Al2Sn（n=210）团簇结构特征和稳定性的密度泛函理论研究

吕瑾; 杨丽君; 王艳芳; 马文瑾

doi:10.7498/aps.63.163601

摘要

采用密度泛函理论的B3LYP方法，在6-311G**水平上对Al2Sn （n=210）团簇的几何结构和电子结构进行了理论计算. 讨论了铝硫二元离子混合团簇基态结构的变化规律、电荷转移和成键特征. 结果表明，在S簇中掺杂Al原子会使Sn结构发生明显改变. Al2Sn团簇基态结构是以Al2S2四元环为骨架或桥梁，分别与S原子或S簇相结合形成单环到三环的平面和立体结构. 结构中化学键键型和成键数目影响团簇的稳定性. 通过对基态结构的解离能和能量二次差分值的分析得到了Al2Sn团簇的稳定性信息.

关键词:

Abstract

The geometric configurations and electronic structures of the Al2Sn (n=2-10) clusters are calculated by the B3LYP (density functional theory) method at 6-311G** level. The variations of the ground state structure, charge transfer and bonding characteristic of the aluminum-sulfur doped clusters are discussed in detail. The results show that the structures of pure Sn clusters are fundamentally changed due to the doping of the Al atoms. Our work exhibits that the all the ground states of Al2Sn clusters share the same four-member Al2S2 ring, and from single ring to three rings plane and three-dimensional structure structures are formed by inserting one S atom or S clusters. The stability of cluster structure is influenced by both the chemical bond structure and number. The stability information of Al2Sn clusters is obtained by analyzing the dissociation energies and the second-order difference energies of the ground state structures.

Keywords:

作者及机构信息

1.
山西师范大学化学与材料科学学院, 临汾 041004

基金项目: 国家自然科学基金青年科学基金（批准号：21301112）、教育部博士点基金（批准号：20131404120001）和山西省自然科学基金（批准号：2012011009-4，2012021020-1）资助的课题.

Authors and contacts

1.
School of Chemistry and Material Science, Shanxi Normal University, Linfen 041004, China

Funds: Project supported by the Young Scientists Fund of the National Natural Science Foundation of China (Grant No. 21301112), the Ph. D. Program Foundation of Ministry of Education of China (Grant No. 20131404120001), and the Natural Science Foundation of Shanxi Province, China (Grant Nos. 2012011009-4, 2012021020-1).

