Hybrid manganese halides have attracted widespread attention because of their highly emissive optical properties. To understand the underlying structural factors that dictate the photoluminescence quantum yield (PLQY) of these materials, we report five new hybrid manganese bromides with the general formula AmMnBr4 [m = 1 or 2, A = dimethylammonium (DMA), 3-methylpiperidinium (3MP), 3-aminomethylpiperidinium (3AMP), heptamethylenimine (HEP), and trimethylphenylammonium (TMPEA)]. By studying the crystal structures and optical properties of these materials and combining our results with the findings from previously reported analogs, we have found a direct correlation between Mn···Mn distance and the PLQY, where high PLQYs are associated with long Mn···Mn distances. This effect can be viewed as a manifestation of the concentration-quenching effect, except these are in stoichiometric compounds with precise interatomic distances rather than random alloys. To gain better separation of the Mn centers and prevent energy transfer, a bulky singly protonated cation that avoids H-bonding is ideal. We have demonstrated this principle in one of our newly reported material, (TMPEA)2MnBr4, where a PLQY of 70.8% for a powder sample and 98% for a large single crystal sample is achieved. Our study reveals a generalized method for improving PLQYs in hybrid manganese bromides and is readily extended to designing all varieties of highly emissive hybrid materials.

/pdf/design-principles-for-enhancing-photoluminescence-quantum-3lnk7qtrwa.pdf

Design Principles for Enhancing Photoluminescence Quantum Yield in Hybrid Manganese Bromides.

Point-of-care testing (POCT), as a portable and user-friendly technology, can obtain accurate test results immediately at the sampling point. Nowadays, microfluidic paper-based analysis devices (μPads) have attracted the eye of the public and accelerated the development of POCT. A variety of detection methods are combined with μPads to realize precise, rapid and sensitive POCT. This article mainly introduced the development of electrochemistry and optical detection methods on μPads for POCT and their applications on disease analysis, environmental monitoring and food control in the past 5 years. Finally, the challenges and future development prospects of μPads for POCT were discussed. 

/pdf/recent-advances-and-applications-in-paper-based-devices-for-2854xvrz.pdf

Recent Advances and Applications in Paper-Based Devices for Point-of-Care Testing

Scintillators with high light yield, low detection limit, large X‐ray attenuation efficiency as well as stable and nontoxic compositions are of great importance for radiation detection applications. Here, 0D (C8H20N)2Cu2Br4 single crystals are obtained and show blue emission peaking at 468 nm with a near‐unity photoluminescence quantum yield of 99.7%, a large Stokes shift of 148 nm (i.e., negligible self‐absorption), and a good environmental stability along with strong X‐ray absorption capability. Moreover, a high light yield of up to ≈ 91 300 photons/MeV and a low detection limit of 52.1 nGyair s−1 are realized, which is more than one hundred times lower than the dose rate of 5.5 µGyair s−1 required for X‐ray medical diagnostics. (C8H20N)2Cu2Br4 ceramic wafer scintillation screen is fabricated by a cold pressing sintering process, and the clear contrast images of opaque metal box and electronic component with a spatial resolution of 9.54 lp mm−1 are realized. This study not only designs a new lead‐free metal halide scintillator, but also develops a universal strategy for the preparation of large‐sized scintillator screen in nondestructive X‐ray imaging.

Ceramic Wafer Scintillation Screen by Utilizing Near‐Unity Blue‐Emitting Lead‐Free Metal Halide (C8H20N)2Cu2Br4

Inorganic semiconductor materials are best known for their superior physical properties, as well as their structural rigidity and stability. However, the poor solubility and solution-processability of these covalently bonded network structures has long been a serious drawback that limits their use in many important applications. Here, we present a unique and general approach to synthesize robust, solution-processable, and highly luminescent hybrid materials built on periodic and infinite inorganic modules. Structure analysis confirms that all compounds are composed of one-dimensional anionic chains of copper iodide (CumIm+22-) coordinated to cationic organic ligands via Cu-N bonds. The choice of ligands plays an important role in the coordination mode (μ1-MC or μ2-DC) and Cu-N bond strength. Greatly suppressed nonradiative decay is achieved for the μ2-DC structures. Record high quantum yields of 85% (λex = 360 nm) and 76% (λex = 450 nm) are obtained for an orange-emitting 1D-Cu4I6(L6). Temperature dependent PL measurements suggest that both phosphorescence and thermally activated delayed fluorescence contribute to the emission of these 1D-AIO compounds, and that the extent of nonradiative decay of the μ2-DC structures is much less than that of the μ1-DC structures. More significantly, all compounds are remarkably soluble in polar aprotic solvents, distinctly different from previously reported CuI based hybrid materials made of charge-neutral CumXm (X = Cl, Br, I), which are totally insoluble in all common solvents. The greatly enhanced solubility is a result of incorporation of ionic bonds into extended covalent/coordinate network structures, making it possible to fabricate large scale thin films by solution processes.

