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

Christopher Rom, Rebecca Smaha, Celeste Melamed, Rekha Schnepf, Karen Heinselman, John Mangum, Sang-Jun Lee, Stephan Lany, Laura Schelhas, Ann Greenaway, James Neilson, Sage Bauers, Adele Tamboli, Jennifer Andrew

Research output: Contribution to journalArticlepeer-review

4 Scopus Citations

Abstract

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, MnSnN2, via combinatorial sputtering of thin films. Grazing incidence wide-angle X-ray scattering and laboratory X-ray diffraction studies show MnSnN2 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 MnSnN2. 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 MnSnN2 and strong antiferromagnetic correlations. This finding contrasts with bulk, cation-ordered MnSiN2 and MnGeN2, 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 MnSnN2. 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.

Original languageAmerican English
Pages (from-to)2936-2946
Number of pages11
JournalChemistry of Materials
Volume35
Issue number7
DOIs
StatePublished - 2023

Bibliographical note

Publisher Copyright:
© 2023 The Authors. Published by American Chemical Society.

NREL Publication Number

  • NREL/JA-5K00-84850

Keywords

  • diffraction
  • magnetism
  • manganese
  • nitride
  • semiconductor
  • thin film
  • tin

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