Hexagonal-phase NaYF4 (β-NaYF4) has been acknowledged to be one of the most efficient doping hosts to prepare bright lanthanide-doped luminescent nano-bioprobes for various biomedical applications. However, to date, it remains a great challenge to synthesize ultra-bright lanthanide-doped β-NaYF4 nano-bioprobes under a low reaction temperature by using conventional synthetic methods. Herein, we first develop an acetic acid (HAc)-mediated coprecipitation method for the preparation of ultra-bright lanthanide-doped β-NaYF4 nanoprobes under a low reaction temperature at 200 °C. Based on a series of comparative spectroscopic investigations, we show that the use of HAc in the reaction environment can not only promote the rapid α–β phase transformation of NaYF4 host at 200 °C within 1 h but also boost the absolute photoluminescence quantum yield (PLQY) of NaYF4 nanocrystals to 30.68% for near-infrared emission and to 3.79% for upconversion luminescence, both of which are amongst the highest values for diverse lanthanide-doped luminescent nanocrystals ever reported. By virtue of their superior near-infrared luminescence, we achieve optical-guided dynamic vasculature imaging in vivo of the whole body at a high spatial resolution (23.8 µm) under 980 nm excitation, indicating its potential for the diagnosis and treatment evaluation of vasculature-related diseases.
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Self-trapped excitons (STEs) emission from halide perovskites with strong exciton-phonon coupling has attracted considerable attention due to the widespread application in optoelectronic devices. Nevertheless, the in-depth understanding of the relationship between exciton-phonon coupling and luminescence intensity remains incomplete. Herein, a doping-enhanced exciton-phonon coupling effect is observed in Cs3Cu2I5 nanocrystals (NCs), which leads to a remarkable increasement of their STEs emission efficiency. Mechanism study shows that the hetero-valent substitution of Cu+ with alkaline-earth metal ions (AE2+) causes a greater degree of Jahn–Teller distortion between the ground state and excited state structures of [Cu2I5]3− clusters as evidenced by our spectral analysis and first-principles calculations. As a consequence, an X-ray detector based on these Cs3Cu2I5:AE NCs delivers an X-ray imaging resolution of up to 10 lp·mm−1 and a low detection limit of 0.37 μGyair·s−1, disclosing the potential of doping-enhanced exciton-phonon coupling effect in improving STEs-emission and practical application for X-ray imaging.
The practical application of all-inorganic semiconductor lead halide perovskite nanocrystals (LHP NCs) has been limited by their poor stability. Recently, a lot of research on core–shell structure has been done to improve the stability of perovskite NCs, but the effect was far from the application requirements. Herein, we, for the first time, report a convenient approach to synthesize organic–inorganic double shell CsPbBr3@SiO2@polystyrene (PS) NCs with an inter-core of CsPbBr3, the intermediate layer of SiO2 shell, and outmost PS shell. Particularly, the CsPbBr3@SiO2@PS NCs maintained more than 90% of their initial photoluminescence (PL) intensity under one month's ultraviolet lamp irradiation or in 85 °C and 85% relative humidity (RH) condition. The white-light-emitting-diodes (WLEDs) were fabricated by encapsulating commercial InGaN chip with CsPbBr3@SiO2@PS NCs and K2SiF6:Mn4+ (KSF:Mn4+) phosphor with a luminous efficacy of ~ 100 lm/W at 20 mA current and a color gamut of 128% of the National Television Standards Committee (NTSC) standard. In addition, these WLEDs still maintain 91% of the initial luminous efficacy after 1200 h of continuous lighting. These results demonstrated that double shell-protected CsPbBr3 perovskite NCs have great potential in the field of WLEDs.