Highly emissive Sb3+-doped 0D cesium indium chloride nanocrystals with switchable photoluminescence

Highly emissive Sb3+-doped 0D cesium indium chloride nanocrystals with switchable photoluminescence
Graphical abstract. Credit: Nano Today (2022). DOI: 10.1016/j.nantod.2022.101460

All-inorganic lead-free luminescent metal halide nanocrystals (NCs) are very important in optoelectronics, but their applications are limited by the low photoluminescence (PL) efficiency. It is an effective approach via ns2-metal ions doping for tailoring the optical properties of metal halide NCs and expanding their applications.

However, the PL origin of ns2-metal ion doped metal halides remains controversial and not well understood. Moreover, the controlled synthesis of Sb3+-doped 0D In-based NCs and the size effect on the and dynamics remain unexplored.

In a study published in Nano Today, the research group led by Prof. CHEN Xueyuan from Fujian Institute of Research on the Structure of Matter (FJIRSM) of the Chinese Academy of Sciences (CAS) reported the controlled synthesis of Sb3+-doped 0D Cs3InCl6 NCs with tunable sizes and investigated the effect of NC size on the optical properties and excited-state dynamics of Sb3+.

The researchers obtained 0D Cs3InCl6: Sb3+ NCs with tunable sizes by the controlled synthesis based on a HCl hot-injection method. The as-synthesized NCs exhibit bright green PL with a broad emission band.

They comprehensively surveyed the effects of NC size and Sb3+ concentration on the electronic structures and PL properties of the NCs and the excited-state dynamics of Sb3+ by means of temperature-dependent steady-state and transient PL and ultrafast femtosecond transient absorption (fs-TA) spectroscopies.

Owing to the strong electron-phonon coupling of Sb3+ in the spatially confined 0D structure of Cs3InCl6, Sb3+ ions experienced a dynamic Jahn-Teller distortion in the 3P1 excited state and an off-center position in the 1S0 , which resulted in intense broadband emission of Sb3+ from the inter-configurational 3P11S0 transition with a large Stokes shift and a high PL quantum yield (QY) of 52.3%.

Furthermore, taking advantage of the hydroscopicity of the NCs, the researchers demonstrated the water-triggered chemical transformation of the NCs from green-emitting Cs3InCl6: Sb3+ to orange-emitting Cs2InCl5·H2O: Sb3+ with a PLQY up to 75.3%, thus revealing the superiority of the Sb3+ luminescence in metal halide NCs.

These findings provide fundamental insights into the excited-state dynamics of Sb3+ in 0D In-based halide NCs, thereby laying a foundation for future design of novel lead-free metal halide NCs with tunable structure and switchable PL through ns2-metal ion doping or alloying towards versatile applications such as luminescent chemosensors.

More information: Zhongliang Gong et al, Highly efficient Sb3+ emitters in 0D cesium indium chloride nanocrystals with switchable photoluminescence through water-triggered structural transformation, Nano Today (2022). DOI: 10.1016/j.nantod.2022.101460

Journal information: Nano Today

Citation: Highly emissive Sb3+-doped 0D cesium indium chloride nanocrystals with switchable photoluminescence (2022, May 19) retrieved 25 April 2024 from https://phys.org/news/2022-05-highly-emissive-sb3-doped-0d-cesium.html
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