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Atomic layer deposition of cubic tin–calcium sulfide alloy films

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Abstract

We deposit films of tin–calcium sulfide by atomic layer deposition (ALD) and demonstrate the metastability of this material. Rough and spiky films are obtained by using Sn and Ca precursors with different ligands, whereas compact and smooth films are obtained when the two metal sources share the same ligands. Compositional and quartz crystal microbalance results indicate that part of the underlaying SnS film is replaced and/or removed during the CaS ALD cycle during the ternary film deposition, possibly via a temperature-dependent cation exchange mechanism. The crystal structure transforms from orthorhombic to cubic as the calcium content increases. Furthermore, resistivity increases with calcium content in the alloy films, whereas optical band gap only depends weakly on Ca content. After annealing at 400 °C in an H2S environment, the cubic alloy film undergoes a phase transition into the orthorhombic phase and its resistivity also decreases. Both phenomena could be explained by phase separation of the metastable alloy.

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Acknowledgments

This research was supported in part by the Center for the Next Generation of Materials by Design, an Energy Frontier Research Center funded by the U.S. DOE, Office of Science. Part of the work was performed at the Center for Nanoscale Systems (CNS) at Harvard University, a member of the National Nanotechnology Infrastructure Network (NNIN), which is supported by the National Science Foundation under NSF award no. ECS-0335765. Use of the SSRL, SLAC National Accelerator Laboratory, was supported by the U.S. Department of Energy, Office of Basic Energy Sciences under Contract No. DE-AC02-76SF00515.

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Authors and Affiliations

  1. Department of Chemistry, Harvard University, Cambridge, Massachusetts, 02138, USA

    Chuanxi Yang, Xizhu Zhao, Sang Bok Kim, Xiabing Lou & Roy G. Gordon

  2. Stanford Synchrotron Radiation Lightsource, SLAC National Accelerator Laboratory, Menlo Park, California, 94025, USA

    Laura T. Schelhas

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  1. Chuanxi Yang
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Correspondence to Roy G. Gordon.

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Yang, C., Zhao, X., Kim, S.B. et al. Atomic layer deposition of cubic tin–calcium sulfide alloy films. Journal of Materials Research 35, 795–803 (2020). https://doi.org/10.1557/jmr.2019.337

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