Chemistry Division, Los Alamos National Laboratory, Los Alamos, New Mexico 87545, USA.
Nano Lett. 2010 Jul 14;10(7):2401-7. doi: 10.1021/nl1004652.
The development of nanocrystal quantum dots (NQDs) with suppressed nonradiative Auger recombination has been an important goal in colloidal nanostructure research motivated by the needs of prospective applications in lasing devices, light-emitting diodes, and photovoltaic cells. Here, we conduct single-nanocrystal spectroscopic studies of recently developed core-shell NQDs (so-called "giant" NQDs) that comprise a small CdSe core surrounded by a 16-monolayer-thick CdS shell. Using both continuous-wave and pulsed excitation, we observe strong emission features due both to neutral and charged biexcitons, as well as multiexcitons of higher order. The development of pronounced multiexcitonic peaks in steady-state photoluminescence of individual nanocrystals, as well as continuous growth of the emission intensity in the range of high pump levels, point toward a significant suppression of nonradiative Auger decay that normally renders multiexcitons nonemissive. The unusually high multiexciton emission efficiencies in these systems open interesting opportunities for studies of multiexciton phenomena using well-established methods of single-dot spectroscopy, as well as new exciting prospects for applications, that have previously been hampered by nonradiative Auger decay.
抑制非辐射俄歇复合的纳米晶量子点(NQDs)的发展一直是胶体纳米结构研究的一个重要目标,这是由激光器件、发光二极管和光伏电池等预期应用的需求所驱动的。在这里,我们对最近开发的核壳型 NQDs(所谓的“巨型”NQDs)进行了单纳米晶体光谱研究,这些 NQDs 由一个小的 CdSe 核组成,周围是 16 层厚的 CdS 壳。我们使用连续波和脉冲激发,观察到由于中性和带电双激子以及更高阶的多激子而产生的强烈发射特征。单个纳米晶体的稳态光致发光中明显出现多激子峰,以及在高泵浦水平范围内发射强度的连续增长,表明非辐射俄歇衰减得到了显著抑制,通常情况下,多激子是非发射的。在这些系统中,多激子发射效率异常高,为使用单一点光谱学的成熟方法研究多激子现象以及以前因非辐射俄歇衰减而受到阻碍的新的令人兴奋的应用前景提供了有趣的机会。