Institute of Physics of the ASCR, vvi, Cukrovarnicka 10, 162 53 Prague 6, Czech Republic.
ACS Nano. 2010 Aug 24;4(8):4495-504. doi: 10.1021/nn1005182.
Silicon nanocrystals are an extensively studied light-emitting material due to their inherent biocompatibility and compatibility with silicon-based technology. Although they might seem to fall behind their rival, namely, direct band gap based semiconductor nanocrystals, when it comes to the emission of light, room for improvement still lies in the exploitation of various surface passivations. In this paper, we report on an original way, taking place at room temperature and ambient pressure, to replace the silicon oxide shell of luminescent Si nanocrystals with capping involving organic residues. The modification of surface passivation is evidenced by both Fourier transform infrared spectroscopy and nuclear magnetic resonance measurements. In addition, single-nanocrystal spectroscopy reveals the occurrence of a systematic fine structure in the emission single spectra, which is connected with an intrinsic property of small nanocrystals since a very similar structure has recently been observed in specially passivated semiconductor CdZnSe nanoparticles. The organic capping also dramatically changes optical properties of Si nanocrystals (resulting ensemble photoluminescence quantum efficiency 20%, does not deteriorate, radiative lifetime 10 ns at 550 nm at room temperature). Optically clear colloidal dispersion of these nanocrystals thus exhibits properties fully comparable with direct band gap semiconductor nanoparticles.
硅纳米晶体是一种被广泛研究的发光材料,因为它们具有固有的生物相容性和与硅基技术的兼容性。尽管它们在发光方面可能落后于其竞争对手,即直接带隙半导体纳米晶体,但在发光方面仍有改进的空间,这在于对各种表面钝化的开发。在本文中,我们报告了一种在室温常压下用涉及有机残留物的封端取代发光 Si 纳米晶体的氧化硅壳的原始方法。表面钝化的修饰通过傅里叶变换红外光谱和核磁共振测量得到了证实。此外,单纳米晶体光谱揭示了发射单光谱中系统的精细结构的发生,这与小纳米晶体的固有特性有关,因为最近在经过特殊钝化的半导体 CdZnSe 纳米粒子中观察到了非常相似的结构。有机封端也显著改变了 Si 纳米晶体的光学性质(导致整体光致发光量子效率为 20%,不会恶化,在室温下 550nm 处的辐射寿命为 10ns)。这些纳米晶体的光学透明胶体分散体因此表现出与直接带隙半导体纳米粒子完全可比的性质。