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Mechanism of Fluorescent Silicon Nanoparticles

机译:荧光硅纳米粒子的机理

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Silicon (Si) is known to have an indirect bandgap transition, which means it has poor fluorescence properties. However, when engineered into sub-nm sized particles, Si nanoparticles become emissive due to quantum confinement. However, in unmodified Si particles, this effect is limited to generating red or near-infrared emission with low quantum yield. To resolve these limitations, surface-modification methods have successfully generated Si particles that emit in the blue, cyan, and green with quantum yields up to ~90%. These modifications have also made the Si nanoparticles water-soluble, making them promising in biological applications. To date, the mechanism of emission in these species is still unclear although it has been speculated that charge transfer of Si-O-N could be responsible. To investigate whether emission by these Si nanoparticles proceeds via a charge transfer mechanism, Stark spectroscopy is used. In this method, an external electric field is applied to the Si nanoparticles. Changes in the absorption and/or emission spectra due to the applied field can be taken as strong evidence for a charge transfer mechanism. From the results of Stark spectroscopy, Si nanoparticles are revealed to have ligand to metal charge transfer mechanism along with electric-field quenching, which is useful information for utilization into applications. Addition to the information found, a method of how to tune the emission maxima based on selection of ligands is prosed.
机译:已知硅(Si)具有间接带隙跃迁,这意味着其荧光性能较差。但是,当将其设计成亚纳米尺寸的颗粒时,由于量子限制,Si纳米颗粒会发光。但是,在未改性的Si颗粒中,这种影响仅限于以低量子产率产生红色或近红外发射。为了解决这些局限性,表面改性方法成功地生成了以蓝色,青色和绿色发光的硅粒子,其量子产率高达〜90%。这些修饰还使Si纳米颗粒具有水溶性,使其在生物学应用中很有前途。迄今为止,尽管已经推测这些物种的发射机理尚不清楚,但据推测可能是Si-O-N电荷转移的原因。为了研究这些Si纳米粒子的发射是否通过电荷转移机制进行,使用了Stark光谱。在该方法中,将外部电场施加至Si纳米颗粒。由于施加的电场引起的吸收光谱和/或发射光谱的变化可以作为电荷转移机制的有力证据。根据Stark光谱的结果,发现Si纳米颗粒具有配体到金属的电荷转移机制以及电场猝灭,这对于应用中的应用是有用的信息。除了发现的信息外,还提出了一种基于配体选择来调节发射最大值的方法。

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