Parity Alternation of Silicon-doped Ternary Cationic Clusters HCnSi2+ (n = 1–9)

摘要
图/表
参考文献(48)
相关文章 (0)

全文: PDF (708 KB) HTML (1 KB)
输出: BibTeX | EndNote (RIS)

摘要 Systematic study on the electronic/geometrical structures and the parity alternation effect of silicon-doped ternary cationic clusters HC_nSi₂⁺ (n = 1～9) have been carried out at the coupled cluster level. The ground-state (G-S) isomers of the clusters have been defined. The C_n chains of the G-S isomers display polyacetylene-like structures. The even-n cations are more stable than the odd-n ones. Such a trend of even/odd alternation has been elaborated based on concepts of the bond character, atomic charge, incremental binding energy, ionization potential, proton affinity and fragmentation energies of the systems. The findings accord with the relative intensities of HC_nSi₂⁺ species recorded in the related mass spectrometric experiments.

	服务

	把本文推荐给朋友
	加入我的书架
	加入引用管理器
	E-mail Alert
	RSS
	作者相关文章
	齐嘉媛
	朱焕焕
	黄昕

关键词 ： silicon-doped carbon clusters , HC_nSi₂⁺, ternary cationic clusters, coupled cluster method

Abstract：Systematic study on the electronic/geometrical structures and the parity alternation effect of silicon-doped ternary cationic clusters HC_nSi₂⁺ (n = 1～9) have been carried out at the coupled cluster level. The ground-state (G-S) isomers of the clusters have been defined. The C_n chains of the G-S isomers display polyacetylene-like structures. The even-n cations are more stable than the odd-n ones. Such a trend of even/odd alternation has been elaborated based on concepts of the bond character, atomic charge, incremental binding energy, ionization potential, proton affinity and fragmentation energies of the systems. The findings accord with the relative intensities of HC_nSi₂⁺ species recorded in the related mass spectrometric experiments.

Key words：

silicon-doped carbon clusters HC_nSi₂⁺ ternary cationic clusters coupled cluster method method

收稿日期: 2013-12-04 出版日期: 2014-04-01

基金资助:This work was supported by the Research Fund for the Doctoral Program of Higher Education of China (RFDP, 20123514120003) and Foundations of Fuzhou University (0041-600566 and 2012-XQ-12)

作者简介: 齐嘉媛: jyqi@fzu.edu.cn

引用本文:

齐嘉媛;朱焕焕;黄昕. Parity Alternation of Silicon-doped Ternary Cationic Clusters HC_nSi₂⁺ (n = 1–9)[J]. 结构化学, 2014, 33(7): 959-970.
QI Jia-Yuan;ZHU Huan-Huan;HUANG Xin. Parity Alternation of Silicon-doped Ternary Cationic Clusters HC_nSi₂⁺ (n = 1–9). CHINESE JOURNAL OF STRUCTURAL CHEMISTRY, 2014, 33(7): 959-970.

链接本文:

http://manu30.magtech.com.cn/jghx/CN/ 或 http://manu30.magtech.com.cn/jghx/CN/Y2014/V33/I7/959

(1) Weltner, W. J.; Van Zee, R. J. Carbon molecules, ions, and clusters. Chem. Rev. 1989, 89, 1713-1747.

(2) Le Teuff, Y. H.; Millar, T. J.; Markwick, A. J. The UMIST database for astrochemistry 1999. Astron. Astrophys. Suppl. Ser. 2000, 146, 157-168.

(3) Millar, T. J. Organic molecules in the interstellar medium. Astrophys. Space Sci. Libr. 2004, 305, 17-31.

(4) Brünken, S.; Gupta, H.; Gottlieb, C. A.; McCarthy, M. C.; Thaddeus, P. Detection of the carbon chain negative ion C₈H^- in TMC-1. Astrophys. J. 2007, 664, 43-46.

(5) Cernicharo, J.; Guélin, M.; Agúndez, M.; McCarthy, M. C.; Thaddeus, P. Detection of C₅N^- and vibrationally excited C₆H in IRC+102161. Astrophys. J. 2008, 688, 83.

(6) Schilke, P.; Comito, C.; Thorwirth, S. First detection of vibrationally excited HNC in space. Astrophys. J. 2003, 582, 101-104.

(7) Rolffs, R.; Schilke, P.; Wyrowski, F.; Dullemond, C.; Menten, K. M.; Thorwirth, S.; Belloche, A. Hot HCN around young massive stars at 0.1'' resolution. Astron. Astrophys 2011, 529, 76.

(8) Neufeld, D. A.; Schilke, P.; Menten, K. M.; Wolfire, M. G.; Black, J. H.; Schuller, F. C.; Muller, H. S. P.; Thorwirth, S.; Gusten, R.; Philipp, S. Discovery of interstellar CF⁺. Astron. Astrophys 2008, 454, L37-L40.

