Open-shell nature of molecules are origins of their unique characters, and the characters result in the molecular functions. In the materials, the molecules are interacted with so many solids, and the functions will be varied by the solid surfaces. The varied functions are applied to catalysts, fuel cells, magnets, batteries, and so on (Fig. 1). However, the theoretical investigations on the interfaces between solids and open-shell molecules are difficult, and we have not fully understood the interactions. The deepening our understanding of the solid-molecule interactions will therefore unveil a roadmap for reaching brand-new materials.
The reason why the theoretical investigation of solid/molecule interfaces is difficult is simple: solid/molecule interfaces are also physics/chemistry interfaces. For molecules, we investigate them using chemistry such as molecular orbital calculations, and this approach show high accuracy for isolated systems. However, the computational cost is too high to apply it to periodic systems. On the other hand, using physics, we can investigate the solid systems. Band calculation by density functional theory with plane-wave basis (DFT/plane-wave) is a high-throughput approach for periodic systems, but it is difficult to apply it to open-shell molecules due to the lack of correction and analysis scheme. Therefore, theoretical development was necessary to handle the systems with solid/open-shell molecule interfaces.
My challenge is that the band calculation results are analysed and corrected using techniques of quantum chemistry. Namely, when investigating the solid/molecule interfaces, the results by physics are discussed within knowledge of chemistry. To achieve it, I developed spin projection schemes, which are methods for correction and analysis of open-shell molecules in quantum chemistry, for DFT/plane-wave method [1-20]. The developed scheme has opened diradical chemistry and physics on solid-molecule interfaces. I will present the essence of theoretical development, some of applications, and remained issues to achieve ab initio data-driven science for complexes of solid and open-shell molecules.
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