The interface microenvironment mediates the emission of a semiconductor nanocluster via surface-dopant-involving direct charge transfer

Zhiqiang Wang; Hao Ma; Jiaxu Zhang; Yingjia Lan; Jia-Xing Liu; Shang-Fu Yuan; Xiao-Ping Zhou; Xiaohong Li; Chaochao Qin; Dong-Sheng Li; Tao Wu

doi:10.1039/D3SC03091A

The interface microenvironment mediates the emission of a semiconductor nanocluster via surface-dopant-involving direct charge transfer†

Zhiqiang Wang,‡^ab Hao Ma,‡^a Jiaxu Zhang,‡^ab Yingjia Lan,‡^b Jia-Xing Liu,^a Shang-Fu Yuan,

^a Xiao-Ping Zhou,

^a Xiaohong Li,^b Chaochao Qin,^c Dong-Sheng Li

^d and Tao Wu

*^ab

Author affiliations

* Corresponding authors

^a College of Chemistry and Materials Science, Guangdong Provincial Key Laboratory of Functional Supramolecular Coordination Materials and Applications, Jinan University, Guangzhou 510632, China
E-mail: wutao@jnu.edu.cn

^b College of Chemistry, Chemical Engineering and Materials Science, Soochow University, Suzhou, Jiangsu 215123, China

^c Henan Key Laboratory of Infrared Materials & Spectrum Measures and Applications, School of Physics, Henan Normal University, Xinxiang 453007, China

^d College of Materials and Chemical Engineering, Hubei Provincial Collaborative Innovation Center for New Energy Microgrid, Key Laboratory of Inorganic Nonmetallic Crystalline and Energy Conversion Materials, China Three Gorges University, Yichang, Hubei 443002, China

Abstract

The interface microenvironment of doped quantum dots (QDs) is crucial in optimizing the properties associated with the photogenerated excitons. However, the imprecision of QDs' surface structures and compositions impedes a thorough understanding of the modulation mechanism caused by the complex interface microenvironment, particularly distinguishing the contribution of surface dopants from inner ones. Herein, we investigated interface-mediated emission using a unique model of an atomically precise chalcogenide semiconductor nanocluster containing uniform near-surface Mn²⁺ dopants. Significantly, we discovered that Mn²⁺ ions can directly transfer charges with hydrogen-bonding-bound electron-rich alkylamines with matched molecular configurations and electronic structures at the interface. This work provides a new pathway, the use of atomically precise nanoclusters, for analyzing and enhancing the interface-dependent properties of various doped QDs, including chalcogenides and perovskites.

Chemical Science

The interface microenvironment mediates the emission of a semiconductor nanocluster via surface-dopant-involving direct charge transfer†

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The interface microenvironment mediates the emission of a semiconductor nanocluster via surface-dopant-involving direct charge transfer

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