Novel phase diagram behavior and materials design in heterostructural semiconductor alloys

Holder, Aaron M.; Siol, Sebastian; Ndione, Paul F.; Peng, Haowei; Deml, Ann M.; Matthews, Bethany E.; Schelhas, Laura T.; Toney, Michael F.; Gordon, Roy G.; Tumas, William; Perkins, John D.; Ginley, David S.; Gorman, Brian P.; Tate, Janet; Zakutayev, Andriy; Lany, Stephan

doi:10.1126/sciadv.1700270

Cited by 52 publications

(63 citation statements)

References 36 publications

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“…Alloys of materials having different crystal structures in their pure forms (heterostructural alloys) provide enhanced opportunities for accessing nonequilibrium states and otherwise inaccessible properties [1]. The Al 1−x Sc x N system is an interesting case study in heterostructural alloying as a tool for property improvement.…”

Section: Introductionmentioning

confidence: 99%

Implications of heterostructural alloying for enhanced piezoelectric performance of (Al,Sc)N

Talley

Millican

Mangum

et al. 2018

Phys. Rev. Materials

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An understanding of the heterostructural implications on alloying in the aluminum nitride-scandium nitride system (Al 1−x Sc x N) can highlight opportunities and design principles for enhancing desired material properties by leveraging nonequilibrium states. The fundamental thermodynamics, and therefore composition-and structuredependent 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 Al 1−x Sc x 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 Al 1−x Sc x N system, suggests material design strategies for even greater property enhancements, and demonstrates the increased property tunability and underexplored nature of nonequilibrium heterostructural alloys.

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Section: Introductionmentioning

confidence: 99%

Implications of heterostructural alloying for enhanced piezoelectric performance of (Al,Sc)N

Talley

Millican

Mangum

et al. 2018

Phys. Rev. Materials

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“…Hence, a semilocal functional, such as PBE, with proper SIC and vdWC, may improve the polymorphism energetics for TM oxides. This would facilitate material design based on heterostructural alloys [31] as in the recent tetrahedral Mn 1−x Zn x O alloy (x ∼ 0.5) for water splitting [32], where the accurate ∆E ZB/RS of MnO was critical during the computational design.…”

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confidence: 99%

Synergy of van der Waals and self-interaction corrections in transition metal monoxides

Peng

Perdew

2017

Phys. Rev. B

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“…While high-throughput techniques are commonly used in other areas of materials science (i.e. novel materials for thin lm PV [23][24][25][26] or materials by design 27,28 ) such combinatorial approaches are rather uncommon in TE research. 29,30 Combinatorial thin lm deposition was performed using radio frequency (RF) magnetron cosputtering from multiple targets leading to composition gradients along the substrate, and resulting in combinatorial sample libraries (see Fig.…”

Section: Combinatorial Screeningmentioning

confidence: 99%

Solubility limits in quaternary SnTe-based alloys

et al. 2017

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The controlled decomposition of metastable alloys is an attractive route to form nanostructured thermoelectric materials with reduced thermal conductivity. The ternary SnTe-MnTe and SnTe-SnSe heterostructural alloys have been demonstrated as promising materials for thermoelectric applications.In this work, the quaternary Sn 1Ày Mn y Te 1Àx Se x phase space serves as a relevant model system to explore how a combination of computational and combinatorial-growth methods can be used to study equilibrium and non-equilibrium solubility limits. Results from first principle calculations indicate low equilibrium solubility for x,y < 0.05 that are in good agreement with results obtained from bulk equilibrium synthesis experiments and predict significantly higher spinodal limits. An experimental screening using sputtered combinatorial thin film sample libraries showed a remarkable increase in nonequilibrium solubility for x,y > 0.2. These theoretical and experimental results were used to guide the bulk synthesis of metastable alloys. The ability to reproduce the non-equilibrium solubility levels in bulk materials indicates that such theoretical calculations and combinatorial growth can inform bulk synthetic routes. Further, the large difference between equilibrium and non-equilibrium solubility limits in Sn 1Ày Mn y Te 1Àx Se x indicates these metastable alloys are attractive in terms of nano-precipitate formation for potential thermoelectric applications.

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Novel phase diagram behavior and materials design in heterostructural semiconductor alloys

Abstract: Theoretically predicted metastable phases are realized in thin-film synthesis of Mn1−xZnxO and Sn1−xCaxS alloys.

Cited by 52 publications

References 36 publications

Implications of heterostructural alloying for enhanced piezoelectric performance of (Al,Sc)N

Implications of heterostructural alloying for enhanced piezoelectric performance of (Al,Sc)N

Synergy of van der Waals and self-interaction corrections in transition metal monoxides

Solubility limits in quaternary SnTe-based alloys

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