One-step sputtering of MoSSe metastable phase as thin film and predicted thermodynamic stability by computational methods

采用一步溅射法制备亚稳态MoSSe薄膜,并通过计算方法预测其热力学稳定性

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Abstract

We present the fabrication of a MoS(2-x)Se(x) thin film from a co-sputtering process using MoS(2) and MoSe(2) commercial targets with 99.9% purity. The sputtering of the MoS(2) and MoSe(2) was carried out using a straight and low-cost magnetron radio frequency sputtering recipe to achieve a MoS(2-x)Se(x) phase with x = 1 and sharp interface formation as confirmed by Raman spectroscopy, time-of-flight secondary ion mass spectroscopy, and cross-sectional scanning electron microscopy. The sulfur and selenium atoms prefer to distribute randomly at the octahedral geometry of molybdenum inside the MoS(2-x)Se(x) thin film, indicated by a blue shift in the A(1g) and E(1)(g) vibrational modes at 355 cm(-1) and 255 cm(-1), respectively. This work is complemented by computing the thermodynamic stability of a MoS(2-x)Se(x) phase whereby density functional theory up to a maximum selenium concentration of 33.33 at.% in both a Janus-like and random distribution. Although the Janus-like and the random structures are in the same metastable state, the Janus-like structure is hindered by an energy barrier below selenium concentrations of 8 at.%. This research highlights the potential of transition metal dichalcogenides in mixed phases and the need for further exploration employing low-energy, large-scale methods to improve the materials' fabrication and target latent applications of such structures.

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