A density functional study of thorium tetrahalides

被引:18
作者
Gagliardi, L
Skylaris, CK
Willetts, A
Dyke, JM
Barone, V
机构
[1] Univ Bologna, Dipartimento Chim Fis & Inorgan, I-40136 Bologna, Italy
[2] CINECA, I-40033 Bologna, Italy
[3] Univ Cambridge, Dept Chem, Cambridge CB2 1EW, England
[4] Univ Southampton, Dept Chem, Southampton SO17 1BJ, Hants, England
[5] Univ Naples Federico II, Dipartimento Chim, I-80134 Naples, Italy
关键词
D O I
10.1039/b001447h
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
The results of a study on the ground states of thorium tetrahalides using density functional theory are presented. The equilibrium geometries of ThX4 (X=F, Cl, Br, I) have been optimized and their harmonic frequencies have been calculated. In the geometry optimizations the results were generated by using two different density functional programs, namely GAUSSIAN98 and MAGIC. Both local and non-local functionals were used. This allowed us to benchmark the MAGIC program and check the consistency of the theoretical predictions between different codes. Equilibrium structures, harmonic frequencies and zero-point energies were then calculated for a wider range of methods using GAUSSIAN98. Among these methods Hartree-Fock and Moller-Plesset second-order perturbation theory are included. All the calculated results are compared with experimental values where available. The frequencies of only the nu(3) and nu(4) vibrational modes have been measured for ThF4 and only nu(3) has been measured for ThCl4, while no vibrational frequencies have been measured for ThBr4 and ThI4. It is thus important to obtain improved values for all the vibrational frequencies of these molecules. Comparison can then be made with existing values, most of which have been derived from empirical correlations with results from related lighter tetrahalide molecules.
引用
收藏
页码:3111 / 3114
页数:4
相关论文
共 32 条
[1]   Toward reliable density functional methods without adjustable parameters: The PBE0 model [J].
Adamo, C ;
Barone, V .
JOURNAL OF CHEMICAL PHYSICS, 1999, 110 (13) :6158-6170
[2]   Exchange functionals with improved long-range behavior and adiabatic connection methods without adjustable parameters:: The mPW and mPW1PW models [J].
Adamo, C ;
Barone, V .
JOURNAL OF CHEMICAL PHYSICS, 1998, 108 (02) :664-675
[3]  
AKISHIN PA, 1958, PRIB TEKH EKSP, V3, P70
[4]   STRUCTURE, THERMOCHEMISTRY, AND MAGNETIC-PROPERTIES OF BINARY COPPER CARBONYLS BY A DENSITY-FUNCTIONAL APPROACH [J].
BARONE, V .
JOURNAL OF PHYSICAL CHEMISTRY, 1995, 99 (30) :11659-11666
[5]   DENSITY-FUNCTIONAL EXCHANGE-ENERGY APPROXIMATION WITH CORRECT ASYMPTOTIC-BEHAVIOR [J].
BECKE, AD .
PHYSICAL REVIEW A, 1988, 38 (06) :3098-3100
[6]  
BEECHING L, UNPUB
[7]   AB-INITIO ENERGY-ADJUSTED PSEUDOPOTENTIALS FOR ELEMENTS OF GROUPS 13-17 [J].
BERGNER, A ;
DOLG, M ;
KUCHLE, W ;
STOLL, H ;
PREUSS, H .
MOLECULAR PHYSICS, 1993, 80 (06) :1431-1441
[8]   Auxiliary basis sets for main row atoms and transition metals and their use to approximate Coulomb potentials [J].
Eichkorn, K ;
Weigend, F ;
Treutler, O ;
Ahlrichs, R .
THEORETICAL CHEMISTRY ACCOUNTS, 1997, 97 (1-4) :119-124
[9]   AUXILIARY BASIS-SETS TO APPROXIMATE COULOMB POTENTIALS [J].
EICHKORN, K ;
TREUTLER, O ;
OHM, H ;
HASER, M ;
AHLRICHS, R .
CHEMICAL PHYSICS LETTERS, 1995, 240 (04) :283-289
[10]  
Frisch M.J., 1998, GAUSSIAN 98