Abstract
Developing novel lead-free ferroelectric materials is crucial for next-generation microelectronic technologies that are energy efficient and environment friendly. However, materials discovery and property optimization are typically time-consuming due to the limited throughput of traditional synthesis methods. In this work, we use a high-throughput combinatorial synthesis approach to fabricate lead-free ferroelectric superlattices and solid solutions of (Ba0.7Ca0.3)TiO3 (BCT) and Ba(Zr0.2Ti0.8)O3 (BZT) phases with continuous variation of composition and layer thickness. High-resolution x-ray diffraction (XRD) and analytical scanning transmission electron microscopy (STEM) demonstrate high film quality and well-controlled compositional gradients. Ferroelectric and dielectric property measurements identify the “optimal property point” achieved at the composition of 48BZT–52BCT. Displacement vector maps reveal that ferroelectric domain sizes are tunable by varying {BCT–BZT}N superlattice geometry. This high-throughput synthesis approach can be applied to many other material systems to expedite new materials discovery and properties optimization, allowing for the exploration of a large area of phase space within a single growth. (Figure presented.).
| Original language | English |
|---|---|
| Article number | e12561 |
| Journal | InfoMat |
| Volume | 6 |
| Issue number | 9 |
| DOIs | |
| State | Published - Sep 2024 |
Funding
We thank Dr. Kazuo Ishizuka from HREM Inc. for the helpful discussions on using SmartAlign plug\u2010in in DM for the drift\u2010correction work of HAADF\u2010STEM images. The work at Los Alamos National Laboratory was supported by the NNSA's Laboratory Directed Research and Development (LDRD) Program, and was performed, in part, at the Center for Integrated Nanotechnologies, an Office of Science User Facility operated for the U.S. Department of Energy (DOE) Office of Science by Los Alamos National Laboratory (contract 89233218CNA000001) and Sandia National Laboratories (contract DE\u2010NA0003525). Los Alamos National Laboratory, an affirmative action equal opportunity employer, is managed by Triad National Security, LLC for the U.S. Department of Energy's NNSA, under Contract No. 89233218CNA000001. Sandia National Laboratories is a multiprogram laboratory managed and operated by National Technology and Engineering Solutions of Sandia, LLC, a wholly owned subsidiary of Honeywell International, Inc., for the U.S. Department of Energy's National Nuclear Security Administration under contract DE\u2010NA0003525. This paper describes objective technical results and analysis. Any subjective views or opinions that might be expressed in the paper do not necessarily represent the views of the U.S. Department of Energy or the United States Government. The synchrotron x\u2010ray diffraction measurements done at Argonne National Laboratory was supported by the U.S. Department of Energy, Office of Science, Basic Energy Sciences, Materials Science and Engineering Division, and the XRD data analysis was based on work supported by Laboratory Directed Research and Development (LDRD) funding from Argonne National Laboratory, provided by the Director, Office of Science, of the U.S. Department of Energy and by the U.S. DOE Office of Science\u2010Basic Energy Sciences under Contract No. DE\u2010AC02\u201006CH11357. This research used resources of the Advanced Photon Source, a U.S. Department of Energy (DOE) Office of Science user facility operated for the DOE Office of Science by Argonne National Laboratory under Contract No. DE\u2010AC02\u201006CH11357. The aberration\u2010corrected HAADF\u2010STEM portion of this research was supported by the Center for Nanophase Materials Sciences (CNMS), which is a US Department of Energy, Office of Science User Facility at Oak Ridge National Laboratory. The PFM measurements at Texas A&M University were supported by the National Science Foundation under the Award No. CMMI\u20102311573 and by the donors of the ACS Petroleum Research Fund under Doctoral New Investigator Grant 62603\u2010DNI10. Q.T. served as Principal Investigator on ACS 62603\u2010DNI10 that provided support for D.K.
Keywords
- ferroelectrics
- high-resolution x-ray diffraction
- high-throughput combinatorial synthesis
- pulsed laser deposition
- scanning transmission electron microscopy
- superlattices