Tunable quadruple-well ferroelectric van der Waals crystals
Abstract
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.
- Authors:
-
[2];
[4];
[2];
[2];
[2];
[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)
- Publication Date:
- Research Org.:
- Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES); Air Force Research Laboratory (AFRL); National Research Council (NRC)
- OSTI Identifier:
- 1606851
- Grant/Contract Number:
- AC05-00OR22725; AC02-05CH11231; FG02-09ER46554; 14RQ08COR
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Nature Materials
- Additional Journal Information:
- Journal Volume: 19; Journal Issue: 1; Journal ID: ISSN 1476-1122
- Publisher:
- Springer Nature - Nature Publishing Group
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 36 MATERIALS SCIENCE; density functional theory; thiophosphates; CuInP2S6; van-der-Waals; negative piezoelectric coefficient; polarization; piezoresponse force microscopy
Citation Formats
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, and Balke, Nina. Tunable quadruple-well ferroelectric van der Waals crystals. United States: N. p., 2019.
Web. doi:10.1038/s41563-019-0532-z.
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. Tunable quadruple-well ferroelectric van der Waals crystals. United States. https://doi.org/10.1038/s41563-019-0532-z
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, and Balke, Nina. Mon .
"Tunable quadruple-well ferroelectric van der Waals crystals". United States. https://doi.org/10.1038/s41563-019-0532-z. https://www.osti.gov/servlets/purl/1606851.
@article{osti_1606851,
title = {Tunable quadruple-well ferroelectric van der Waals crystals},
author = {Brehm, John A. and Neumayer, Sabine M. and Tao, Lei and O’Hara, Andrew and Chyasnavichus, Marius and Susner, Michael A. and McGuire, Michael A. and Kalinin, Sergei V. and Jesse, Stephen and Ganesh, Panchapakesan and Pantelides, Sokrates T. and Maksymovych, Petro and Balke, Nina},
abstractNote = {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.},
doi = {10.1038/s41563-019-0532-z},
journal = {Nature Materials},
number = 1,
volume = 19,
place = {United States},
year = {Mon Nov 18 00:00:00 EST 2019},
month = {Mon Nov 18 00:00:00 EST 2019}
}
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