journal article·2023-04-11Open access

Combinatorial Synthesis of Cation-Disordered Manganese Tin Nitride MnSnN2 Thin Films with Magnetic and Semiconducting Properties

Christopher L. Rom, Rebecca W. Smaha, Celeste L. Melamed, Rekha R. Schnepf, Karen N. Heinselman, John S. Mangum, Sang-Jun Lee, Stephan Lany, Laura T. Schelhas, Ann L. Greenaway, James R. Neilson, Sage R. Bauers, Adele C. Tamboli, Jennifer S. Andrew

Chemistry of Materials· Volume 35· Issue 7

Abstract

High Resolution Image Download MS PowerPoint Slide Magnetic semiconductors may soon improve the energy efficiency of microelectronics, but materials exhibiting these dual properties remain underexplored. Here, we report the computational prediction and realization of a new magnetic and semiconducting material, MnSnN 2, via combinatorial sputtering of thin films. Grazing incidence wide-angle X-ray scattering and laboratory X-ray diffraction studies show MnSnN 2 exhibits a wurtzite-like crystal structure with cation disorder. This new material has a wide composition tolerance, with a single-phase region ranging from 20% < Mn/(Mn + Sn) < 65%. Spectroscopic ellipsometry identifies an optical absorption onset of 1 eV, consistent with the computationally predicted 1.2 eV bandgap. Resistivity measurements as a function of temperature support the semiconducting nature of MnSnN 2 . Hall effect measurements show carrier density has a weak inverse correlation with temperature, indicating that the charge transport mechanisms are more complex than in a pristine semiconductor. Magnetic susceptibility measurements reveal a low-temperature magnetic ordering transition (≈10 K) for MnSnN 2 and strong antiferromagnetic correlations. This finding contrasts with bulk, cation-ordered MnSiN 2 and MnGeN 2, which exhibited antiferromagnetic ordering above 400 K in previous studies. To probe the origin of this difference, we perform Monte Carlo simulations of cation-ordered and cation-disordered MnSnN 2 . They reveal that cation disorder lowers the magnetic transition temperature relative to the ordered phase. In addition to discovering a new compound, this work shows that future efforts could use cation (dis)order to tune magnetic transitions in semiconducting materials for precise control of properties in microelectronics.
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Research context

OpenAlex topics: Machine Learning in Materials Science · Metal and Thin Film Mechanics · Electronic and Structural Properties of Oxides

SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.

Affiliations

Department of Chemistry, Colorado State University, Fort Collins, Colorado 80523-1872, United States

National Renewable Energy Laboratory, Golden, Colorado 80401, United States

Physics Department, Colorado School of Mines, Golden, Colorado 80401, United States

Stanford Synchrotron Radiation Lightsource, SLAC National Accelerator Laboratory, Menlo Park, California 94025, United States

School of Advanced Materials Discovery, Colorado State University, Fort Collins, Colorado 80523-1872, United States

Department of Materials Science and Engineering, University of Florida, Gainesville, Florida 32611, United States

Funding

Basic Energy Sciences · National Renewable Energy Laboratory

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