Development of the KMLYP density functional theory method, and application of quantum chemistry in modeling surface chemical reactions

The past few decades have seen dramatic improvements in our ability to simulate complicated chemical systems using quantum simulation. This has led to the concept of quantum simulations as a “third way” of doing science, closer to experiment than theory, but complimentary to both. Like experiments, quantum simulations produce data rather than theories, and the data that it provides are often impossible to obtain in any other way. However, challenges remain in applying quantum computational tools to extended systems. These challenges include: (a) accurate ab initio methods are still extremely computationally expensive for systems with more than 10 heavy atoms, (b) relatively efficient density functional theory (DFT) methods still do not have the accuracy to predict molecular properties of the extended systems with chemical accuracy (less than 1.4 kcal/mol of errors), and (c) there exists no framework for determining how to design a simulation for a given system due to the uncertainty arising from the various simulation choices made.; My research program is designed to meet these challenges by developing new methods and systematically designing simulation approaches to solving chemical reactions in extended systems with three main research areas: (a)  development of new simulation methods, (b) reactions on semiconductor surfaces, and (c) novel semiconductor processing. These areas reflect my interest in semiconductor processing, while also focusing on key issues confronting the semiconductor industry. My approach involves systematic application of quantum chemical methods to representative systems in order to uncover the underlying principles that govern the chemistry of each class. Furthermore, this systematic approach allows us to then apply these principles to design simulation approaches for classes of reactions which will greatly aid other scientists who wish to design efficient and accurate simulations to study reactions in analogous systems. In addition to establishing the framework for designing simulations, this work also allows us to improve the methods for studying reactive extended systems. With improved accuracy and simulation design principles researchers will be able to confidently use these methods to understand and design new processes without having to design a quantum chemical approach for their specific system.