(9) Cataldo, F. Monocyanopolyynes from a carbon arc in ammonia: about the relative abundance of polyynes series formed in a carbon arc and those detected in the circumstellar shells of AGB stars. Int. J. Astrobiol. 2006, 5, 37-45.

(10) Thaddeus, P.; McCarthy, M. C. Carbon chains and rings in the laboratory and in space. Spectrochim. Acta. Part A 2001, 57A, 757-774.

(11) Thaddeus, P.; McCarthy, M. C.; Travers, M. J.; Gottlieb, C. A.; Chen, W. New carbon chains in the laboratory and in interstellar space. Faraday Discuss 1998, 109, 121-135.

(12) McCarthy, M. C.; Apponi, A. J.; Gottlieb, C. A.; Thaddeus, P. Laboratory detection of five new linear silicon carbides. SiC₃, SiC₅, SiC₆, SiC₇, and SiC₈. Astrophys. J. 2000, 538, 766-772.

(13) McCarthy, M. C.; Gottlieb, C. A.; Gupta, H.; Thaddeus, P. Laboratory and astronomical identification of the negative molecular ion C₆H^-. Astrophys. J. 2006, 652, 141-144.

(14) Thaddeus, P.; Gottlieb, C. A.; Gupta, H.; Brünken, S.; McCarthy, M. C.; Agúndez, M.; Guélin, M.; Cernicharo, J. Laboratory and astronomical detection of the negative molecular ion C₃N^-. Astrophys. J. 2008, 677, 1132.

(15) Huang, Q. J.; Liu, Z. Y.; Liu, H. F.; Huang, R. B.; Zheng, L. S. Structural studies of laser-generated C_nSi_m^± and C_nSi_mH⁺. Chin. J. Chem. Phys. 1995, 8, 113-117.

(16) Huang, R. B.; Liu, Z. Y.; Wang, C.; Huang, Q. J.; Zheng, L. S. Binary cluster ions Si_nX_m^± (X = C, P, S, O) produced by laser ablation. Acta. Chimica Sinica 1996, 54, 475-480.

(17) Botschwina, P.; Oswald, R. NC₅NC: results of coupled cluster calculations and an unusual anharmonicity effect. Chem. Phys. Lett. 2000, 319, 587-594.

(18) McCarthy, M. C.; Cooksy, A. L.; Mohamed, S.; Gordon, V. D.; Thaddeus, P. Rotational spectra of the nitrogen-sulfur carbon chains NC_nS, n = 1～7. Astrophys. J. Suppl. Ser. 2003, 144, 287-297.

(19) Mladenovic, M.; Botschwina, P.; Puzzarini, C. Six-dimensional potential energy surface and rovibrational energies of the HCCN radical in the ground electronic state. J. Phys. Chem. A 2006, 110, 5520-5529.

(20) Scemama, A.; Chaquin, P.; Gazeau, M. C.; Benilan, Y. Theoretical study of the structure and properties of polyynes and monocyano- and dicyanopolyynes: predictions for long chain compounds. J. Phys. Chem. A 2002, 106, 3828-3837.

(21) Qi, J. Y.; Chen, M. D.; Wu, W.; Zhang, Q. E.; Au, C. T. Parity alternation of interstellar molecules cyanopolyynes HC_nN (n = 1～17). Chem. Phys. 2009, 364, 31-38.

(22) Flores, J. R. Electronic spectra of SC_nH radicals (n = 2～4): an ab initio study. J. Phys. Chem. B 2003, 107, 9711-9716.

(23) Bundhun, A.; Abdallah, H. H.; Ramasami, P.; Gaspar, P. P.; Schaefer, H. F. Dicyanogermylenes: a tale of isomers and interconversions. Inorg. Chem. 2012, 51, 12152-12164.

(24) Yang, J.; Qi, J. Y.; Liu, J.; Chen, M. D.; Zhang, Q. E.; Au, C. T. Parity alternation of linear ground-state hydrogenated cationic carbon clusters HC_nSi⁺ (n = 1～10). Int. J. Mass Spectrom. 2008, 272, 172-179.

(25) Thorwirth, S.; Harding, M. E. Coupled-cluster calculations of C₂H₂Si and CNHSi structural isomers. J. Chem. Phys. 2009, 130, 214303.

(26) McCarthy, M. C.; Gottlieb, C. A.; Thaddeus, P.; Thorwirth, S.; Gauss, J. Rotational spectra and equilibrium structures of H₂SiS and Si₂S. J. Chem. Phys. 2011, 134, 034306.

