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幻数尺寸Li-n-1,Lin,Li+ n+1(n=20,40)团簇的几何结构、电子与光学性质的第一性原理研究

郭钊 陆斌 蒋雪 赵纪军

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幻数尺寸Li-n-1,Lin,Li+ n+1(n=20,40)团簇的几何结构、电子与光学性质的第一性原理研究

郭钊, 陆斌, 蒋雪, 赵纪军

Structural, electronic, and optical properties of Li-n-1, Lin and Li+ n+1(n=20, 40) clusters by first-principles calculations

Guo Zhao, Lu Bin, Jiang Xue, Zhao Ji-Jun
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  • 基于密度泛函理论,采用第一性原理分子动力学模拟退火方法,对Li-n-1,Lin,Li+n+1 (n=20,40)的最低能量结构进行了全局搜索. 发现锂团簇的生长模式是以单个或多个嵌套的正多面体为核心,其余原子以五角锥为基本单元围绕核心生长. 基于最低能量结构的第一性原理电子结构计算得到锂团簇的分子轨道能级分布与无结构凝胶模型给出的电子壳层完全一致. 在总电
    The lowest-energy structures of Li-n-1, Lin and Li+n+1 clusters (n=20, 40) were determined from first-principles simulated annealing followed by geometry optimization within the density functional theory. The growth mechanism of Lin clusters is based on nested multiple polyhedron. Other atoms form pentagonal pyramid centered on the core polyhedron. From our first-principles calculations, the molecular orbital levels can be divided into several groups, which are in good agreement with the electron shells described by structureless jellium model. With the same amount of valence electrons, the number of ions and charge states in the Li clusters have only little effect on the electronic structures. Li-19, Li20, Li+21 and Li-39, Li40, Li+41 exhibit similar energy level distributions, respectively, indicating that the momentum order is the dominating factor for these clusters. The optical absorption spectra of Li-n-1, Lin and Li+n+1 (n=20, 40) clusters from time-dependent density functional theory calculations show giant resonance phenomenon and the simulated resonance peaks agree with experimental values. With same amount of valence electrons, the polarizability decreases with the number of ions and the optical resonance peaks blueshift as the ionic number increases.
    • 基金项目: 大学生创新性实验计划(批准号:081014115) 和教育部新世纪优秀人才支持计划(批准号:NCET-06-0281)资助的课题.
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    Chen L, Xu C, Zhang X F 2009 Acta Phys. Sin. 58 1603(in Chinese)[陈 亮、徐 灿、张小芳 2009 物理学报 58 1603]

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    Lu Z H, Cao J X, 2008 Chin. Phys. B 17 3336

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    Zhang C R, Chen Y H, Wang D B, Wu Y Z, Chen H S 2008 Chin. Phys. B 17 2938

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    [39]

    Li J, Li X, Zhai H J, Wang L S 2003 Science 299 864

    [40]

    Wang J, Wang G, Zhao J 2003 Chem. Phys. Lett. 380 716

    [41]

    Ekardt W 1984 Phys. Rev. B 29 1558

    [42]

    Bjφrnholm S 1990 Comtemp. Phys. 31 390

  • [1]

    Li B, Yang C L, Qi K T, Zhang Y, Sheng Y 2009 Acta Phys. Sin. 58 3104 (in Chinese) [李 兵、杨传路、齐凯天、张 岩、盛 勇 2009 物理学报 58 3104]

    [2]

    Chen L, Xu C, Zhang X F 2009 Acta Phys. Sin. 58 1603(in Chinese)[陈 亮、徐 灿、张小芳 2009 物理学报 58 1603]

    [3]

    Lu Z H, Cao J X, 2008 Chin. Phys. B 17 3336

    [4]

    Zhang C R, Chen Y H, Wang D B, Wu Y Z, Chen H S 2008 Chin. Phys. B 17 2938

    [5]

    Ellert C, Schmidt M, Schmitt C, Haberland H, Guet C 1999 Phys. Rev. B 59 R7841

    [6]

    Knight W D, Clemenger K, de Heer W A, Saunders W A, Chou M Y, Cohen M L 1984 Phys. Rev. Lett. 52 2141

    [7]

    de Heer W A 1993 Rev. Mod. Phys. 65 611

    [8]

    Yannouleas C, Vigezzi E, Broglia R A 1993 Phys. Rev. B 47 9849

    [9]

    Bréchignac C, Connerade J P 1994 J. Phys. B 27 3795

    [10]

    Kornath A, Kaufmann A, Zoermer A, Ludwig R 2003 J. Chem. Phys. 118 6957

    [11]

    Bréchignac C, Cahuzac P, Leygnier J, Sarfati A 1993 Phys. Rev. Lett. 70 2036

    [12]

    Bréchignac C, Busch H, Cahuzac P, Leygnier J 1994 J. Chem. Phys. 101 6992

    [13]

    Dugourd P, Rayane D, Labastie P, Vezin B, Chevaleyre J, Broyer M 1992 Chem. Phys. Lett. 197 433

    [14]

    Benichou E, Antoine R, Rayane D, Vezin B, Dalby F W, Dugourd P, Broyer M, Ristori C, Chandezon F, Huber B A, Rocco J C, Blundell S A, Guet C 1999 Phys. Rev. A 59 R1

    [15]

    Antoine R, Rayane D, Allouche A R, Aubert-Frecon M, Benichou E, Dalby F W, Dugourd P, Broyer M, Guet C 1999 J. Chem. Phys. 110 5568

    [16]

