Geometries, stabilities and fragmental channels of neutral and charged sulfur clusters: SnQ (n = 3–20, Q = 0, ±1)
文献信息
Yuanyuan Jin, George Maroulis, Xiaoyu Kuang, Liping Ding, Cheng Lu, Jingjing Wang, Chuanzhao Zhang, Meng Ju
We have performed unbiased searches for the global minimum structures of neutral and charged sulfur clusters SnQ (n = 3–20, Q = 0, ±1) relying on the CALYPSO structure searching method combined with density functional theory geometric optimization. Very accurate ab initio calculations are used to determine relative stabilities and energy ranking among competing low-lying isomers of the neutral and charged sulfur clusters obtained from the structure search. The harmonic vibrational analysis is also undertaken to assure that the optimized geometries are the true minima. It is shown that the most equilibrium geometries of sulfur clusters are closed three-dimensional (3D) helical rings, which is in agreement with the experimental observations. The binding energies, second-order energy differences, and highest occupied–lowest unoccupied molecular orbital (HOMO–LUMO) gaps of the considered species are calculated and analyzed systematically. Additionally, the fragmentation channels are determined and the results indicate that the SnQ → S2 + Sn−2Q channel is a route that the small clusters (n = 3–10) favor, while the larger species (n = 13–20) prefer the SnQ → S8 + Sn−8Q channel.
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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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