Implementation of time-dependent density functional response equations

被引:668
作者
van Gisbergen, SJA
Snijders, JG
Baerends, EJ
机构
[1] Free Univ Amsterdam, Theoret Chem Sect, NL-1081 HV Amsterdam, Netherlands
[2] Univ Groningen, Dept Chem Phys, NL-9747 AG Groningen, Netherlands
[3] Univ Groningen, Ctr Mat Sci, NL-9747 AG Groningen, Netherlands
关键词
density functional theory; optical response properties of molecules;
D O I
10.1016/S0010-4655(99)00187-3
中图分类号
TP39 [计算机的应用];
学科分类号
081203 ; 0835 ;
摘要
Time-dependent density functional theory provides a first principles method for the calculation of frequency-dependent polarizabilities, hyperpolarizabilities, excitation energies and many related response properties. In recent years, the molecular results obtained by several groups have shown that this approach is in general more accurate than the time-dependent Hartree-Fock approach, and is often competitive in accuracy with computationally more demanding conventional ab initio approaches. In this paper, our implementation of the relevant equations in the Amsterdam Density Functional program is described. We will focus on certain aspects of the implementation which are necessary for an efficient evaluation of the desired properties, enabling the treatment of large molecules. Such an efficient implementation is obtained by: using the full symmetry of the molecule, using a set of auxiliary functions for fitting the (zeroth- and first-order) electron density, using a highly vectorized and parallelized code, using linear scaling techniques, and, most importantly, by solving the response equations iteratively. (C) 1999 Elsevier Science B.V.
引用
收藏
页码:119 / 138
页数:20
相关论文
共 106 条
[81]   LINEAR-RESPONSE THEORY WITHIN THE DENSITY-FUNCTIONAL FORMALISM - APPLICATION TO ATOMIC POLARIZABILITIES [J].
STOTT, MJ ;
ZAREMBA, E .
PHYSICAL REVIEW A, 1980, 21 (01) :12-23
[82]   LOCAL DENSITY THEORY OF IONIC HYPERPOLARIZABILITY [J].
SUBBASWAMY, KR ;
MAHAN, GD .
JOURNAL OF CHEMICAL PHYSICS, 1986, 84 (06) :3317-3319
[83]  
SUNDERAM VS, 1990, CONCURRENCY PRACTICE, V2
[84]   NONLINEAR OPTICAL-PROPERTIES OF THE C-60 MOLECULE - THEORETICAL AND EXPERIMENTAL STUDIES [J].
TALAPATRA, GB ;
MANICKAM, N ;
SAMOC, M ;
ORCZYK, ME ;
KARNA, SP ;
PRASAD, PN .
JOURNAL OF PHYSICAL CHEMISTRY, 1992, 96 (13) :5206-5208
[85]   3RD-ORDER OPTICAL NONLINEARITY OF C-60, C-70, AND CS2 IN BENZENE AT 1.06-MU-M [J].
TANG, N ;
PARTANEN, JP ;
HELLWARTH, RW ;
KNIZE, RJ .
PHYSICAL REVIEW B, 1993, 48 (11) :8404-8408
[86]  
TEVELDE G, 1909, TH4SIS VRIJE U AMSTE
[87]  
TOER DJ, 1998, J CHEM PHYS, V108, P2545
[88]   Time-dependent density-functional theory for strong-field multiphoton processes: Application to the study of the role of dynamical electron correlation in multiple high-order harmonic generation [J].
Tong, XM ;
Chu, SI .
PHYSICAL REVIEW A, 1998, 57 (01) :452-461
[89]   TIME-DEPENDENT OPTIMIZED EFFECTIVE POTENTIAL [J].
ULLRICH, CA ;
GOSSMANN, UJ ;
GROSS, EKU .
PHYSICAL REVIEW LETTERS, 1995, 74 (06) :872-875
[90]  
ULLRICH CA, 1995, THESIS U WURZBURG