Hybrid Materials: Still Challenging for Ab Initio Theory?

Abstract

Hybrid inorganic/organic systems (HIOS) open new avenues for tailoring them with respect to desired features and functions by exploiting the respective advantages of their components. Therefore, these materials are actively explored in many experimental studies and devices. On the theory side, similar investigations are rather scarce as such interfaces, in addition to exhibiting large unit cells, require highest‐level theories to be described reliably. Consequently, hybrid materials pose a challenge for electronic structure theory, starting from density‐functional theory to methods beyond, particularly many‐body perturbation theory. This concerns both conceptual aspects and computational bottlenecks. In this perspective, the performance of state‐of‐the‐art theoretical approaches applied to HIOS is summarized, mainly focusing on optoelectronic properties. Recent achievements, open challenges, and urgent needs are addressed.