This work is a quantitative study of the conditions required for a long-term passivation of the interface silicon-alkyl monolayers prepared by thermal hydrosilyation of neat 1-alkenes on well-defined H-Si(111) surfaces. We present electrochemical capacitance measurements (C-U) in combination with ex situ atomic force microscopy (AFM) observations and X-ray photoelectron spectroscopy (XPS) measurements. Capacitance measurements as a function of the reaction time and XPS data reveal close correlations between the chemical composition at the interface and its electronic properties. A very low density of states is found if suboxide formation is carefully prevented. The monitoring of C-U plots and AFM imaging upon exposure of the sample in diverse conditions indicate that the initial electronic properties and structure of the interface are long-lasting only when the monolayer surface coverage is theta > 0.42. A model demonstrates that this threshold value corresponds to a monolayer with intermolecular channels narrower than approximately 2.82 A, which is equal to the diameter of a water molecule. Water exclusion from the monolayer promotes long-term passivation of the silicon surface against oxidation in air and water as well as perfect corrosion inhibition in 20% NH(4)F. We provide two criteria to assess when a sample is optimized: The first one is an effective dielectric constant <2.5, and the second one is a very characteristic energy diagram at open circuit potential.
A series of Mg2-xAl4Si5O18:xDy(3+) (0 ≤x≤ 0.18) samples were synthesized, for the first time, by a solid state method both in a reducing atmosphere and in air. XRD, diffuse reflectance spectra, excitation spectra, emission spectra, decay times and thermal quenching were used to investigate the structure, photoluminescence, energy transfer and thermal properties. The results show that Mg2Al4Si5O18:Dy(3+) can efficiently absorb UV light and emit violet-blue light in the range of 400 to 500 nm from oxygen vacancies in the host as well as blue light (∼480 nm) and yellow light (∼576 nm) from the f-f transitions of Dy(3+). The emission intensities of the samples obtained under a reducing atmosphere are far superior to those of the samples obtained in air due to an efficient energy transition from oxygen vacancies in the host to Dy(3+). An analysis of the thermal quenching shows that the phosphor Mg2Al4Si5O18:Dy(3+) has excellent thermal properties. The emission intensities of typical samples synthesized in a reducing atmosphere and in air at 250 °C are 70% and 81% of their initial intensities at 20 °C, respectively. In addition, the emission colors of all of the samples are located in the white light region and the optimal chromaticity coordinates and Correlated Color Temperature are (x = 0.34, y = 0.33) and 5129 K, respectively. Therefore, these white Mg2Al4Si5O18:Dy(3+) phosphors could serve as promising candidates for white-light UV-LEDs.
The formation mechanism of the all-inorganic halide perovskite (AIHP)-related (e.g., CsPbBr3, Cs4PbBr6, and CsPb2Br5) nanocrystals have been studied, which is helpful to realize rational design of AIHP-related nanocrystals.
Reduced dimensional lead halide perovskites (RDPs) have attracted great research interest in diverse optical and optoelectronic fields. However, their poor stability is one of the most challenging obstacles prohibiting them from practical applications. Here, we reveal that ultrastable laurionite-type Pb(OH)Br can spontaneously encapsulate the RDPs in their formation solution without introducing any additional chemicals, forming RDP@Pb(OH)Br core− shell microparticles. Interestingly, the number of the perovskite layers within the RDPs can be conveniently and precisely controlled by varying the amount of CsBr introduced into the reaction solution. A single RDP@Pb(OH)Br core−shell microparticle composed of RDP nanocrystals with different numbers of perovskite layers can be also prepared, showing different colors under different light excitations. More interestingly, barcoded RDP@Pb(OH)Br microparticles with different parts emitting different lights can also be prepared. The morphology of the emitting microstructures can be conveniently manipulated. The RDP@ Pb(OH)Br microparticles demonstrate outstanding environmental, chemical, thermal, and optical stability, as well as strong resistance to anion exchange processes. This study not only deepens our understanding of the reaction processes in the extensively used saturation recrystallization method but also points out that it is highly possible to dramatically improve the performance of the optoelectronic devices through manipulating the spontaneous formation process of Pb(OH)Br.
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