(27) Largo, A.; Barrientos, C. Theoretical study of the structures and stabilities of (SiC₂H₂)⁺ species: the reaction of Si⁺ with acetylene. J. Phys. Chem. 1994, 98, 3978-3984.

(28) Redondo, P.; Sagueillo, A.; Barrientos, C.; Largo, A. Theoretical study of the reaction of Si⁺ with C₃H₂. J. Phys. Chem. A 1999, 103, 3310-3320.

(29) Roy D. II; Keith, T.; Millam, J. GaussView 5.0.8. Semichem Inc.: Shawnee Mission KS, 2009.

(30) Frisch, M. J.; Trucks, G. W.; Schlegel, H. B.; Scuseria, G. E.; Robb, M. A.; Cheeseman, J. R.; Montgomery, J. A. Jr.; 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 (Revision D.01). Gaussian Inc.: Wallingford CT 2004.

(31) Lee, C.; Yang, W.; Parr, R. G. Development of the colle-salvetti correlation-energy formula into a functional of the electron density. Phys. Rev. B: Condens. Matter. 1988, 37, 785-789.

(32) Becke, A. D. Density-functional thermochemistry III: the role of exact exchange. J. Chem. Phys. 1993, 98, 5648-5652.

(33) Foresman, J. B.; Frisch, A. Exploring chemistry with electronic structure methods. Gaussian Inc.: Pittsburgh PA 1996.

(34) Purvis, G. D. I.; Bartlett, R. J. A full coupled-cluster singles and doubles model: the inclusion of disconnected triples. J. Chem. Phys. 1982, 76, 1910-1918.

(35) Scuseria, G. E.; Janssen, C. L.; Schaefer, H. F. I. An efficient reformulation of the closed shell coupled cluster single and double excitation (CCSD) equations. J. Chem. Phys. 1988, 89, 7382-7387.

(36) Raghavachari, K.; Trucks, G. W.; Pople, J. A.; Head-Gordon, M. A fifth-order perturbation comparison of electron correlation theories. Chem. Phys. Lett. 1989, 157, 479-483.

(37) Watts, J. D.; Gauss, J.; Bartlett, R. J. Coupled-cluster methods with non-iterative triple excitations for restricted open-shell hartree-fock and other general single-determinant reference functions energies and analytical gradients. J. Chem. Phys. 1993, 98, 8718-8733.

(38) Bartlett, R. J.; Musial, M. Coupled-cluster theory in quantum chemistry. Rev. Mod. Phys. 2007, 79, 291-352.

(39) Liu, Z. Y.; Tang, Z. C.; Huang, R. B.; Zhang, Q.; Zheng, L. S. Experimental and theoretical studies of laser-generated sulfur polycarbon hydride ions: collision-induced dissociation and ab initio calculations. J. Phys. Chem. A 1997, 101, 4019-4025.

(40) Thaddeus, P.; Cummins, S. E.; Linke, R. A.Identification of the SiCC radical toward IRC+10216: the first molecular ring in an astronomical source. Astrophys. J. 1984, 283, L45.

(41) MacKay, D. D. S.; Charnley, S. B. The silicon chemistry of IRC+10216. Mon, N. R. Astron. Soc. 1999, 302, 793.

(42) Van Orden, A.; Saykally, R. J. Small carbon clusters: spectroscopy, structure, and energetics. Chem. Rev. 1998, 98, 2313-2357.

(43) Pascoli, G.; Lavendy, H. Structures and energies of C_nSi⁺ (4 < n < 15) silicon carbide clusters. Int. J. Mass Spectrom. Ion Processes 1998, 173, 41-54.

(44) Lavendy, H.; Robbe, J. M.; Flament, J. P.; Pascoli, G. Density functional study of silicon carbide cluster cations C₄⁺, C₃Si⁺, C₂Si₂⁺, CSi₃⁺ and Si₄⁺. J. Chim. Phys. Pcb. 1997, 94, 1779-1793.

(45) Botschwina, P. An accurate equilibrium structure and CCSD (T) spectroscopic constants for linear C₃Si₂. J. Mol. Spectrosc. 1999, 198, 192-193.

(46) Davico, G. E.; Schwartz, R. L.; Lineberger, W. C. Photoelectron spectroscopy of C₃Si and C₄Si₂ anions. J. Chem. Phys. 2001, 115, 1789-1794.

(47) Pascoli, G.; Lavendy, H. Density functional study of mixed silicon carbide cluster cations C_nSi_p⁺ (n + p = 5, 6). Int. J. Mass Spectrom. 1998, 177, 31-45.

(48) Rao, B. K.; Khanna, S. N.; Jena, P. Equilibrium geometries, magic numbers and electronic structure of small carbon clusters. Solid State Commun. 1986, 58, 53-56.