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Furthermore, the separation is shown to be sensitive to the presence of missing linker defects in the nanosheets. Only 10% of missing linkers result in nonselective nanosheets. Hence, the importance of a defect-free synthetic method for CuBDC nanosheets is underlined.Treatment of trans-chalcone with dibenzo-7-phosphanorbornadiene EtOPA (A = C14H10, anthracene), a source of ethoxyphosphinidene, followed by formal elimination of ethanol yields 3,5-diphenyl-2-phosphafuran (DPF) in 43% yield. We show that the phosphadiene moiety of DPF is a potent diene in the Diels-Alder reaction and reacts with dienophiles dimethyl acetylenedicarboxylate (DPF·DMAD, 68%), norbornene (DPF·norbornene, 73%), and ethylene (DPF·C2H4, 80%) under ambient conditions. Mild heating of DPF·C2H4 results in the corresponding retro-Diels-Alder reaction, establishing DPF as a molecule that is able to reversibly bind ethylene.The practical utility of Møller-Plesset (MP) perturbation theory is severely constrained by the use of Hartree-Fock (HF) orbitals. It has recently been shown that the use of regularized orbital-optimized MP2 orbitals and scaling of MP3 energy could lead to a significant reduction in MP3 error [Bertels, L. W.; J. Phys. Chem. Lett. 2019, 10, 4170 4176]. In this work, we examine whether density functional theory (DFT)-optimized orbitals can be similarly employed to improve the performance of MP theory at both the MP2 and MP3 levels. We find that the use of DFT orbitals leads to significantly improved performance for prediction of thermochemistry, barrier heights, noncovalent interactions, and dipole moments relative to the standard HF-based MP theory. Indeed, MP3 (with or without scaling) with DFT orbitals is found to surpass the accuracy of coupled-cluster singles and doubles (CCSD) for several data sets. We also found that the results are not particularly functional sensitive in most cases (although range-separated hybrid functionals with low delocalization error perform the best). MP3 based on DFT orbitals thus appears to be an efficient, noniterative O(N6) scaling wave-function approach for single-reference electronic structure computations. Scaled MP2 with DFT orbitals is also found to be quite accurate in many cases, although modern double hybrid functionals are likely to be considerably more accurate.We studied degradation mechanisms of ultraviolet InGaN laser diodes emitting in the UVA range. Short wavelength nitride devices are subjected to much faster degradation, under the same packaging and testing conditions, than their longer wavelength counterparts. Transmission electron microscopy analysis of the degraded laser diodes showed pronounced damage to facets in the area of the active layer (waveguide, quantum wells, and electron blocking layer). Energy-dispersive X-ray spectroscopy showed that the active layers were heavily oxidized, forming a compound close in composition to Ga2O3 with proportional addition of Al in the respective area. The oxidation depth was roughly proportional to the intensity of the optical field. We propose UV-light-induced water splitting on a semiconductor surface as a mechanism of the oxidation and degradation of these devices.Broadband near-infrared (NIR) light sources present attractive opportunities for potential applications in high-capacity telecommunication, temperature sensing, energy conversion, and NIR spectroscopy. While significant effort has been spent on materials doped with rare-earth and transition-metal ions, the achievement of these materials with ultrabroadband NIR emission and desired wavelength region remains a long-standing challenge, especially operating in the spectral region between 700 and 1300 nm. Here, such emission is developed in tellurium (Te) cluster-doped silicate glass for the first time. Furthermore, the mechanism of the NIR luminescence due to D2h-symmetric tetratellurium (Te4) clusters is identified by density functional theory (DFT) calculations. For intense luminescence, a model for the generation and stabilization of Te clusters by tailoring topological cages via adjustment of the Na2O and Al2O3 contents and by optimizing the content of the dopant is proposed. Various stable Te clusters embedded into glass exhibit intense visible (Vis) to NIR broadband luminescence (400-1300 nm) with a spectral gap of 900 nm. In a demonstration experiment, a light-emitting diode (LED) device is fabricated from Te cluster-doped glass. This study opens a new opportunity for Te cluster-doped glass as a broadband NIR light source for spectroscopy applications.Two-dimensional polyimide covalent organic framework (2D PI-NT COF) films were constructed on indium tin oxide-coated glass substrates to fabricate two-terminal sandwiched resistive memory devices. The 2D PI-NT COF films condensated from the reaction between 4,4',4″-triaminotriphenylamine and naphthalene-1,4,5,8-tetracarboxylic dianhydride under solvothermal conditions demonstrated high crystallinity, good orientation preference, tunable thickness, and low surface roughness. The well-aligned electron-donor (triphenylamine unit) and -acceptor (naphthalene diimide unit) arrays rendered the 2D PI-NT COF films a promising candidate for electronic applications. HygromycinB The memory devices based on 2D PI-NT COF films exhibited a typical write-once-read-many-time resistive switching behavior under an operating voltage of +2.30 V on the positive scan and -2.64 V on the negative scan. A high ON/OFF current ratio (>106 for the positive scan and 104-106 for the negative scan) and long-term retention time indicated the high fidelity, low error, and high stability of the resistive memory devices. The memory behavior was attributed to an electric field-induced intramolecular charge transfer in an ordered donor-acceptor system, which provided the effective charge-transfer channels for injected charge carriers. This work represents the first example that explores the resistive memory properties of 2D PI-COF films, shedding light on the potential application of 2D COFs as information storage media.Ti-doped ZrO2 is a chemically stable and persistent luminescence material. Doping and co-doping is an effective approach for improving the afterglow properties of phosphors, but few studies have investigated the co-doping of ZrO2Ti systems. This study aimed to synthesize ZrO2Ti, M (M = Ca2+, Y3+, Ti single-doped, Nb5+, W6+) and evaluate the luminescent properties of the resulting materials, with a specific focus on the relationship between trap depth and the valence state of the co-doped cation. The ratio of the luminescent center to co-doped ion was optimized using the combinatorial approach, where 0.09 mol % Ti led to the best afterglow duration. The emission decay curves of each co-doped sample differed significantly, where a change in curvature was observed in the Ti single-doped and W6+ co-doped samples due to the presence of multiple traps. From the thermoluminescence glow curves, the trap originating in an oxygen vacancy with a peak at around 270 K was observed. The trap depth was dependent on electrostatic interactions between the trapped electrons and their surrounding cations, and thus related to the valence of the co-dopant.
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