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纳米晶体生长中的表面配体动力学

Surface ligand dynamics in growth of nanocrystals.

作者信息

Pradhan Narayan, Reifsnyder Danielle, Xie Renguo, Aldana Jose, Peng Xiaogang

机构信息

Department of Chemistry and Biochemistry, University of Arkansas, Fayetteville, AR 72701, USA.

出版信息

J Am Chem Soc. 2007 Aug 1;129(30):9500-9. doi: 10.1021/ja0725089. Epub 2007 Jul 10.

Abstract

Amine ligands were identified to bond on the surface of CdSe nanocrystals in a dynamic fashion under elevated temperatures in the reproducible growth domain of the specific designed growth reactions. The surface ligand dynamics was found to strongly depend on the growth temperature, the ligand concentration, and the ligand chain length. The strong chain-length dependence was originated from the interligand interactions in the ligand monolayer of a nanocrystal, provided fatty amines being weak ligands for CdSe nanocrystals. When the growth reaction was above the boiling point of an amine ligand, the surface ligand dynamics was violent, a quasi-gas-phase state, indicated by strong temperature-dependent and fast growth rates of the nanocrystals. Approximately below its boiling point, a significantly weak temperature dependence of the growth rate of the nanocrystals associated with the quasi-liquid state of the surface ligands was observed. A direct result of studying the surface ligand dynamics of this well-established nanocrystal system was the formation of high-quality CdSe nanocrystals under much reduced temperature, 150 degrees C, in comparison to the standard 250-350 degrees C temperature range. This was achieved by using fatty amines with a short hydrocarbon chain at a low ligand concentration in the solution. Preliminary results indicate that a similar temperature (160 degrees C) also worked for the growth of InP nanocrystals.

摘要

在特定设计的生长反应的可重复生长区域内,在高温下,胺配体以动态方式键合在CdSe纳米晶体表面。发现表面配体动力学强烈依赖于生长温度、配体浓度和配体链长。强烈的链长依赖性源于纳米晶体配体单层中的配体间相互作用,前提是脂肪胺是CdSe纳米晶体的弱配体。当生长反应高于胺配体的沸点时,表面配体动力学剧烈,呈现准气相状态,这由纳米晶体强烈的温度依赖性和快速生长速率表明。大约在其沸点以下,观察到纳米晶体生长速率与表面配体的准液态相关的明显较弱的温度依赖性。研究这个成熟的纳米晶体系统的表面配体动力学的一个直接结果是,与标准的250-350℃温度范围相比,在低得多的温度(150℃)下形成了高质量的CdSe纳米晶体。这是通过在溶液中使用低浓度的短烃链脂肪胺实现的。初步结果表明,类似的温度(160℃)也适用于InP纳米晶体的生长。

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