多孔硅吸附性能的量子化学研究
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摘要
用量子化学方法中的密度泛函理论,在B3LYP/6-31G(d)水平上,采用模型化学方法和Gaussion03程序,计算由不同数目硅原子组成的一维量子线模型和二维网状模型分别吸附氢原子、氧原子、氧分子、硝酸根和高氯酸根的模型进行计算,考察各模型吸附前后的电子状态、能隙、原子电荷、键强等因素,计算结果表明:在吸附有不同原子、分子的多孔硅表面上,表面硅原子与内层硅原子间的化学键均被削弱,对于解释多孔硅的发光和爆炸性质有一定的理论指导意义.
With the methods of model chemistry and DFT calculation,we calculated the model of different number of silicon atoms,which consisted of one dimension quantum line and two dimension net model which of them adsorbed H,O,O2,NO-3,ClO-4,and then we analysed the factors of electron state,energy gap,atom charge and bond intensity on absorbing process of different models.The results showed that on the porous silicon surfaces with different atoms or molecules adsorbed,the chemical bond between the surface silicon atom with an inner layer of silicon atoms were weakened.The research was signficant to the explanation of light and explosion of porous silicon.
With the methods of model chemistry and DFT calculation,we calculated the model of different number of silicon atoms,which consisted of one dimension quantum line and two dimension net model which of them adsorbed H,O,O2,NO-3,ClO-4,and then we analysed the factors of electron state,energy gap,atom charge and bond intensity on absorbing process of different models.The results showed that on the porous silicon surfaces with different atoms or molecules adsorbed,the chemical bond between the surface silicon atom with an inner layer of silicon atoms were weakened.The research was signficant to the explanation of light and explosion of porous silicon.
引文
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[2]Canham L T.Bioactive silicon structure fabrication through nano-etching techniques[J].Adv Mater,1995,7:1033-1037.
[3]Kovacs G T A,Maluf N I,Peteren K E.Bulk Micromachinging of silicon[J].Proceedings of the IEEE,1998,86(8):1536-1551.
[4]Shi J J,Zhu Y F,Baeyens W R G,et al.Recent developments in nanomaterial optical sensors[J].Trends inAnalytical Chemistry,2004,23(5):351-360.
[5]Lehmanna V.Porous silicon matrix for chemical synthesis and chromatograpy[J].Phys Stat sol,2005,202(8):1365-1368.
[6]Ouyang H,Viard R,Miller B L,et al.Macroporous silicon microcavities for macromoleculedetection[J].Adv FunctMater,2005,15:1851-1859.
[7]Fll H,Langa S,Carstensen J,et al.PorousⅢ-Ⅴcompound semiconductors:formation,properties and comparisonto silicon[J].phys stat sol,2003,a197(1):61-70.
[8]Buda F,Kohan J,Parrinello M.Optical propeties of porous silicon:a first-principles study[J].Physical ReviewLetters,1992,69:1272-1275.
[9]Read A J,Needs R J,Nash K J,et al.Firsprinclples calculations of the electronic properties properties silicon quantumwires[J].Physical Review Letters,1992,69:1232-1235.
[10]Ohno T,Shiraishi K,Ogawa T,et al.Intrinsic origin of visible light emission from silicon quantum wires:electronicstructure and geometncally restricted exciton[J].Physical Review Letters,1992,69(16):2400-2403.
[11]Xia J B,Chang Y C.Theory of electronic structure of porous Si[J].Physical Review B,1993,49(5):179-186.
[12]Proot J P,Deleruc,Allen G,et al.Eletruonic structure and optical properties of silicon crystallites[J].AppliedSurface Science,1993,65/66:423-425.
[13]Yeh C Y,Zhang S B,Zunger A.Identity of the light-emitting states in porous silicon wires[J].Applied Physicsletters,1993,63:3455-3457.
[14]施琼玲,魏锡文,李燕飞,等.多孔硅表面状态和吸附性能研究[J].计算机与应用化学,2007,24(2):141-144.