Engineering Brightness Matched Indium Phosphide Quantum Dots.
Engineering Brightness Matched Indium Phosphide Quantum Dots.
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工程亮度匹配磷化型量子点。
DOI：
10.1021/acs.chemmater.0c03181
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发表时间：
2021-03-23
期刊：
影响因子：
--
通讯作者：
Dennis AM
中科院分区：
文献类型：
--
作者：
Toufanian R;Chern M;Kong VH;Dennis AM
半导体纳米晶体量子点的尺寸相关光电性质对颜色可调性有很大的好处，但在发射不同颜色的量子点中会导致固有的相对发光亮度不匹配，因为较大的发射体比较小的粒子吸收更多的入射光子。在这里，我们考察了在不同的激发波长下，核的组成、壳的组成和壳的厚度对量子点的光学性质的影响，包括高能量吸收、量子产率(QY)以及InP/ZnS和InP/ZnSe核/壳和InP/ZnSe核/壳的相对亮度。我们的分析表明，中间层的存在改变了增强吸收的起始波长，并导致了高度激发波长依赖性的量子发光。从商用的CdSe/ZnS转换到InP/ZnS，将绿色和红色发射器之间的亮度不匹配从33倍减少到5倍。在量子点异质结中加入一层4层厚的光吸收ZnSe壳层，并在油酸锌和三辛基膦的溶液中加热量子点，得到的InP/ZnSe/ZnS量子点比InP/ZnS量子点的亮度高约10倍。与由于准II型能带结构而只能在红色波长发光且具有较厚的CDS壳层的CdSe/CDS核/壳/壳量子点不同，I型InP/ZnSe/ZnS量子点特别适合于创建可见发射、亮度匹配的发射体的彩虹。通过调整中间层的厚度，得到了无重金属、亮度匹配的绿色和红色发射体。这项研究强调了通过异质核/壳InP基量子点的协同材料设计来克服量子点固有的亮度不匹配的能力。基于其基本结构，红色发射半导体量子点(QD)比相同组成的绿色发射粒子更大、更亮。不同厚度的中间ZnSe壳层增强了InP/ZnSe/ZnS核/壳/壳量子点的吸收，产生了跨越可见波长范围的第一道彩虹，即亮度匹配的无镉量子点。
The size-dependent optoelectronic properties of semiconductor nanocrystals quantum dots (QDs) are hugely beneficial for color tunability but induce an inherent relative PL brightness mismatch in QDs emitting different colors, as larger emitters absorb more incident photons than smaller particles. Here, we examine the effect of core composition, shell composition, and shell thickness on optical properties including high energy absorption, quantum yield (QY), and the relative brightness of InP/ZnS and InP/ZnSe core/shell and InP/ZnSe/ZnS core/shell/shell QDs at different excitation wavelengths. Our analysis reveals that the presence of an intermediate ZnSe shell changes the wavelength of enhanced absorption onset and leads to highly excitation wavelength dependent QYs. Switching from commercial CdSe/ZnS to InP/ZnS reduces the brightness-mismatch between green and red emitters from 33- to 5-fold. Incorporating a 4-monolayer thick optically absorbing ZnSe shell into the QD heterostructure and heating the QDs in a solution of zinc oleate and trioctylphosphine produces InP/ZnSe/ZnS QDs that are ~10-fold brighter than their InP/ZnS counterparts. In contrast to CdSe/CdS/ZnS core/shell/shell QDs, which only photoluminesce at red wavelengths with thicker CdS shells due to their Quasi-Type II bandstructure, Type I InP/ZnSe/ZnS QDs are uniquely suited to creating a rainbow of visible-emitting, brightness matched emitters. By tailoring the thickness of the intermediate ZnSe shell, heavy metal-free, brightness-matched green and red emitters are produced. This study highlights the ability to overcome the inherent brightness mismatch seen in QDs through concerted materials design of heterostructured core/shell InP-based QDs. Based on their fundamental structure, red-emitting semiconductor quantum dots (QDs) are larger and brighter than green-emitting particles of the same composition. An intermediate ZnSe shell of varying thickness enhances the absorption of InP/ZnSe/ZnS core/shell/shell QDs to produce the first rainbow of brightness-matched, cadmium-free QDs spanning the visible wavelength range.
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