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Growth of Multinary Copper-Based Sulfide Shells on CuInSe2 Nanocrystals for Significant Improvement of Their Near-Infrared Emission
Chemistry of Materials ( IF 7.2 ) Pub Date : 2020-08-31 , DOI: 10.1021/acs.chemmater.0c02500 Jiajia Ning 1 , Yuan Xiong 2 , Fei Huang 3, 4 , Zonghui Duan 1 , Stephen V. Kershaw 1 , Andrey L. Rogach 1
Chemistry of Materials ( IF 7.2 ) Pub Date : 2020-08-31 , DOI: 10.1021/acs.chemmater.0c02500 Jiajia Ning 1 , Yuan Xiong 2 , Fei Huang 3, 4 , Zonghui Duan 1 , Stephen V. Kershaw 1 , Andrey L. Rogach 1
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A range of different copper-based sulfide shells, such as CuInS2, CuInZnS2, CuInS2-xSex, and CuInZnS2-xSex, have been grown on CuInSe2 (CISe) nanocrystals (NCs) in order to improve their photoluminescence quantum yield (PLQY). Starting from initial CISe core NCs with PLQY of 0.4%, the deposition of the CuInS2 shell has increased the PLQY to 4.5%, while introducing Zn or Se elements into the CuInS2 shell to form cation-alloyed CuInZnS2 or anion-alloyed CuInS2-xSex shells improved their PLQYs to 8% and 11%, respectively. Limitations on PLQY for the mentioned shell materials were related to the lattice mismatch with the CISe core material, and the band gap alignment in the core/shell NCs for quasi type-II nanostructures. This could be mitigated by growing a multinary CuInZnS2-xSex shell on the CISe core NCs, which resulted in further improvement of their PLQY to 20% for the emission centered at 920 nm. This study offers guidance for the rational selection of copper-based sulfide shell materials that are able to significantly improve the PLQY of heavy-metal free CISe NCs in the near-infrared spectral range of 834–1028 nm, which is relevant for biological labeling, optoelectronics, and sensing.
中文翻译：
在CuInSe 2纳米晶体上生长多元铜基硫化物壳，以显着改善其近红外发射
不同铜基硫化物壳如的CuInS的范围2，CuInZnS 2，的CuInS 2- X硒X，和CuInZnS 2- X硒X，已经生长在的CuInSe 2，以便（CISE）纳米晶体（NCS），以改善它们的光致发光量子产率（PLQY）。从0.4％PLQY初始CISE芯的NC开始，的CuInS的沉积2壳具有PLQY提高到4.5％，同时引入Zn或硒元素带入的CuInS 2壳以形成阳离子合金CuInZnS 2或阴离子合金的CuInS 2- x Se x炮弹的PLQY分别提高了8％和11％。上述壳材料的PLQY限制与与CISe核材料的晶格失配以及准II型纳米结构在核/壳NC中的带隙排列有关。可以通过在CISe核心NC上生长多层CuInZnS 2- x Se x壳来缓解这种情况，这对于以920 nm为中心的发射将PLQY进一步提高到20％。这项研究为合理选择铜基硫化物壳材料提供了指导，这些材料能够在834-1028 nm的近红外光谱范围内显着提高不含重金属的CISe NCs的PLQY，这与生物标记有关，光电和传感。
更新日期：2020-09-22
中文翻译：
在CuInSe 2纳米晶体上生长多元铜基硫化物壳，以显着改善其近红外发射
不同铜基硫化物壳如的CuInS的范围2，CuInZnS 2，的CuInS 2- X硒X，和CuInZnS 2- X硒X，已经生长在的CuInSe 2，以便（CISE）纳米晶体（NCS），以改善它们的光致发光量子产率（PLQY）。从0.4％PLQY初始CISE芯的NC开始，的CuInS的沉积2壳具有PLQY提高到4.5％，同时引入Zn或硒元素带入的CuInS 2壳以形成阳离子合金CuInZnS 2或阴离子合金的CuInS 2- x Se x炮弹的PLQY分别提高了8％和11％。上述壳材料的PLQY限制与与CISe核材料的晶格失配以及准II型纳米结构在核/壳NC中的带隙排列有关。可以通过在CISe核心NC上生长多层CuInZnS 2- x Se x壳来缓解这种情况，这对于以920 nm为中心的发射将PLQY进一步提高到20％。这项研究为合理选择铜基硫化物壳材料提供了指导，这些材料能够在834-1028 nm的近红外光谱范围内显着提高不含重金属的CISe NCs的PLQY，这与生物标记有关，光电和传感。
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