Interdiffusion-enhanced cation exchange for HgSe and HgCdSe nanocrystals with infrared bandgaps

0 CHEMISTRY, MULTIDISCIPLINARY Nature synthesis Pub Date : 2024-07-03 DOI:10.1038/s44160-024-00597-3
Wonseok Lee, Andrew M. Smith
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Abstract

Colloidal semiconductor nanocrystals based on CdSe have been precisely optimized for photonic applications in the visible spectrum, with modern products exhibiting structural uniformity, near 100% quantum yield and linewidths narrower than 100 meV. Here we report homogeneous nanocrystals with tunable bandgaps in the infrared spectrum based on HgSe and HgxCd1−xSe alloys deriving from CdSe precursors. We find that Ag+ catalyses cation interdiffusion to reduce the CdSe–HgSe alloying temperature from 250 °C to 80 °C. Together with ligands that modulate surface cation exchange rates, interdiffusion-enhanced Hg2+ exchange of diverse CdSe nanocrystals proceeds homogeneously and completely. The products retain the size, shape and uniformity of the parent nanocrystals but exhibit enhanced absorption. After passivation with heteroepitaxial CdZnS shells, photoluminescence wavelengths are tunable in the shortwave infrared by composition without changing size, with 80–91% quantum yield and linewidths near 100 meV. These materials may find applications in infrared photonic devices and infrared bioimaging. CdSe nanocrystals are used as synthetic templates for HgSe and alloyed HgxCd1−xSe nanocrystals with tunable, diverse structures. Cd2+-to-Hg2+ exchange occurs homogeneously and completely through interdiffusion enhancement with Ag+ catalysts and with surface cation exchange modulated by alkylthiol ligands.

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具有红外带隙的 HgSe 和 HgCdSe 纳米晶体的互扩散增强型阳离子交换
基于硒化镉的胶体半导体纳米晶体已针对可见光谱中的光子应用进行了精确优化,其现代产品表现出结构均匀性、接近 100% 的量子产率以及小于 100 meV 的线宽。在此,我们报告了基于硒化镉前驱体的 HgSe 和 HgxCd1-xSe 合金的在红外光谱中具有可调带隙的同质纳米晶体。我们发现,Ag+ 催化阳离子相互扩散,将 CdSe-HgSe 合金温度从 250 °C 降低到 80 °C。与调节表面阳离子交换率的配体一起,相互扩散增强的 Hg2+ 交换在不同的 CdSe 纳米晶体中均匀、完全地进行。生成物保留了母体纳米晶体的尺寸、形状和均匀性,但吸收能力增强。用异质外延 CdZnS 壳钝化后,光致发光波长在短波红外范围内可根据成分进行调节,而不会改变尺寸,量子产率为 80-91%,线宽接近 100 meV。这些材料可应用于红外光子器件和红外生物成像。
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