    Rao B K, Jena P 1985 Phys. Rev. B 32 2058

    [17]

    Rao B K, Jena P, Manninen M 1985 Phys. Rev. B 32 477

    [18]

    Wang F, Andriopoulos N, Wright N, Nagy-Felsobuki E I 1991 J. Cluster Sci. 2 203

    [19]

    Boustani I, Pewestorf W, Fantucci P, Bonai Dc' -Kouteck V, Koutecky J 1987 Phys. Rev. B 35 9437

    [20]

    Sugino O, Kamimura H 1990 Phys. Rev. Lett. 65 2696

    [21]

    Wheeler S E, Schaefer III H F 2005 J. Chem. Phys. 122 204328

    [22]

    Gardet G, Rogemond F, Chermette H 1996 J. Chem. Phys. 105 9933

    [23]

    Fournier R, Cheng J B Y, Wong A 2003 J. Chem. Phys. 119 9444

    [24]

    Jose K V J, Gadre S R 2008 J. Chem. Phys. 129 164314

    [25]

    Chandrakumar K R S, Ghanty T K, Ghosh S K 2004 J. Phys. Chem. A 108 6661

    [26]

    Bréchignac C, Cahuzac P, Carlier F, Leygnier J 1989 Chem. Phys. Lett. 164 433

    [27]

    Dugourd P, Blanc J, Bona i Dc' -Kouteck V, Broyer M, Chevaleyre J, Koutecky J, Pittner J, Wolf J P, Wste L 1991 Phys. Rev. Lett. 67 2638

    [28]

    Blanc J, Bona i Dc' -Kouteck V, Broyer M, Chevaleyre J, Dugourd P, Koutecky J, Scheuch C, Wolf J P, Wste L 1992 J. Chem. Phys. 96 1793

    [29]

    Pacheco J M, Martins J L 1997 J. Chem. Phys. 106 6039

    [30]

    Blundell S A, Guet C 1995 Z. Phys. D 33 153

    [31]

    Yabana K, Bertsch G F 1995 Z. Phys. D 32 329

    [32]

    Harris J 1985 Phys. Rev. B 31 1770

    [33]

    Perdew J P, Burke K, Ernzerhof M 1996 Phys. Rev. Lett. 77 3865

    [34]

    Delley B 1990 J. Chem. Phys. 92 508

    [35]

    Onida G, Reining L, Rubio A 2002 Rev. Mod. Phys. 74 601

    [36]

    Beck T L 2000 Rev. Mod. Phys. 72 1041

    [37]

    Becke A D 1993 J. Chem. Phys. 98 5648

    [38]

    Frisch M J, Trucks G W, Schlegel H B, Scuseria G E, Robb M A, Cheeseman J R, Montgomery Jr J A, Vreven T, Kudin K N, Burant J C, Millam J M, Iyengar S S, Tomasi J, Barone V, Mennucci B, Cossi M, Scalmani G, Rega N, Petersson G A, Nakatsuji H, Hada M, Ehara M, Toyota K, Fukuda R, Hasegawa J, Ishida M, Nakajima T, Honda Y, Kitao O, Nakai H, Klene M, Li X, Knox J E, Hratchian H P, Cross J B, Bakken V, Adamo C, Jaramillo J, Gomperts R, Stratmann R E, Yazyev O, Austin A J, Cammi R, Pomelli C, Ochterski J W, Ayala P Y, Morokuma K, Voth G A, Salvador P, Dannenberg J J, Zakrzewski V G, Dapprich S, Daniels A D, Strain M C, Farkas O, Malick D K, Rabuck A D, Raghavachari K, Foresman J B, Ortiz J V, Cui Q, Baboul A G, Clifford S, Cioslowski J, Stefanov B B, Liu G, Liashenko A, Piskorz P, Komaromi I, Martin R L, Fox D J, Keith T, Al-Laham M A, Peng C Y, Nanayakkara A, Challacombe M, Gill P M W, Johnson B, Chen W, Wong M W, Gonzalez C, Pople J A, Gaussian 03 (Gaussian, Inc., Wallingford CT, 2004)

    [39]

    Li J, Li X, Zhai H J, Wang L S 2003 Science 299 864

    [40]

    Wang J, Wang G, Zhao J 2003 Chem. Phys. Lett. 380 716

    [41]

    Ekardt W 1984 Phys. Rev. B 29 1558

    [42]

    Bjφrnholm S 1990 Comtemp. Phys. 31 390

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出版历程
  • 收稿日期:  2010-01-12
  • 修回日期:  2010-02-23
  • 刊出日期:  2011-01-15

幻数尺寸Li-n-1,Lin,Li+ n+1(n=20,40)团簇的几何结构、电子与光学性质的第一性原理研究

  • 1. (1)大连理工大学物理与光电工程学院,大连 116024; (2)大连理工大学物理与光电工程学院,大连 116024;大连理工大学高科技研究院,大连 116024
    基金项目: 大学生创新性实验计划(批准号:081014115) 和教育部新世纪优秀人才支持计划(批准号:NCET-06-0281)资助的课题.

摘要: 基于密度泛函理论,采用第一性原理分子动力学模拟退火方法,对Li-n-1,Lin,Li+n+1 (n=20,40)的最低能量结构进行了全局搜索. 发现锂团簇的生长模式是以单个或多个嵌套的正多面体为核心,其余原子以五角锥为基本单元围绕核心生长. 基于最低能量结构的第一性原理电子结构计算得到锂团簇的分子轨道能级分布与无结构凝胶模型给出的电子壳层完全一致. 在总电

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