InP-Based Quantum Dots Having an InP Core, Composition-Gradient ZnSeS Inner Shell, and ZnS Outer Shell with Sharp, Bright Emissivity, and Blue Absorptivity for Display Devices
InP-Based Quantum Dots Having an InP Core, Composition-Gradient ZnSeS Inner Shell, and ZnS Outer Shell with Sharp, Bright Emissivity, and Blue Absorptivity for Display Devices
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DOI：
10.1021/acsanm.0c00008
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发表时间：
2020-02-01
影响因子：
5.9
通讯作者：
Yang, Heesun
中科院分区：
文献类型：
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作者：
Jo, Jung-Ho;Jo, Dae-Yeon;Yang, Heesun
磷化铟（InP）被认为是最有希望应用于下一代显示器件的可见量子点（QD）发射体成分，主要是因为它对环境无害。为了实现高效率、宽色域的显示设备，必须追求亮度高、发射率高的InP量子点。基于合成技术的进步，InP量子点的光致发光性能得到了极大的提高，能够保证核心尺寸的均匀性和形成精致的核/壳异质结构。到目前为止，高质量的荧光InP量子点只能通过使用三甲基膦（TMS）(3)P的有害磷(P)前体来实现。在这项工作中，我们报告了一个绿色InP量子点的合成突破，通过使用更便宜，更安全的三（二甲氨基）磷化氢(（DMA)(3)P）的P替代品来实现窄，明亮的发射。为此，QD合成通过所谓的两步方法进行，其中生长的InP岩心经过逐步的尺寸分选过程，然后放置在组成梯度ZnSexS1-x内层和ZnS外层的连续双壳层中。在0.09-0.36范围内改变ZnSexS1-x内壳层的化学成分(x)，探讨其对PL量子产率（QY）、尺寸和蓝激发光吸收率的影响。由于有效的核心尺寸分块和精心设计的异质结构，所得到的InP/ZnSexS1-x/ZnS量子点表现出特殊的绿色（527 nm） PL特征，其锐利的线宽为37 nm，高PL QY为87%，这是迄今为止应用最佳内壳成分时非（TMS）(3) p基量子点所无法实现的。
Indium phosphide (InP) has been regarded as the most promising composition of visible quantum dot (QD) emitters for the application to next-generation display devices primarily because of its environmental benignity. Bright, sharp emissivity of InP QDs should be pursued for the realization of high-efficiency, wide-color gamut display devices. Photoluminescence (PL) performance of InP QDs has been greatly improved based on synthetic advances enabling the securement of core size homogeneity and the formation of exquisite core/shell heterostructure. Until now, high-quality fluorescent InP QDs have been attainable exclusively through the use of a hazardous phosphorus (P) precursor of tris(trimethylsily)phosphine ((TMS)(3)P) against green chemistry. In this work, we report a synthetic breakthrough of green InP QDs toward narrow, bright emissivity by using a much cheaper, safer P alternative of tris(dimethylamino)phosphine ((DMA)(3)P). For this, QD synthesis proceeds via a so-called two-step approach, where as-grown InP cores are subjected to a stepwise size fractionation process and then placed in the consecutive double shelling of a composition-gradient ZnSexS1-x inner and a ZnS outer shell. The chemical composition (x) of the ZnSexS1-x inner shell in the range of 0.09-0.36 is varied to explore its effects on PL quantum yield (QY), size, and blue excitation light absorptivity. Because of the effective core size fractionation and elaborately designed heterostructure, the resulting InP/ZnSexS1-x/ZnS QDs exhibit exceptional green (527 nm) PL features of a sharp line width of 37 nm and a high PL QY of 87%, which have not been achievable to date from non-(TMS)(3)P-based QDs, when an optimal inner shell composition is applied.