Chemistry of Diamond Nucleation and Growth: Kinetic Measurement, Modeling, and Film Characterization via REMP/MSand Solid State NMR

金刚石薄膜由于其特殊的物理性质，具有许多潜在的技术应用。提高薄膜质量、沉积速率和均匀性是实现这一潜力的关键，这需要理解和控制金刚石的成核和生长。特别是，用于半导体器件的异质外延金刚石薄膜尚未实现。这是一种多方面的方法，包括实验测量和物种撞击生长表面的理论预测，结合表征和建模对于解开金刚石沉积化学的复杂性至关重要。pi计划发展对金刚石生长的机械理解，可用于设计结晶、高质量金刚石薄膜的设备和工艺。利用热丝反应器对金刚石生长的动力学机制进行了实验探索。利用分子束采样提取撞击加热晶圆表面的物质，利用共振增强多光子电离质谱（REMPI/MS）测量金刚石沉积的前驱体。气相浓度也将使用激光诱导荧光（LIF）和相干反斯托克斯拉曼光谱（CARS）进行测量。为了确定控制金刚石成核、生长和缺陷形成动力学的主要过程或步骤，将根据实验数据构建和测试化学和物理输运模型。金刚石薄膜的缺陷结构将采用碳13固态核磁共振（NMR）和传统技术进行测量。将分析核磁共振结果以确定缺陷的类型和数量，并将与传统技术（如拉曼散射）相关联，以将这些研究与文献中的其他研究联系起来。选择性碳13同位素标记将用于深入了解金刚石形成的动力学。利用扫描隧道显微镜（STM）对金刚石生长初期的核进行计数和测量，定量分析了金刚石生长的成核过程。器件将被制造和测试，其特性将与金刚石生长参数和薄膜表征相关。

Diamond thin films have numerous potential technological applications due to their extraordinary physical properties. Improvements in film quality, deposition rate, and uniformity are keys to the realization of this potential, requiring understanding and control of diamond nucleation and growth. In particular, heteroepitaxial diamond thin films for semiconductor devices have yet to be achieved. A multifaceted approach involving both experimental measurements and theoretical predictions of species impinging upon the growing surface, coupled with characterization and modeling is essential for unlocking the complexities of diamond deposition chemistry. The PIs plan to develop a mechanistic understanding of diamond growth which can be used for the design of equipment and processes for crystalline, high quality diamond thin films. The kinetic mechanisms of diamond growth will be experimentally probed using a hot-filament reactor. Using molecular beam sampling to extract the species striking the heated wafer surface, the precursors for diamond deposition will be measured using Resonancely Enhanced Multiphoton Ionization Mass Spectrometry (REMPI/MS). The gas phase concentrations will also be measured using Laser Induced Fluorescence (LIF) and Coherent, Anti-Stokes Raman Spectroscopy (CARS). Both chemical and physical transport models will be constructed and tested against the experimental data in order to identify the main processes or steps that control the kinetics of diamond nucleation, growth, and defect formation. The defect structures of diamond films will be measured using Carbon 13 solid state Nuclear Magnetic Resonance (NMR) as well as conventional techniques. The NMR results will be analyzed to identify the type and quantity of defects and will be correlated to conventional techniques such as Raman scattering to relate these studies to others in the literature. Selective Carbon 13 isotopic labeling will be used to gain insight into the kinetics of diamond formation. The nucleation of diamond growth will be quantified using Scanning Tunneling Microscopy (STM) to count and measure the nuclei during the initial phases of growth. Devices will be fabricated and tested, and their characteristics will be correlated with the diamond growth parameters and film characterization.