Simons Jasmin, Steinberg Simon
Institute of Inorganic Chemistry, RWTH Aachen University, Landoltweg 1, D-52074 Aachen, Germany.
ACS Omega. 2019 Sep 13;4(13):15721-15728. doi: 10.1021/acsomega.9b02368. eCollection 2019 Sep 24.
The tailored (computational) design of materials addressing future challenges requires a thorough understanding of their electronic structures. This becomes very apparent for a given material existing in a certain homogeneity range, as its particular composition influences its electronic structure and, eventually, its physical properties. This led us to explore the influence and, furthermore, the origin of vacancies in the crystal structures of rock salt-type superconductors by means of quantum-chemical techniques. In doing so, we examined the vibrational properties, electronic band structures, and nature of bonding for a series of superconducting transition-metal sulfides, i.e., MS (M = Sc, Y, Zr, Lu), which were identified to exist over certain homogeneity ranges. The outcome of our research indicates that the subtle competing interplay between two electronically unfavorable situations at the Fermi levels, i.e., the occupations of flat bands and the populations of antibonding states, appears to control the presence of vacancies in the crystal structures of the sulfides.
针对未来挑战的材料定制（计算）设计需要对其电子结构有透彻的理解。对于存在于特定均匀性范围内的给定材料，这一点变得非常明显，因为其特定组成会影响其电子结构，并最终影响其物理性质。这促使我们借助量子化学技术探索岩盐型超导体晶体结构中空位的影响及其起源。在此过程中，我们研究了一系列超导过渡金属硫化物，即MS（M = Sc、Y、Zr、Lu）的振动性质、电子能带结构和键合性质，这些硫化物被确定存在于特定的均匀性范围内。我们的研究结果表明，在费米能级处两种电子不利情况之间微妙的竞争相互作用，即平带的占据和反键态的填充，似乎控制着硫化物晶体结构中空位的存在。
