Implications of heterostructural alloying for enhanced piezoelectric performance of (Al,Sc)N
Abstract
An understanding of the heterostructural implications on alloying in the aluminum nitride-scandium nitride system ($${\mathrm{Al}}_{1{-}x}{\mathrm{Sc}}_{x}\mathrm{N}$$) can highlight opportunities and design principles for enhancing desired material properties by leveraging nonequilibrium states. The fundamental thermodynamics, and therefore composition- and structure-dependent mechanisms, underlying property evolution in this system have not been fully described, despite significant recent efforts driven by interest in enhanced piezoelectric performance. Practical realization of these enhanced properties, however, is hindered by the strong driving thermodynamic driving force for phase separation in the system, highlighting the need for increased study into the role of heterostructural alloying on the thermodynamics and composition-structure-property relationships in this system. With this need in mind, ab initio computed alloy thermodynamics and properties are compared to combinatorial thin-film synthesis and characterization to develop a more complete picture of the structure and property evolution across the $${\mathrm{Al}}_{1{-}x}{\mathrm{Sc}}_{x}\mathrm{N}$$ composition space. The combination of structural frustration and a flattened free-energy landscape lead to substantial increases in electromechanical response. The energy scale of alloy metastability is found to be much larger than previously reported, helping to explain difficulties in achieving homogeneous materials with high scandium concentration. Scandium substitution for aluminum softens the wurtzite crystal lattice, and energetic proximity to the competing hexagonal boron-nitride structure enhances the piezoelectric stress coefficient. Overall, this work provides insight into the understanding of the structure-processing-property relationships in the $${\mathrm{Al}}_{1{-}x}{\mathrm{Sc}}_{x}\mathrm{N}$$ system, suggests material design strategies for even greater property enhancements, and demonstrates the increased property tunability and underexplored nature of nonequilibrium heterostructural alloys.
- Authors:
- Publication Date:
- Research Org.:
- Energy Frontier Research Centers (EFRC) (United States). Center for Next Generation of Materials by Design: Incorporating Metastability (CNGMD); National Renewable Energy Laboratory (NREL), Golden, CO (United States); Colorado School of Mines, Golden, CO (United States); Univ. of Colorado, Boulder, CO (United States)
- Sponsoring Org.:
- USDOE Office of Energy Efficiency and Renewable Energy (EERE); USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF)
- OSTI Identifier:
- 1457812
- Alternate Identifier(s):
- OSTI ID: 1462331
- Report Number(s):
- NREL/JA-5K00-71970
Journal ID: ISSN 2475-9953; PRMHAR; 063802
- Grant/Contract Number:
- AC36-08GO28308; DMREF-1534503; CBET-1433521
- Resource Type:
- Published Article
- Journal Name:
- Physical Review Materials
- Additional Journal Information:
- Journal Name: Physical Review Materials Journal Volume: 2 Journal Issue: 6; Journal ID: ISSN 2475-9953
- Publisher:
- American Physical Society (APS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 36 MATERIALS SCIENCE; dielectric properties; elastic modulus; phase diagrams; piezoelectricity; spinodal decomposition
Citation Formats
Talley, Kevin R., Millican, Samantha L., Mangum, John, Siol, Sebastian, Musgrave, Charles B., Gorman, Brian, Holder, Aaron M., Zakutayev, Andriy, and Brennecka, Geoff L. Implications of heterostructural alloying for enhanced piezoelectric performance of (Al,Sc)N. United States: N. p., 2018.
Web. doi:10.1103/PhysRevMaterials.2.063802.
Talley, Kevin R., Millican, Samantha L., Mangum, John, Siol, Sebastian, Musgrave, Charles B., Gorman, Brian, Holder, Aaron M., Zakutayev, Andriy, & Brennecka, Geoff L. Implications of heterostructural alloying for enhanced piezoelectric performance of (Al,Sc)N. United States. https://doi.org/10.1103/PhysRevMaterials.2.063802
Talley, Kevin R., Millican, Samantha L., Mangum, John, Siol, Sebastian, Musgrave, Charles B., Gorman, Brian, Holder, Aaron M., Zakutayev, Andriy, and Brennecka, Geoff L. Fri .
"Implications of heterostructural alloying for enhanced piezoelectric performance of (Al,Sc)N". United States. https://doi.org/10.1103/PhysRevMaterials.2.063802.
@article{osti_1457812,
title = {Implications of heterostructural alloying for enhanced piezoelectric performance of (Al,Sc)N},
author = {Talley, Kevin R. and Millican, Samantha L. and Mangum, John and Siol, Sebastian and Musgrave, Charles B. and Gorman, Brian and Holder, Aaron M. and Zakutayev, Andriy and Brennecka, Geoff L.},
abstractNote = {An understanding of the heterostructural implications on alloying in the aluminum nitride-scandium nitride system (${\mathrm{Al}}_{1{-}x}{\mathrm{Sc}}_{x}\mathrm{N}$) can highlight opportunities and design principles for enhancing desired material properties by leveraging nonequilibrium states. The fundamental thermodynamics, and therefore composition- and structure-dependent mechanisms, underlying property evolution in this system have not been fully described, despite significant recent efforts driven by interest in enhanced piezoelectric performance. Practical realization of these enhanced properties, however, is hindered by the strong driving thermodynamic driving force for phase separation in the system, highlighting the need for increased study into the role of heterostructural alloying on the thermodynamics and composition-structure-property relationships in this system. With this need in mind, ab initio computed alloy thermodynamics and properties are compared to combinatorial thin-film synthesis and characterization to develop a more complete picture of the structure and property evolution across the ${\mathrm{Al}}_{1{-}x}{\mathrm{Sc}}_{x}\mathrm{N}$ composition space. The combination of structural frustration and a flattened free-energy landscape lead to substantial increases in electromechanical response. The energy scale of alloy metastability is found to be much larger than previously reported, helping to explain difficulties in achieving homogeneous materials with high scandium concentration. Scandium substitution for aluminum softens the wurtzite crystal lattice, and energetic proximity to the competing hexagonal boron-nitride structure enhances the piezoelectric stress coefficient. Overall, this work provides insight into the understanding of the structure-processing-property relationships in the ${\mathrm{Al}}_{1{-}x}{\mathrm{Sc}}_{x}\mathrm{N}$ system, suggests material design strategies for even greater property enhancements, and demonstrates the increased property tunability and underexplored nature of nonequilibrium heterostructural alloys.},
doi = {10.1103/PhysRevMaterials.2.063802},
journal = {Physical Review Materials},
number = 6,
volume = 2,
place = {United States},
year = {Fri Jun 29 00:00:00 EDT 2018},
month = {Fri Jun 29 00:00:00 EDT 2018}
}
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