Green's function formalism coupled with Gaussian broadening of discrete states for quantum transport: application to atomic and molecular wires.
Green's function formalism coupled with Gaussian broadening of discrete states for quantum transport: application to atomic and molecular wires.
复制标题
DOI：
10.1063/1.1799991
复制
发表时间：
2004-10
期刊：
影响因子：
--
通讯作者：
T. Tada;M. Kondo;K. Yoshizawa
中科院分区：
文献类型：
--
作者：
T. Tada;M. Kondo;K. Yoshizawa
本文提出了一种结合加宽态密度的绿色函数方法来计算电导。在团簇-分子-团簇体系中，将团簇的展宽态密度定义为电极的连续态密度，并用于计算电极的绿色函数。将该方法与密度泛函理论相结合，应用于金原子线和由苯-1，4-二硫醇盐、苯-1，4-二甲硫醇盐、4，4（'）-联吡啶、己二硫醇盐和辛烷二硫醇盐组成的分子线的电传输。电导的计算采用了LANL 2DZ、CEP和SDD基组的B3 LYP、B3 PW 91、MPW 1 PW 91、SVWN和BPW 91泛函。成功地确定了金原子线的宽度参数，再现了金原子线电导的量子单位2 e（2）/h。B3 LYP杂化泛函和CEP-31 G基组的组合在再现Tao等人[Science 301，1221（2003）; J. Am. 125，16164（2003）; Nano Lett. 4，267（2004）]。
A Green's function formalism incorporating broadened density of states (DOS) is proposed for the calculation of electrical conductance. In cluster-molecule-cluster systems, broadened DOS of the clusters are defined as continuous DOS of electrodes and used to calculate Green's function of electrodes. This approach combined with density functional theory is applied to the electrical transmission of gold atomic wires and molecular wires consisting of benzene-1,4-dithiolate, benzene-1,4-dimethanethiolate, 4,4(')-bipyridine, hexane dithiolate, and octane dithiolate. The B3LYP, B3PW91, MPW1PW91, SVWN, and BPW91 functionals with the LANL2DZ, CEP, and SDD basis sets are employed in the calculation of conductance. The width parameter was successfully determined to reproduce the quantum unit of conductance 2e(2)/h in gold atomic wires. The combination of the B3LYP hybrid functional and the CEP-31G basis set is excellent in reproducing measured conductances of molecular wires by Tao et al. [Science 301, 1221 (2003); J. Am. Chem. Soc. 125, 16164 (2003); Nano Lett. 4, 267 (2004)].