Center for Chemistry of Novel & High-Performance Materials, and Department of Chemistry, Zhejiang University , Hangzhou 310027, PR China.
J Am Chem Soc. 2017 Mar 8;139(9):3302-3311. doi: 10.1021/jacs.6b11431. Epub 2017 Feb 15.
Colloidal quantum dots are promising optical and optoelectronic materials for various applications, whose performance is dominated by their excited-state properties. This article illustrates synthetic control of their excited states. Description of the excited states of quantum-dot emitters can be centered around exciton. We shall discuss that, different from conventional molecular emitters, ground-state structures of quantum dots are not necessarily correlated with their excited states. Synthetic control of exciton behavior heavily relies on convenient and affordable monitoring tools. For synthetic development of ideal optical and optoelectronic emitters, the key process is decay of band-edge excitons, which renders transient photoluminescence as important monitoring tool. On the basis of extensive synthetic developments in the past 20-30 years, synthetic control of exciton behavior implies surface engineering of quantum dots, including surface cation/anion stoichiometry, organic ligands, inorganic epitaxial shells, etc. For phosphors based on quantum dots doped with transition metal ions, concentration and location of the dopant ions within a nanocrystal lattice are found to be as important as control of the surface states in order to obtain bright dopant emission with monoexponential yet tunable photoluminescence decay dynamics.
胶体量子点是一类很有前途的光学和光电材料,在很多应用中都有出色的表现,而它们的性能主要取决于其激发态特性。本文介绍了对其激发态的合成控制。量子点发射器的激发态描述可以以激子为中心。我们将讨论,与传统的分子发射器不同,量子点的基态结构不一定与其激发态相关。激子行为的合成控制严重依赖于方便且负担得起的监测工具。对于理想的光学和光电发射器的合成发展,关键过程是带边激子的衰减,这使得瞬态光致发光成为重要的监测工具。在过去 20-30 年的广泛合成发展的基础上,激子行为的合成控制意味着对量子点进行表面工程,包括表面阳离子/阴离子化学计量比、有机配体、无机外延壳等。对于基于过渡金属离子掺杂的量子点荧光粉,发现纳米晶格内掺杂离子的浓度和位置与控制表面态一样重要,这样才能获得具有单指数衰减且可调的磷光衰减动力学的明亮掺杂发射。