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在纳米多孔阳极氧化铝膜中尺寸可控的硅量子点的空间受限合成氧化硅纳米棒。

Spatially confined synthesis of SiOx nano-rod with size-controlled Si quantum dots in nano-porous anodic aluminum oxide membrane.

作者信息

Pai Yi-Hao, Lin Gong-Ru

机构信息

Institute of Photonics and Optoelectronics, Department of Electrical Engineering, National Taiwan University, Taipei, Taiwan.

出版信息

Opt Express. 2011 Jan 17;19(2):896-905. doi: 10.1364/OE.19.000896.

Abstract

By depositing Si-rich SiOx nano-rod in nano-porous anodic aluminum oxide (AAO) membrane using PECVD, the spatially confined synthesis of Si quantum-dots (Si-QDs) with ultra-bright photoluminescence spectra are demonstrated after low-temperature annealing. Spatially confined SiOx nano-rod in nano-porous AAO membrane greatly increases the density of nucleated positions for Si-QD precursors, which essentially impedes the route of thermally diffused Si atoms and confines the degree of atomic self-aggregation. The diffusion controlled growth mechanism is employed to determine the activation energy of 6.284 kJ mole(-1) and diffusion length of 2.84 nm for SiO1.5 nano-rod in nano-porous AAO membrane. HRTEM results verify that the reduced geometric dimension of the SiOx host matrix effectively constrain the buried Si-QD size at even lower annealing temperature. The spatially confined synthesis of Si-QD essentially contributes the intense PL with its spectral linewidth shrinking from 210 to 140 nm and its peak intensity enhancing by two orders of magnitude, corresponding to the reduction on both the average Si-QD size and its standard deviation from 2.6 to 2.0 nm and from 25% to 12.5%, respectively. The red-shifted PL wavelength of the Si-QD reveals an inverse exponential trend with increasing temperature of annealing, which is in good agree with the Si-QD size simulation via the atomic diffusion theory.

摘要

通过等离子体增强化学气相沉积(PECVD)法在纳米多孔阳极氧化铝(AAO)膜中沉积富硅的氧化硅纳米棒,经低温退火后,实现了具有超亮光致发光光谱的硅量子点(Si-QDs)的空间受限合成。纳米多孔AAO膜中的空间受限氧化硅纳米棒极大地增加了Si-QD前驱体的成核位置密度,这从根本上阻碍了硅原子的热扩散路径,并限制了原子自聚集程度。采用扩散控制生长机制确定了纳米多孔AAO膜中SiO1.5纳米棒的活化能为6.284 kJ·mol⁻¹,扩散长度为2.84 nm。高分辨率透射电子显微镜(HRTEM)结果证实,即使在更低的退火温度下,氧化硅主体基质减小的几何尺寸也有效地限制了埋入的Si-QD尺寸。Si-QD的空间受限合成本质上导致了强烈的光致发光,其光谱线宽从210 nm缩小到140 nm,峰值强度提高了两个数量级,这分别对应于平均Si-QD尺寸及其标准偏差从2.6 nm减小到2.0 nm以及从25%减小到12.5%。Si-QD的光致发光波长红移显示出随着退火温度升高呈反指数趋势,这与通过原子扩散理论进行的Si-QD尺寸模拟结果高度吻合。

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