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Abstract Fundamental understanding of the effect of doping on the optical properties of 3D double perovskites (DPs) especially the dynamics of self‐trapped excitons (STEs) is of vital importance for their optoelectronic applications. Herein, a unique strategy via Cu+ doping to achieve efficient STE emission in the alloyed lead‐free Cs2(Ag/Na)InCl6 DPs is reported. A small amount (1.0 mol%) of Cu+ doping results in boosted STE emission in the crystals, with photoluminescence (PL) quantum yield increasing from 19.0% to 62.6% and excitation band shifting from 310 to 365 nm. Temperature‐dependent PL and femtosecond transient absorption spectroscopies reveal that the remarkable PL enhancement originates from the increased radiative recombination rate and density of STEs, as a result of symmetry breakdown of the STE wavefunction at the octahedral Ag+ site. These findings provide deep insights into the STE dynamics in Cu+‐doped Cs2(Ag/Na)InCl6, thereby laying a foundation for the future design of new lead‐free DPs with efficient STE emission.

Abstract Intracellular detection is highly desirable for biological research and clinical diagnosis, yet its quantitative analysis with noninvasivity, sensitivity, and accuracy remains challenging. Herein, a near‐infrared (NIR) dual‐excitation strategy is reported for ratiometric intracellular detection through the design of dye‐sensitized upconversion probes and employment of a purpose‐built NIR dual‐laser confocal microscope. NIR dye IR808, a recognizer of intracellular analyte hypochlorite, is introduced as energy donor and Yb,Er‐doped NaGdF4 upconversion nanoparticles are adopted as energy acceptor in the as‐designed nanoprobes. The efficient analyte‐dependent energy transfer and low background luminescence endow the nanoprobes with ultrahigh sensitivity. In addition, with the nonanalyte‐dependent upconversion luminescence (UCL) excited by 980 nm as a self‐calibrated signal, the interference from environmental fluctuation can be alleviated. Furthermore, the dual 808/980 nm excited ratiometric UCL is demonstrated for the quantification of the level of intracellular hypochlorite. Particularly, the intrinsic hypochlorite with only nanomolar concentration in live MCF‐7 cells in the absence of exogenous stimuli is determined. Such an NIR dual‐excitation ratiometric strategy based on dye‐sensitized UCL probes can be easily extended to detect various intracellular analytes through tailoring the reactive NIR dyes, which provides a promising tool for probing biochemical processes in live cells and diagnosing diseases.

Fundamental understanding of the effect of doping on the optical properties of 3D double perovskites (DPs) especially the dynamics of self‐trapped excitons (STEs) is of vital importance for their optoelectronic applications. Herein, a unique strategy via Cu+ doping to achieve efficient STE emission in the alloyed lead‐free Cs2(Ag/Na)InCl6 DPs is reported. A small amount (1.0 mol%) of Cu+ doping results in boosted STE emission in the crystals, with photoluminescence (PL) quantum yield increasing from 19.0% to 62.6% and excitation band shifting from 310 to 365 nm. Temperature‐dependent PL and femtosecond transient absorption spectroscopies reveal that the remarkable PL enhancement originates from the increased radiative recombination rate and density of STEs, as a result of symmetry breakdown of the STE wavefunction at the octahedral Ag+ site. These findings provide deep insights into the STE dynamics in Cu+‐doped Cs2(Ag/Na)InCl6, thereby laying a foundation for the future design of new lead‐free DPs with efficient STE emission. [ABSTRACT FROM AUTHOR]

Intracellular detection is highly desirable for biological research and clinical diagnosis, yet its quantitative analysis with noninvasivity, sensitivity, and accuracy remains challenging. Herein, a near‐infrared (NIR) dual‐excitation strategy is reported for ratiometric intracellular detection through the design of dye‐sensitized upconversion probes and employment of a purpose‐built NIR dual‐laser confocal microscope. NIR dye IR808, a recognizer of intracellular analyte hypochlorite, is introduced as energy donor and Yb,Er‐doped NaGdF4 upconversion nanoparticles are adopted as energy acceptor in the as‐designed nanoprobes. The efficient analyte‐dependent energy transfer and low background luminescence endow the nanoprobes with ultrahigh sensitivity. In addition, with the nonanalyte‐dependent upconversion luminescence (UCL) excited by 980 nm as a self‐calibrated signal, the interference from environmental fluctuation can be alleviated. Furthermore, the dual 808/980 nm excited ratiometric UCL is demonstrated for the quantification of the level of intracellular hypochlorite. Particularly, the intrinsic hypochlorite with only nanomolar concentration in live MCF‐7 cells in the absence of exogenous stimuli is determined. Such an NIR dual‐excitation ratiometric strategy based on dye‐sensitized UCL probes can be easily extended to detect various intracellular analytes through tailoring the reactive NIR dyes, which provides a promising tool for probing biochemical processes in live cells and diagnosing diseases. [ABSTRACT FROM AUTHOR]