Photoabsorption spectra from adiabatically exact time-dependent density-functional theory in real time
文献信息
Mark Thiele, Stephan Kümmel
Photoabsorption spectra for 2-electron singlet systems are obtained from the real-time propagation of the time-dependent Kohn–Sham equations in the adiabatically exact approximation. The latter is provided by the exact ground state exchange–correlation potential corresponding to the instantaneous density. The results are compared to exact data obtained from the solution of the interacting Schrödinger equation. We find that the adiabatically exact approximation provides very good results for transitions of genuinely single excitation character but yields incorrect results if double excitations contribute substantially. However, the extent of the error can vary: some double excitations are just shifted in energy whereas others are missed completely. These situations are analyzed with the help of transition densities.
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Physical Chemistry Chemical Physics

Physical Chemistry Chemical Physics (PCCP) is an international journal co-owned by 19 physical chemistry and physics societies from around the world. This journal publishes original, cutting-edge research in physical chemistry, chemical physics and biophysical chemistry. To be suitable for publication in PCCP, articles must include significant innovation and/or insight into physical chemistry; this is the most important criterion that reviewers and Editors will judge against when evaluating submissions. The journal has a broad scope and welcomes contributions spanning experiment, theory, computation and data science. Topical coverage includes spectroscopy, dynamics, kinetics, statistical mechanics, thermodynamics, electrochemistry, catalysis, surface science, quantum mechanics, quantum computing and machine learning. Interdisciplinary research areas such as polymers and soft matter, materials, nanoscience, energy, surfaces/interfaces, and biophysical chemistry are welcomed if they demonstrate significant innovation and/or insight into physical chemistry. Joined experimental/theoretical studies are particularly appreciated when complementary and based on up-to-date approaches.











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