Chemistry of Ammonothermal Synthesis and Novel Nitrides

该合作项目的主要目标是从选定的案例研究开始，对氮化物的氨合成过程进行基本了解，并利用这些知识合理合成新型氮化物材料。为了实现这一目标，我们希望采用合成化学，溶液中的光谱研究（特别关注NMR光谱学）和分子模拟（包括分子力学和量子方法）的相互作用，这将通过申请人小组之间的密切合作来实现，每个小组都专注于一个子学科。 一个更合理的方法，以过程优化的基本先决条件是获得一个详细的原子理解的化学反应途径涉及氨合成。为了实现这一目标，我们将分离出关键的反应中间体，并通过适当的实验技术对其进行表征，包括固体和在液氨中重新溶解后。与那些的起始材料和产品，以及在量子化学和QM/MM分子动力学研究的光的签名和它们的变化的解释所获得的光谱签名的比较，使溶解的物种的形态和反应途径的跟踪。最终，所获得的知识将能够直接合成新型氮化锌，被确定为具有高潜力的电子和光电器件的相关目标材料。

The main objective of this collaborative project is to develop a fundamental understanding of the processes during ammonothermal synthesis of nitrides starting from selected case studies and reaching out to using this knowledge for the rational synthesis of novel nitride materials. To achieve this goal, we want to employ an interplay of synthetic chemistry, spectroscopic investigations in solution (with special focus on NMR spectroscopy), and molecular simulations (encompassing molecular mechanics and quantum approaches) that will be implemented through a close collaboration between the applicants' groups, each specialized in one of the sub-disciplines. An essential prerequisite for a more rational approach to process optimization is obtaining a detailed atomistic understanding of the chemical reaction pathways involved in ammonothermal syntheses. To approach this goal, we will isolate key reaction intermediates and characterize them by suitable experimental techniques both as solids and after re-dissolution in liquid ammonia. Comparison of the spectral signatures obtained with those of starting materials and products as well as interpretation of the signatures and their changes in the light of quantum chemical and QM/MM molecular dynamics studies enables both speciation of dissolved species and tracing of reaction pathways. Eventually, the knowledge gained shall enable a directed synthesis of novel zinc nitrides, identified as relevant target materials with high potential for electronic and optoelectronic devices.