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施引文献

[1]	Cui M, Feng J K, Ge M F, Wang S F, Sun J Z, Liu J B, Gao Z, Kong F A 1999 Acta Chim. Sin. 57 1062 (in Chinese) [崔勐, 封继康, 葛茂发, 王素凡, 孙家钟, 刘剑波, 高振, 孔繁敖 1999 化学学报 57 1062]
[2]	Zakrzewski V G, Niessen W V 1994 Theor. Chim. Acta 88 75
[3]
[4]	Suontamo R J, Laitinen R S, Pakkanen T A 1994 J. Mol. Struct.-Theochem. 313 189
[5]
[6]	Chen M D, Liu M L, Luo H B, Zhang Q E, Au C T 2001 J. Mol. Struct.-Theochem. 548 133
[7]
[8]
[9]	Bai Y L, Chen X R, Yang X D, Lu P F 2003 Acta Phys. Chim. Sin. 19 1102
[10]	Chen M D, Liu M H, Liu J W, Jiao Y C, Zhang Q E 2002 Chin. J. Chem. Phys. 15 357 (in Chinese) [陈明旦, 刘明宏, 刘建文, 焦毓才, 张乾二 2002 化学物理学报 15 357]
[11]
[12]	Chen M D, Liu M H, Liu J W, Jiao Y C, Zhang Q E 2002 Chin. J. Struct. Chem. 21 557 (in Chinese) [陈明旦, 刘明宏, 刘建文, 焦毓才, 张乾二 2002 结构化学 21 557]
[13]
[14]	Chen M D, Liu M H, Luo H B, Qiu Z J, Zhang Q E 2001 Chin. J. Struct. Chem. 20 399 (in Chinese) [陈明旦, 刘明宏, 罗海彬, 邱志军, 张乾二 2001 结构化学 20 399]
[15]
[16]	Zhao Y C, Yuan J Y, Zhang Z G, Xu H G, Zheng W J 2011 Dalton Trans. 40 2502
[17]
[18]	Liang B Y, Wang X F, Andrews L 2009 J. Phys. Chem. A 113 5375
[19]
[20]	Liang B Y, Wang X F, Andrews L 2009 J. Phys. Chem. A 113 3336
[21]
[22]
[23]	Feng X Q, Feng X H, Jiang Z Y 2010 Acta Phys. Sin. 59 7838 (in Chinese) [冯选旗, 冯雪红, 姜振益 2010 物理学报 59 7838]
[24]
[25]	Guo L 2010 J. Alloys. Compd. 498 121
[26]	Feng X J, Luo Y H 2007 J. Phys. Chem. A 111 2420
[27]
[28]
[29]	Li X, Wang L S, Boldyrev A I, Simons J 1999 J. Am. Chem. Soc. 121 6033
[30]	Averkiev B B, Boldyrev A I, Li X, Wang L S 2007 J. Phys. Chem. A 111 34
[31]
[32]
[33]	Averkiev B B, Call S, Boldyrev A I, Wang L M, Huang W, Wang L S 2008 J. Phys. Chem. A 112 1873
[34]
[35]	Yang P, Ge J H, Jiang Z Y 2007 Chin. Phys. 16 1014
[36]	Gu J B, Yang X D, Wang H Q, Li H F 2012 Chin. Phys. B 21 043102
[37]
[38]
[39]	Nakajima A, Taguwa T, Nakao K, Hoshino K, Iwata S, Kaya K 1995 J. Chem. Phys. 102 660
[40]	Nakajima A, Taguwa T, Nakao K, Hoshino K, Iwata S, Kaya K 1996 Surf. Rev. Lett. 3 417
[41]
[42]
[43]	Nakajima A, Zhang N, Kawamata H, Hayase T, Nakao K, Kaya K 1995 Chem. Phys. Lett. 241 295
[44]	Zhong M M, Kuang X Y, Wang Z H, Shao P, Ding L P 2013 J. Mol. Model. 19 263
[45]
[46]
[47]	Zhang N, Shi Y, Gao Z, Kong F A, Zhu Q H 1994 J. Chem. Phys. 101 1219
[48]	Jensen J O 2003 J. Mol. Struct.-Theochem. 664 37
[49]
[50]	Jensen J O 2004 Spectrochim. Acta Part A 60 2547
[51]
[52]
[53]	Zhang Z G, Xu H G, Feng Y, Zheng W J 2010 J. Chem. Phys. 132 161103
[54]	Li T X, Wang L, Wang F, Chen J, Jiang Z Y, Li L S 2011 Chin. Phys. B 20 033101
[55]
[56]	Becke A D 1993 J. Chem. Phys. 98 5648
[57]
[58]	Lee C, Yang W, Parr R G 1988 Phys. Rev. B 37 785
[59]
[60]	Frisch M J, Trucks G W, Schlegel H B, Scuseria G E, Robb M A, Cheeseman J R, Montgomery 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 J, Pople A 2004 Gaussian 03 Revision D.01 (Wallingford: Gaussian Inc.)
[61]
[62]
[63]	Guo L, Wu H S 2007 Eur. Phys. J. D 42 259
[64]
[65]	Chen X H, Gao T, Luo S Z, Ma M Z, Xie A D, Zhu Z H 2006 Acta Phys. Sin. 55 1113 (in Chinese) [谌晓洪, 高涛, 罗顺忠, 马美仲, 谢安东, 朱正和 2006 物理学报 55 1113]
[66]
[67]	Xu W G, Zhang Y C, Zhai L 2009 Sci. China B: Chem. 52 2237
[68]
[69]	John A W H, Dorothea K S, Frank H S 1996 J. Phys. Chem. 100 1098
[70]	Zhao G F, Zhi L L, Guo L J, Zeng Z 2007 J. Chem. Phys. 127 234705
[71]
[72]	Gutirrez G, Johansson B 2002 Phys. Rev. B 65 104202
[73]
[74]
[75]	Bonacic K V, Fantucci P, Koutecky J 1991 Chem. Rev. 91 1035
[76]	Wang J L, Wang G H, Zhao J J 2001 J. Phys. Rev. B 64 205411
[77]

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