Computing the Optical Properties of Large Systems

This work addresses the computation of excited-state properties of systems containing thousands of atoms. To achieve this, the author combines the linear response formulation of time-dependent density functional theory (TDDFT) with linear-scaling techniques known from ground-state density-functional theory. This extends the range of TDDFT, which on its own cannot tackle many of the large and interesting systems in materials science and computational biology. The strengths of the approach developed in this work are demonstrated on a number of problems involving large-scale systems, including exciton coupling in the Fenna-Matthews-Olson complex and the investigation of low-lying excitations in doped p-terphenyl organic crystals.

Nominated as an outstanding Ph.D. thesis by Imperial College London, UK Presents a full introduction to density-functional theory (DFT) and time-dependent DFT with a special focus on standard algorithms used in the community Provides an introduction to linear-scaling techniques, as well as a full derivation of a novel linear-scaling time-dependent DFT algorithm Includes an in-depth study of two systems of practical interest: the Fenna-Matthews-Olson complex and pentacene-derived molecular defects in p-terphenyl crystal Includes supplementary material: sn.pub/extras

Contenu
Introduction.- Theoretical background: Prerequisites.- Approximations to the ground state.- Approximations to excited states.- The ONETEP code.- Linear-scaling TDDFT in ONETEP.- Linear-scaling TDDFT within the PAW formalism.- Subsystem TDDFT.- Large-scale applications.- Conclusion and future work.