Chemical insight into the origin of red and blue photoluminescence arising from freestanding silicon nanocrystals.
Chemical insight into the origin of red and blue photoluminescence arising from freestanding silicon nanocrystals.
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DOI：
10.1021/nn4000644
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发表时间：
2013-03-26
期刊：
影响因子：
17.1
通讯作者：
Veinot, Jonathan G. C.
中科院分区：
文献类型：
--
作者：
Dasog, Mita;Yang, Zhenyu;Regli, Sarah;Atkins, Tonya M.;Faramus, Angelique;Singh, Mani P.;Muthuswamy, Elayaraja;Kauzlarich, Susan M.;Tilley, Richard D.;Veinot, Jonathan G. C.
硅纳米晶是一种极具吸引力的功能材料。它们与标准电子和通信平台兼容，并且具有生物相容性。已经开发了许多方法来实现尺寸控制的Si NC合成。虽然这些过程产生看起来相同的Si NC，但它们的光学响应可能会显着不同。使用高温方法制备的Si NC通常表现出与有效质量近似（EMA）一致的光致发光，而通过溶液方法制备的那些表现出在某种程度上与颗粒尺寸无关的蓝光发射。尽管提出了许多建议，但至少十年来，对这种差异的明确解释一直难以捉摸。这种明显的二分法使我们对Si NC性质的理解产生了疑问，并潜在地限制了它们的应用范围。目前的贡献朝着确定蓝色发射的起源迈出了实质性的一步，这是基于EMA预测所不期望的。它描述了从三个最广泛引用的程序获得的Si NC的详细比较，以及在暴露于含氮试剂时红色发光的Si NC向蓝色发光体的转化。证据的分析与Si NC中甚至在ppm水平下痕量氮和氧的存在引起蓝色发射的假设一致。
Silicon nanocrystals (Si NCs) are attractive functional materials. They are compatible with standard electronics and communications platforms as well being biocompatible. Numerous methods have been developed to realize size-controlled Si NC synthesis. While these procedures produce Si NCs that appear identical, their optical responses can differ dramatically. Si NCs prepared using high-temperature methods routinely exhibit photoluminescence agreeing with the effective mass approximation (EMA), while those prepared via solution methods exhibit blue emission that is somewhat independent of particle size. Despite many proposals, a definitive explanation for this difference has been elusive for no less than a decade. This apparent dichotomy brings into question our understanding of Si NC properties and potentially limits the scope of their application. The present contribution takes a substantial step forward toward identifying the origin of the blue emission that is not expected based upon EMA predictions. It describes a detailed comparison of Si NCs obtained from three of the most widely cited procedures as well as the conversion of red-emitting Si NCs to blue-emitters upon exposure to nitrogen containing reagents. Analysis of the evidence is consistent with the hypothesis that the presence of trace nitrogen and oxygen even at the ppm level in Si NCs gives rise to the blue emission.
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