Quantum confinement and surface chemistry of 0.8-1.6 nm hydrosilylated silicon nanocrystals

doi:10.1088/1674-1056/23/7/076102

中国物理B ›› 2014, Vol. 23 ›› Issue (7): 76102-076102.doi: 10.1088/1674-1056/23/7/076102

• CONDENSED MATTER: STRUCTURAL, MECHANICAL, AND THERMAL PROPERTIES • 上一篇下一篇

Quantum confinement and surface chemistry of 0.8-1.6 nm hydrosilylated silicon nanocrystals

皮孝东, 王蓉, 杨德仁

State Key Laboratory of Silicon Materials and Department of Materials Science and Engineering, Zhejiang University, Hangzhou 310027, China

收稿日期:2013-09-24 修回日期:2014-01-09 出版日期:2014-07-15 发布日期:2014-07-15
基金资助:
Project supported by the National Basic Research Program of China (Grant No. 2013CB632101), the National Natural Science Foundation of China for Excellent Young Researchers (Grant No. 61222404), the Research and Development Program of Ministry of Education of China (Grant No. 62501040202), and the 2012 UAlberta MOST Joint Research Laboratories Program, China.

Quantum confinement and surface chemistry of 0.8-1.6 nm hydrosilylated silicon nanocrystals

Pi Xiao-Dong (皮孝东), Wang Rong (王蓉), Yang De-Ren (杨德仁)

State Key Laboratory of Silicon Materials and Department of Materials Science and Engineering, Zhejiang University, Hangzhou 310027, China

Received:2013-09-24 Revised:2014-01-09 Online:2014-07-15 Published:2014-07-15
Contact: Yang De-Ren E-mail:mseyang@zju.edu.cn
About author:61.46.Hk; 71.15.Mb; 12.38.Aw; 47.55.dr
Supported by:
Project supported by the National Basic Research Program of China (Grant No. 2013CB632101), the National Natural Science Foundation of China for Excellent Young Researchers (Grant No. 61222404), the Research and Development Program of Ministry of Education of China (Grant No. 62501040202), and the 2012 UAlberta MOST Joint Research Laboratories Program, China.

摘要/Abstract

摘要： In the framework of density functional theory (DFT), we have studied the electronic properties of alkene/alkyne-hydrosilylated silicon nanocrystals (Si NCs) in the size range from 0.8 nm to 1.6 nm. Among the alkenes with all kinds of functional groups considered in this work, only those containing -NH₂ and -C₄H₃S lead to significant hydrosilylation-induced changes in the gap between the highest occupied molecular orbital (HOMO) and the lowest unoccupied molecular orbital (LUMO) of an Si NC at the ground state. The quantum confinement effect is dominant for all of the alkene-hydrosilylated Si NCs at the ground state. At the excited state, the prevailing effect of surface chemistry only occurs at the smallest (0.8 nm) Si NCs hydrosilylated with alkenes containing -NH₂ and -C₄H₃S. Although the alkyne hydrosilylation gives rise to a more significant surface chemistry effect than alkene hydrosilylation, the quantum confinement effect remains dominant for alkyne-hydrosilylated Si NCs at the ground state. However, at the excited state, the effect of surface chemistry induced by the hydrosilylation with conjugated alkynes is strong enough to prevail over that of quantum confinement.

关键词: silicon nanocrystals, hydrosilylation, quantum confinement, surface chemistry

Abstract: In the framework of density functional theory (DFT), we have studied the electronic properties of alkene/alkyne-hydrosilylated silicon nanocrystals (Si NCs) in the size range from 0.8 nm to 1.6 nm. Among the alkenes with all kinds of functional groups considered in this work, only those containing -NH₂ and -C₄H₃S lead to significant hydrosilylation-induced changes in the gap between the highest occupied molecular orbital (HOMO) and the lowest unoccupied molecular orbital (LUMO) of an Si NC at the ground state. The quantum confinement effect is dominant for all of the alkene-hydrosilylated Si NCs at the ground state. At the excited state, the prevailing effect of surface chemistry only occurs at the smallest (0.8 nm) Si NCs hydrosilylated with alkenes containing -NH₂ and -C₄H₃S. Although the alkyne hydrosilylation gives rise to a more significant surface chemistry effect than alkene hydrosilylation, the quantum confinement effect remains dominant for alkyne-hydrosilylated Si NCs at the ground state. However, at the excited state, the effect of surface chemistry induced by the hydrosilylation with conjugated alkynes is strong enough to prevail over that of quantum confinement.

Key words: silicon nanocrystals, hydrosilylation, quantum confinement, surface chemistry

中图分类号: (Nanocrystals)

61.46.Hk

71.15.Mb (Density functional theory, local density approximation, gradient and other corrections) 12.38.Aw (General properties of QCD (dynamics, confinement, etc.)) 47.55.dr (Interactions with surfaces)

皮孝东, 王蓉, 杨德仁. Quantum confinement and surface chemistry of 0.8-1.6 nm hydrosilylated silicon nanocrystals[J]. 中国物理B, 2014, 23(7): 76102-076102.

Pi Xiao-Dong (皮孝东), Wang Rong (王蓉), Yang De-Ren (杨德仁). Quantum confinement and surface chemistry of 0.8-1.6 nm hydrosilylated silicon nanocrystals[J]. Chin. Phys. B, 2014, 23(7): 76102-076102.

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Quantum confinement and surface chemistry of 0.8-1.6 nm hydrosilylated silicon nanocrystals

Quantum confinement and surface chemistry of 0.8-1.6 nm hydrosilylated silicon nanocrystals

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