A relativistic density functional study of gaseous uranium tetrahalides |
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| Authors: | Yunguang Zhang Ce Hao |
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| Institution: | 1. School of Electronics and Information Engineering, Sichuan University , Chengdu, Sichuan, 610065, China;2. State Key Laboratory of Fine Chemicals, Dalian University of Technology , Dalian, 116024, China;3. Virtual Laboratory of Computational Chemistry, CNIC, Chinese Academy of Sciences , Beijing, China |
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| Abstract: | The molecular structures and vibrational frequencies of gaseous UX4 (X = F, Cl, Br and I) molecules have been investigated using generalized gradient approximation (GGA) functions (BP, BLYP, PBE and RPBE) with triple-zeta polarized (TZP) basis set. Scalar relativistic effects are introduced via the zeroth-order regular approximation (ZORA) approach to the Dirac equation in the present study. Of the methods examined here the RPBE has the best performance in terms of the errors compared with experiment and reference for the vibrational frequencies. The bond dissociation energies (BDE) for U–X bonds in the UX4 were obtained using the RPBE method, and are in good agreement with experimental values. In addition, satisfactory calculated entropies of UX4 have also been obtained at temperatures ranging from 600 to 1200 K in 50 steps using the same method. |
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| Keywords: | uranium tetrahalide molecular structures vibrational frequencies BDE |
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