Electronic Structure Insights into the Tunable Luminescence of CuAlxFe1–xS2/ZnS Nanocrystals,The Journal of Physical Chemistry C

当前位置： X-MOL 学术 › J. Phys. Chem. C › 论文详情

Our official English website, www.x-mol.net, welcomes your feedback! (Note: you will need to create a separate account there.)

Electronic Structure Insights into the Tunable Luminescence of CuAlxFe1–xS2/ZnS Nanocrystals
The Journal of Physical Chemistry C ( IF 3.3 ) Pub Date : 2021-01-20 , DOI: 10.1021/acs.jpcc.0c09009
Ranjana Yadav _{1,

2} , Biswajit Bhattacharyya ₁ , Subham Kumar Saha ₁ , Pranab Dutta ₁ , Parna Roy ₁ , Guru Pratheep Rajasekar ₁ , Awadhesh Narayan ₁ , Anshu Pandey ₁

Affiliation

We describe the electronic structure and spectroscopic properties of CuAl_xFe_1–xS₂ nanocrystals and their core/shell structures. The as-synthesized CuAl_xFe_1–xS₂ core exhibits a tetragonal chalcopyrite structure. The core material exhibits tunable band gap that spans the entire visible to near-infrared spectrum, from 3.48 to 0.53 eV. This tunability is achieved by varying the mole fraction of aluminum and iron from 1:0 to 0:1. The band gap variation with composition deviates from Vegard’s law and corresponds to a bowing coefficient of 1.59 eV. Our observations are interpreted using density functional theoretical calculations. In particular, we find that the significant bowing is well accounted for through significant localization of the Fe electronic states. Most significantly, CuAl_xFe_1–xS₂ shows photoluminescence upon making a shell of zinc sulfide, which is tunable from 400 to 1400 nm (3.1 to 0.89 eV). CuAl_xFe_1–xS₂/ZnS are until date the only visible-infrared tunable nanocrystal fluorophore composed entirely of earth abundant elements with atomic numbers 30 and lower.

中文翻译：

电子结构洞察CuAl _x Fe _{1– x} S ₂ / ZnS纳米晶体的可调发光

我们描述了CuAl _x Fe _{1– x} S ₂纳米晶体及其核/壳结构的电子结构和光谱性质。合成后的CuAl _x Fe _{1– x} S ₂核表现出四方黄铜矿结构。核心材料的可调谐带隙范围从3.48 eV到0.53 eV，涵盖了整个可见光谱到近红外光谱。通过将铝和铁的摩尔分数从1：0更改为0：1，可以实现这种可调性。带隙随组成的变化背离了Vegard定律，对应的弯曲系数为1.59 eV。我们的观察结果使用密度泛函理论计算来解释。尤其是，我们发现通过Fe电子态的显着局域性可以很好地解决明显的弯曲。最重要的是，CuAl _x Fe _{1– x} S ₂图1显示了在制作硫化锌壳时的光致发光，该硫化锌可在400至1400 nm（3.1至0.89 eV）之间调节。迄今为止，CuAl _x Fe _{1 – x} S ₂ / ZnS是唯一的完全由原子序数为30或更低的富含地球的元素组成的可见红外可调谐纳米晶体荧光团。

更新日期：2021-02-04

点击分享查看原文

点击收藏

阅读更多本刊最新论文本刊介绍/投稿指南11