Archer Paul I, Santangelo Steven A, Gamelin Daniel R
Department of Chemistry, University of Washington, Seattle, Washington 98195-1700, USA.
J Am Chem Soc. 2007 Aug 8;129(31):9808-18. doi: 10.1021/ja072436l. Epub 2007 Jul 13.
A series of colloidal transition-metal-doped chalcogenide semiconductor nanocrystals (TM2+:CdSe, TM2+:CdS, etc.) has been prepared by thermal decomposition of inorganic cluster precursors. It is shown through extensive spectroscopic and structural characterization that the nanocrystals prepared following literature procedures for synthesis of TM2+:CdSe nanocrystals actually possess an unintended CdSe/TM2+:CdS core/shell morphology. The conditions required for successful formation of TM2+:CdSe and TM2+:CdS by cluster decomposition have been determined. Magneto-optical and photoluminescence spectroscopic results for this series of doped nanocrystals reveal major physical consequences of dopant localization within the shell and demonstrate the capacity to engineer dopant-carrier exchange interactions via core/shell doping strategies. The results presented here illustrate some of the remarkable and unexpected complexities that can arise in nanocrystal doping chemistries and emphasize the need for meticulous characterization to avoid false positives.
通过无机簇前驱体的热分解制备了一系列胶体过渡金属掺杂硫族化物半导体纳米晶体（TM2+：CdSe、TM2+：CdS等）。通过广泛的光谱和结构表征表明，按照文献中合成TM2+：CdSe纳米晶体的方法制备的纳米晶体实际上具有意外的CdSe/TM2+：CdS核/壳形态。已经确定了通过簇分解成功形成TM2+：CdSe和TM2+：CdS所需的条件。该系列掺杂纳米晶体的磁光和光致发光光谱结果揭示了壳层内掺杂剂定位的主要物理后果，并证明了通过核/壳掺杂策略设计掺杂剂-载流子交换相互作用的能力。此处给出的结果说明了纳米晶体掺杂化学中可能出现的一些显著且意想不到的复杂性，并强调了进行细致表征以避免误判的必要性。
