well ferroelectric van der Waals crystals

Brehm, John A.; Neumayer, Sabine M.; Tao, Lei; O’Hara, Andrew; Chyasnavichus, Marius; Susner, Michael A.; McGuire, Michael A.; Kalinin, Sergei V.; Jesse, Stephen; Ganesh, Panchapakesan; Pantelides, Sokrates T.; Maksymovych, Petro; Balke, Nina

doi:10.1038/s41563-019-0532-z

Title: Tunable quadruple-well ferroelectric van der Waals crystals

Journal Article · Mon Nov 18 00:00:00 EST 2019 · Nature Materials

DOI:https://doi.org/10.1038/s41563-019-0532-z· OSTI ID:1606851

Brehm, John A. ^[1];

^[2]; Tao, Lei ^[3];

^[4]; Chyasnavichus, Marius ^[2]; Susner, Michael A. ^[5];

^[2];

^[1];

^[2];

^[2]

Vanderbilt Univ., Nashville, TN (United States); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Vanderbilt Univ., Nashville, TN (United States); Chinese Academy of Sciences (CAS), Beijing (China)
Vanderbilt Univ., Nashville, TN (United States)
Air Force Research Lab., Wright-Patterson Air Force Base, OH (United States)

The family of layered thio- and seleno-phosphates has gained attention as potential control dielectrics for the rapidly growing family of two-dimensional and quasi-two-dimensional electronic materials. Here we report a combination of density functional theory calculations, quantum molecular dynamics simulations and variable-temperature, -pressure and -bias piezoresponse force microscopy data to predict and verify the existence of an unusual ferroelectric property—a uniaxial quadruple potential well for Cu displacements—enabled by the van der Waals gap in copper indium thiophosphate (CuInP₂S₆). The calculated potential energy landscape for Cu displacements is strongly influenced by strain, accounting for the origin of the negative piezoelectric coefficient and rendering CuInP₂S₆ a rare example of a uniaxial multi-well ferroelectric. Experimental data verify the coexistence of four polarization states and explore the temperature-, pressure- and bias-dependent piezoelectric and ferroelectric properties, which are supported by bias-dependent molecular dynamics simulations. As a result, these phenomena offer new opportunities for both fundamental studies and applications in data storage and electronics.

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Research Organization:: Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); Air Force Research Laboratory (AFRL); National Research Council (NRC)

Grant/Contract Number:: AC05-00OR22725; AC02-05CH11231; FG02-09ER46554; 14RQ08COR

OSTI ID:: 1606851

Journal Information:: Nature Materials, Vol. 19, Issue 1; ISSN 1476-1122

Publisher:: Springer Nature - Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 87 works

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Title: Tunable quadruple-well ferroelectric van der Waals crystals

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