/pdf/blending-ionic-and-coordinate-bonds-in-hybrid-semiconductor-2mnb3vt9j8.pdf

Blending Ionic and Coordinate Bonds in Hybrid Semiconductor Materials: A General Approach toward Robust and Solution-Processable Covalent/Coordinate Network Structures

Low-dimensional organic-metal halides are regarded as an emerging class of X-ray scintillation materials, but most of the discovered compounds are confronted with challenges of toxicity and instability. To address these challenges, we herein report two lead-free zero-dimensional (0D) hybrid halides, (Bmpip)2Cu2Br4 and PPh4CuBr2 single crystals, grown by the low-cost solution-processing method. By single-crystal X-ray diffraction refinement, the crystal structures of (Bmpip)2Cu2Br4 and PPh4CuBr2 were determined to be orthorhombic and monoclinic crystal systems, respectively. (Bmpip)2Cu2Br4 and PPh4CuBr2 show broadband orange and yellow emissions peaking at 620 and 538 nm, respectively. Different from the emission nature of the recent reported Cu-based halide hybrids, both (Bmpip)2Cu2Br4 and PPh4CuBr2 emit from excitons bound to defects featuring spin-allowed transition, enabling them to possess fast scintillation decay time of tens of nanoseconds, respectively. In particular, the (Bmpip)2Cu2Br4 single crystal has a high photoluminescence quantum yield of 48.2%, a high scintillation yield of 16,000 photons/MeV, and a low detection limit of 710 nGyair/s. Due to the combination of nontoxicity, long-term stability, and decent detection performance, (Bmpip)2Cu2Br4 could be regarded as a promising X-ray scintillator.

Lead-Free Zero-Dimensional Organic-Copper(I) Halides as Stable and Sensitive X-ray Scintillators.

While a number of highly luminescent copper(I) halide based hybrid materials built on coordinate bonds (Cu-L; L = N, P, S-based ligands) have been obtained, the poor structural stability largely limited their commercialization. In contrast, according to the previous studies, the ionic structures (L-free) are more stable than those built on Cu-L coordinate bonds. However, the extremely weak emission hinders their optical applications. Herein, we report a tetra-alkylammonium-cation-induced strategy for the synthesis of stable and highly luminescent ionic CuBr-based hybrid materials. It is interesting to find that the tetra-alkylammonium cations with different chains could induce diverse CuBr-based anions. Moreover, most of these CuBr-based hybrids are highly luminescent, which makes them promising candidates as an alternative to phosphors and with potential applications in sensing.

Family of Highly Luminescent Pure Ionic Copper(I) Bromide Based Hybrid Materials.

Inkjet-printed paper-based sensor array for highly accurate pH sensing.

The role of the solvent in the solvothermal synthesis of carbon nanodots (CDs) is a long-standing puzzle for comprehensively understanding the CD formation mechanism and the relevant band gap tuning phenomenon. The controversy regarding solvent effect continues, largely because the importance of solvent-related reactions (SRs) has been ignored. In this Letter, we report that the SRs, i.e., oxidation-assisted solvent-involved dehydration and solvent-promoted oligomerization of phenylene/pyridinediamine (PD/PyD), are observed and dominate the formation of corresponding CDs by producing highly C2H4/C2H4O-featured species of precursors and PEG-like oligomer chains, which is very different from previously proposed theories. Moreover, our findings reveal that the photoluminescence (PL) of as-synthesized CDs originates from fluorophores formed by SRs and can be tailored by fluorophore engineering. Based on the SRs theory, three strategies for PL band gap tuning have been demonstrated.

Exploring Solvent-Related Reactions and Corresponding Band Gap Tuning Strategies for Carbon Nanodots Based on Solvothermal Synthesis

Using ratiometric indicator-displacement-assay in semi-quantitative colorimetric determination of tetracyclines

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Family of Highly Luminescent Pure Ionic Copper(I) Bromide Based Hybrid Materials.

Inkjet-printed paper-based sensor array for highly accurate pH sensing.

Exploring Solvent-Related Reactions and Corresponding Band Gap Tuning Strategies for Carbon Nanodots Based on Solvothermal Synthesis

Using ratiometric indicator-displacement-assay in semi-quantitative colorimetric determination of tetracyclines