Density functional theory(DFT) calculations are performed to investigate the electronic and structural properties of the stoichiometric thorium oxide clusters(ThO2)n-/0(n = 1~5). Generalized Koopmans' theorem is a...Density functional theory(DFT) calculations are performed to investigate the electronic and structural properties of the stoichiometric thorium oxide clusters(ThO2)n-/0(n = 1~5). Generalized Koopmans' theorem is applied to predict the vertical detachment energies(VDEs)which are used to simulate the anionic photoelectron spectra(PES). Molecular orbital analyses are performed as well to analyze the chemical bonding in these thorium oxide clusters. The results show that the ground states of(ThO2)_n-/0(n = 1~5) clusters prefer the low-spin structures. With increasing of the cluster size(n), the structure parameters of(ThO2)n-/0(n = 1~5) gradually evolve toward bulk thorium oxide species. It shows that both the coordination number and the average bond length increase gradually in(ThO2)n-/0(n = 1~5) to approach that of ThO2 bulk. What's more, the vibration frequencies of Th=O double bonds are found to be decreasing along with the increased cluster size.展开更多
基金supported by Hunan Police Academy Research Innovation Team-Key Technologies of Road Traffic Safety Law Enforcementthe Key Laboratory of Impression Evidence Examination and Identification Technology,Ministry of Public Security,People’s Republic of China
文摘Density functional theory(DFT) calculations are performed to investigate the electronic and structural properties of the stoichiometric thorium oxide clusters(ThO2)n-/0(n = 1~5). Generalized Koopmans' theorem is applied to predict the vertical detachment energies(VDEs)which are used to simulate the anionic photoelectron spectra(PES). Molecular orbital analyses are performed as well to analyze the chemical bonding in these thorium oxide clusters. The results show that the ground states of(ThO2)_n-/0(n = 1~5) clusters prefer the low-spin structures. With increasing of the cluster size(n), the structure parameters of(ThO2)n-/0(n = 1~5) gradually evolve toward bulk thorium oxide species. It shows that both the coordination number and the average bond length increase gradually in(ThO2)n-/0(n = 1~5) to approach that of ThO2 bulk. What's more, the vibration frequencies of Th=O double bonds are found to be decreasing along with the increased cluster size.
