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arXiv 2512.02168cond-mat.mtrl-sci
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硫化物薄膜通过混合脉冲激光沉积法生长中碳掺杂的评估

Evaluation of carbon incorporation in sulfide thin films grown by hybrid pulsed laser deposition

University of Southern California(南加州大学);National Institute of Standards and Technology(美国国家标准与技术研究院)

Claire Wu, Mythili Surendran, Shin Muramoto, Alexander Grutter, Jayakanth Ravichandran

AI总结:

研究通过混合脉冲激光沉积法评估硫化物薄膜中碳掺杂的影响,发现最佳生长温度和TBDS压力可显著减少碳污染。

摘要:

压力不匹配的材料,如过渡金属硫化物,已逐渐成为电子、光子和量子材料的关键组成部分。混合脉冲激光沉积法(hPLD)已成为这些材料的优选方法,用于获得镜面或纹理生长;然而,非故意的碳(C)掺杂仍然是一个持续的问题,特别是在使用有机硫前驱体作为更安全的替代品以取代有毒的氢化物时。控制C掺杂机制及其对hPLD中薄膜生长和性质的影响仍不明确。在这里,我们研究了由有机硫前驱体热解产生的含C副产物对通过hPLD用叔丁基二硫化物(TBDS)生长的ZnS、BaTiS3和TiS2薄膜的影响。通过X射线衍射和原子力显微镜结合二次离子质谱,系统地检查了生长温度和TBDS分压对薄膜形态、结晶度和C掺杂的影响。ZnS、TiS2和BaTiS3分别在400°C、500°C和700°C的最佳生长温度下被识别。生长在这些温度之上或之下会导致界面和薄膜内部的C掺杂增加,与纹理退化相关。相比之下,高度纹理化的薄膜表现出最低的C含量,与不使用TBDS生长的薄膜相当。对于TiS2,C掺杂强烈依赖于TBDS压力,10^-1 Pa被确定为最小污染的最佳压力。在更高的压力下,观察到纹理的丧失,可能是由于C石墨化毒化了界面和体材料。这些结果为hPLD生长硫化物薄膜中的过程诱导C杂质提供了新的见解,并对硫化物基薄膜技术具有重要的意义。

英文摘要:

Vapor-pressure-mismatched materials, such as transition metal chalcogenides, have emerged as key electronic, photonic, and quantum materials. Hybrid pulsed laser deposition (hPLD) has become a preferred method for epitaxial or textured growth of these materials; however, unintentional carbon (C) incorporation remains a persistent concern, particularly when using organic chalcogen precursors as safer alternatives to toxic hydrides. The mechanisms governing C incorporation and its impact on film growth and properties in hPLD remain poorly understood. Here, we investigate the influence of C-containing side products generated from organosulfur precursor pyrolysis on ZnS, BaTiS$_3$, and TiS$_2$ thin films grown by hPLD using tert-butyl disulfide (TBDS). Structural characterization via X-ray diffraction and atomic force microscopy, combined with secondary ion mass spectrometry, is used to systematically examine the effects of growth temperature and TBDS partial pressure on film morphology, crystallinity, and C incorporation. Optimal growth temperatures of 400°C, 500°C, and 700°C are identified for ZnS, TiS$_2$, and BaTiS$_3$, respectively. Growth above or below these temperatures leads to increased C incorporation at both the interface and within the film, correlating with degraded texture. In contrast, highly textured films exhibit minimal C content, comparable to films grown without TBDS. For TiS$_2$, C incorporation depends strongly on TBDS pressure, with 10$^{-1}$ Pa identified as the optimal pressure for minimizing contamination. At higher pressures, loss of preferential texture is observed, likely due to C graphitization poisoning the interface and bulk. These results provide new insight into process-induced C impurities in hPLD-grown chalcogenide thin films and have important implications for sulfide-based thin film technologies.

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