Short-Range Order Tunes Optical Properties in Long-Range Disordered ZnSnN2–ZnO Alloy

Local site ordering offers a new paradigm for property control in functional materials. However, systems that exhibit a propensity for local order and global disorder are often challenging to characterize, and demonstrations of ordering-induced property tuning are few and far between. Here, we demon...

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Bibliographic Details
Published in:Chemistry of materials 2022-05, Vol.34 (9), p.3910-3919
Main Authors: Melamed, Celeste L., Miller, Moira K., Cordell, Jacob, Pucurimay, Linda, Livingood, Alyssa, Schnepf, Rekha R., Pan, Jie, Heinselman, Karen N., Vila, Fernando D., Mis, Allison, Nordlund, Dennis, Levy-Wendt, Ben, Lany, Stephan, Toberer, Eric S., Christensen, Steven T., Tamboli, Adele C.
Format: Article
Language:English
Subjects:
Absorption,Alloys
Chemical structure
CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSICS,MATERIALS SCIENCE
Diseases and disorders
functional materials
INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
local site ordering
MATERIALS SCIENCE
optical absorption
Oxides
semiconductor
short-range ordering
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Summary:Local site ordering offers a new paradigm for property control in functional materials. However, systems that exhibit a propensity for local order and global disorder are often challenging to characterize, and demonstrations of ordering-induced property tuning are few and far between. Here, we demonstrate that short-range ordering tunes the optical absorption edge in the long-range disordered alloy system (ZnSnN2)1–x (ZnO)2x at x = 0.25. We use combinatorial cosputtering to synthesize a set of thin-film samples spanning this alloy space. X-ray diffraction demonstrates lattice contraction as a function of alloy composition, confirming that a mixed-anion and -cation alloy has been synthesized. Using N and O K-edge X-ray absorption near-edge structure in conjunction with simulations of cation-disordered supercell structures, we find that samples exhibit octet-rule-breaking motifs around both anions. Upon annealing at an alloy composition of x = 0.25, X-ray absorption analysis suggests that local motif structure shifts toward octet-rule-conserving while long-range disorder is maintained. Spectroscopic ellipsometry reveals that local ordering increases the absorption edge energy at constant composition. Additionally, alloy-induced optical absorption edge tuning is demonstrated. This work paves the way toward property tuning with short-range ordering in (ZnSnN2)1–x (ZnO)2x and beyond.
ISSN:0897-4756
1520-5002
DOI:10.1021/acs.chemmater.1c03938