Subsystem density-functional theory: A reliable tool for spin-density based properties

Subsystem density-functional theory compiles a set of features that allow for efficiently calculating properties of very large open-shell radical systems such as organic radical crystals, proteins, or deoxyribonucleic acid stacks. It is computationally less costly than correlated ab initio wave function approaches and can pragmatically avoid the overdelocalization problem of Kohn-Sham density-functional theory without employing hard constraints on the electron-density. Additionally, subsystem density-functional theory calculations commonly start from isolated fragment electron densities, pragmatically preserving a priori specified subsystem spin-patterns throughout the calculation. Methods based on subsystem density-functional theory have seen a rapid development over the past years and have become important tools for describing open-shell properties. In this Perspective, we address open questions and possible developments toward challenging future applications in connection with subsystem density-functional theory for spin-dependent properties. Published under an exclusive license by AIP Publishing.

Automated summary

Subsystem density-functional theory is an efficient method for calculating properties of large open-shell radical systems. It is computationally less costly and avoids the problem of electron overdelocalization. This method has seen rapid development in recent years and has become an important tool for describing open-shell properties.