Silicon doping on nanotubular fullerene D5h–C90 from first principles

Author:

Bai, Hongcun   Xue, Ping   Tao, Jia-Yuan   Ji, Wen-Xin   Han, Zhi-Min   Ma, Yujia   Ji, Yongqiang  

Journal:

Computational and Theoretical Chemistry

Issue Date:

2015

Abstract(summary):

Highlights

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Silicon substitution is more favorable to occur near the cap regions of nanotubular fullerene C₉₀.

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Silicon doping could increase the nonlinear optical property of fullerene C₉₀ cage.

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Silicon doping has no much influence on the aromaticity of the nanotubular fullerene C₉₀.

Abstract

This work presented theoretical studies of nanotubular fullerene C₉₀ upon the silicon substitutional doping by means of density functional theory combined with self-consistent field molecular orbital method. The doping effect on geometrical structure, relative stability, defect formation energy, electronic property, nonlinear optical property and aromaticity of the tube-shaped C₉₀ fullerene has been addressed systemically and in details with B3LYP method. It is observed that the silicon atoms exhibit extroversion trend in the doped structure. The obtained defect formation energy is in the range of 4.861–5.231 eV for the doped C₉₀ studied, and the substitutionally doping the C₉₀ by Si atom is more favorable to occur near the cap region according to the calculated defect formation energies. The distributions for the highest occupied molecular orbital of the doped C₉₀ are approach to that of the pure C₉₀ fullerene. However, the lowest unoccupied orbital of most doped C₉₀ exhibit obvious localization at the silicon site. To study the nonlinear optical property of the doped structures, the third-order nonlinear optical constant, γ is computed with finite-field method. The enhanced values of nonlinear optical constant of the fullerenes upon silicon doping are observed and understand by γ density analysis. Moreover, the doping effect on the aromaticity of the nanotubular is also studied based on the probe of nuclear independent chemical shift.

Graphical abstract

Page:

138-146