Time-dependent quantum dynamical simulations of C2 condensation under extreme conditions
文献情報
Jacek Jakowski, Stephan Irle
We report theoretical studies of the initial phase of bulk C2 condensation into carbon nano-structures by means of Born–Oppenheimer and time-dependent quantum mechanical Liouville–von Neumann molecular dynamics based on the density-functional tight-binding (DFTB) framework for electrons. We observe that the time-dependent quantum mechanical approach leads to faster formation of carbon nanostructures than analogous Born–Oppenheimer simulations. Our results suggest that the condensation of bulk carbon is nonadiabatic in nature, with the critical role of electronic stopping as in ion-irradiation of materials. Contrary to time-dependent quantum mechanical simulations, Born–Oppenheimer dynamics incorrectly predict that the short carbon chains obtained from initial reactive collisions between C2 quickly evaporate, leading to much lower probability of secondary collisions and condensation. We also discuss some deficiencies in Born–Oppenheimer dynamics that lead to unphysical charge polarization and electron transfer.
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掲載誌
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.














