Complexity reduction in density functional theory: Locality in space and energy.

We present recent developments of the NTChem program for performing large scale hybrid density functional theory calculations on the supercomputer Fugaku. We combine these developments with our recently proposed complexity reduction framework to assess the impact of basis set and functional choice on its measures of fragment quality and interaction. We further exploit the all electron representation to study system fragmentation in various energy envelopes. Building off this analysis, we propose two algorithms for computing the orbital energies of the Kohn-Sham Hamiltonian. We demonstrate that these algorithms can efficiently be applied to systems composed of thousands of atoms and as an analysis tool that reveals the origin of spectral properties.

Thermal effect on the morphology and performance of organic photovoltaics.

The morphology of organic photovoltaics (OPVs) is a significant factor in improving performance, and establishing a method for controlling morphology is necessary. In this study, we propose a device-size simulation model, combining reptation and the dynamic Monte Carlo (DMC) algorithm, to investigate the relationship between the manufacturing process, morphology, and OPV performance. The reptation reproduces morphologies under thermal annealing, and DMC showed morphology-dependence of performance: not only short-circuit current density but also open-circuit voltage had optimal interfacial areas due to competition between exciton dissociation and charge collection. Besides, we performed transient absorption spectroscopy of various BHJ morphologies under realistic conditions, which revealed prompt and delayed dynamics of charge generation-the majority of the charges were from excitons that were generated on interfaces and dissociated within a few picoseconds, and the others from excitons that migrated to interfaces and dissociated on the order of sub-nanoseconds.