McKetta Department of Chemical Engineering, Texas Materials Institute, Center for Nano- and Molecular Science and Technology, The University of Texas at Austin , Austin, Texas 78712, United States.
Department of Chemistry, Northwestern University , Evanston, Illinois 60439, United States.
Nano Lett. 2017 Sep 13;17(9):5580-5586. doi: 10.1021/acs.nanolett.7b02386. Epub 2017 Aug 4.
Auger recombination lifetimes, absorption cross sections, and the quantum yields of carrier multiplication (CM), or multiexciton generation (MEG), were determined for solvent-dispersed silicon (Si) nanorods using transient absorption spectroscopy (TAS). Nanorods with an average diameter of 7.5 nm and aspect ratios of 6.1, 19.3, and 33.2 were examined. Colloidal Si nanocrystals of similar diameters were also studied for comparison. The nanocrystals and nanorods were passivated with organic ligands by hydrosilylation to prevent surface oxidation and limit the effects of surface trapping of photoexcited carriers. All samples used in the study exhibited relatively efficient photoluminescence. The Auger lifetimes increased with nanorod length, and the nanorods exhibited higher CM quantum yield and efficiency than the nanocrystals with a similar band gap energy E. Beyond a critical length, the CM quantum yield decreases. Nanorods with the aspect ratio of 19.3 had the highest CM quantum yield of 1.6 ± 0.2 at 2.9E, which corresponded to a multiexciton yield that was twice as high as observed for the spherical nanocrystals.
利用瞬态吸收光谱(TAS)测定了分散在溶剂中的硅(Si)纳米棒的俄歇复合寿命、吸收截面和载流子倍增(CM)或多激子产生(MEG)的量子产率。研究了平均直径为 7.5nm 且纵横比分别为 6.1、19.3 和 33.2 的纳米棒。还研究了具有相似直径的胶体硅纳米晶作为对比。通过硅氢加成反应对纳米晶和纳米棒进行有机配体钝化,以防止表面氧化并限制光激发载流子的表面捕获的影响。研究中使用的所有样品都表现出相对高效的光致发光。俄歇寿命随纳米棒长度的增加而增加,纳米棒表现出比具有相似能带隙能量 E 的纳米晶更高的 CM 量子产率和效率。超过临界长度后,CM 量子产率下降。纵横比为 19.3 的纳米棒在 2.9E 时具有最高的 CM 量子产率 1.6±0.2,这对应于多激子产率,是观察到的球形纳米晶的两倍。