Inexpensive and highly efficient luminescent materials based on multinary halides have received increased attention in recent years. Among those considered most promising are the perovskites such as CsPbX3 because of their highly efficient and tunable emission through precise control of chemical composition and nanostructuring. However, the presence of the toxic heavy metal Pb and relatively poor stability are among the major challenges for the introduction of lead-halide-based materials into the marketplace. Here, we report the optical properties of nontoxic and highly emissive one-dimensional (1D) all-inorganic halides CsCu2X3 (X = Cl, Br, I) and their mixed halide derivatives, which also show improved thermal and air stability. Photoluminescence (PL) measurements show tunable bright room temperature emission from green to yellow with photoluminescence quantum yields ranging from 0.37 (CsCu2Cl1.5Br1.5) to 48.0% (CsCu2Cl3). Temperature- and power-dependent PL measurements suggest that the emission results from self-trapped excitons induced by strong charge localization and structural distortions within the lD ribbon structure.
Low-dimensional hybrid organic–inorganic materials (HOIMs) are being widely investigated for their unique optoelectronic properties. Some of them exhibit broadband white-light (WL) luminescence upon UV excitation, providing a potential for the fabrication of single-component white-light-emitting diodes. Here, we report new examples of low-dimensional HOIMs, based on 4-aminopyridinium (4AMP) and group 12 metals (Hg and Zn), for single-component WL emission. The 4AMP cation containing structures feature HgBr4 and ZnBr4 isolated tetrahedra in (C5H7N2)2HgBr4·H2O (1) and (C5H7N2)2ZnBr4 (2), respectively. The presence of isolated molecular units in the zero-dimensional structures results in strongly localized charges and bright WL luminescence with corresponding Commission Internationale de l’Eclairage color coordinates of (0.34, 0.38) and (0.25, 0.26), correlated color temperatures of 5206 K (1) and 11 630 K (2), and very high color rendering indexes (CRI) of 87 (1) and 96 (2). The visibly bright WL emission at room temperature is corroborated with high measured photoluminescence quantum yield values of 14.87 and 19.18% for 1 and 2, respectively. Notably, the high CRI values for these new HOIMs exceed the commercial requirements and produce both “warm” and “cold” WL depending on the metal used (Hg or Zn). Based on temperature- and powder-dependent photoluminescence (PL), PL lifetimes measurements and density functional theory calculations, the broadband WL emission is assigned to the 4AMP organic molecules emission and self-trapped states.
Recently, interest in developing efficient, low-cost, nontoxic, and stable metal halide emitters that can be incorporated into solid-state lighting technologies has taken hold. Here we report nontoxic, stable, and highly efficient blue-light-emitting Cs3Cu2Br5–x I x (0 ≤ x ≤ 5). Room-temperature photoluminescence measurements show bright blue emission in the 456 to 443 nm range with near-unity quantum yield for Cs3Cu2I5. Density functional theory calculations and power-dependent PL measurements suggest that the emission results from self-trapped excitons induced by strong charge localization within the zero-dimensional cluster structure of Cs3Cu2Br5–x I x .
The United States Department of Energy (DOE) projects an estimated energy cost savings of $630 billion from 2015 to 2035 if reliable solid-state lighting technologies can be developed and DOE goals are met. [1] For the cost-effective implementation of light-emitting diodes (LEDs), development of new inexpensive light emitters is an urgent need. Owing to their outstanding photophysical properties including tunable bandgaps and emission colors, high photoluminescent quantum yields (PLQY) and excellent color purity, metal halide perovskite LEDs (PeLEDs)
We report the synthesis, crystal and electronic structures, as well as optical properties of the hybrid organic-inorganic compounds MACdX (MA = CHNH; X = Cl, Br, I). MACdI is a new compound, whereas, for MACdCl and MACdBr, structural investigations have already been conducted but electronic structures and optical properties are reported here for the first time. Single crystals were grown through slow evaporation of MACdX solutions with optimized conditions yielding mm-sized colorless (X = Cl, Br) and pale yellow (X = I) crystals. Single crystal and variable temperature powder X-ray diffraction measurements suggest that MACdCl forms a 2D layered perovskite structure and has two structural transitions at 283 and 173 K. In contrast, MACdBr and MACdI adopt 0D KSO-derived crystal structures based on isolated CdX tetrahedra and show no phase transitions down to 20 K. The contrasting crystal structures and chemical compositions in the MACdX family impact their air stabilities, investigated for the first time in this work; MACdCl is air-stable, whereas MACdBr and MACdI partially decompose when left in air. Optical absorption measurements suggest that MACdX have large optical band gaps above 3.9 eV. Room temperature photoluminescence spectra of MACdX yield broad peaks in the 375-955 nm range with full width at half-maximum values up to 208 nm. These PL peaks are tentatively assigned to self-trapped excitons in MACdX following the crystal and electronic structure considerations. The bands around the Fermi level have small dispersions, which is indicative of high charge localization with significant exciton binding energies in MACdX. On the basis of our combined experimental and computational results, MACdX and related compounds may be of interest for white-light-emitting phosphors and scintillator applications.
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