Whereas prototypical is not a glass former, amorphous can be formed as thin films through vapor deposition and can serve as a structural model for the glass. The first two-dimensional solid-state NMR experiments for amorphous thin film reveal that four- and five-coordinated species are predominant (95%), while six-coordinated species are minor. Such a species distribution is remarkably similar to what has been predicted theoretically for melts. Upon annealing to the five-coordinated species becomes negligible, indicating the onset of crystallization of .
Perovskite light-emitting diodes (PeLEDs) based on three-dimensional (3D) polycrystalline perovskites suffer from ion migration, which causes overshoot of luminance over time during operation and reduces its operational lifetime. Here, we demonstrate 3D/2D hybrid PeLEDs with extremely reduced luminance overshoot and 21 times longer operational lifetime than 3D PeLEDs. The luminance overshoot ratio of 3D/2D hybrid PeLED is only 7.4% which is greatly lower than that of 3D PeLED (150.4%). The 3D/2D hybrid perovskite is obtained by adding a small amount of neutral benzylamine to methylammonium lead bromide, which induces a proton transfer from methylammonium to benzylamine and enables crystallization of 2D perovskite without destroying the 3D phase. Benzylammonium in the perovskite lattice suppresses formation of deep-trap states and ion migration, thereby enhances both operating stability and luminous efficiency based on its retardation effect in reorientation.
10 June 2008 in Proceedings of the National Academy of Sciences
Silicate melts at the top of the transition zone and the core-mantle boundary have significant influences on the dynamics and properties of Earth's interior. MgSiO 3 -rich silicate melts were among the primary components of the magma ocean and thus played essential roles in the chemical differentiation of the early Earth. Diverse macroscopic properties of silicate melts in Earth's interior, such as density, viscosity, and crystal-melt partitioning, depend on their electronic and short-range local structures at high pressures and temperatures. Despite essential roles of silicate melts in many geophysical and geodynamic problems, little is known about their nature under the conditions of Earth's interior, including the densification mechanisms and the atomistic origins of the macroscopic properties at high pressures. Here, we have probed local electronic structures of MgSiO 3 glass (as a precursor to Mg-silicate melts), using high-pressure x-ray Raman spectroscopy up to 39 GPa, in which high-pressure oxygen K-edge features suggest the formation of tricluster oxygens (oxygen coordinated with three Si frameworks; [3] O) between 12 and 20 GPa. Our results indicate that the densification in MgSiO 3 melt is thus likely to be accompanied with the formation of triculster, in addition to a reduction in nonbridging oxygens. The pressure-induced increase in the fraction of oxygen triclusters >20 GPa would result in enhanced density, viscosity, and crystal-melt partitioning, and reduced element diffusivity in the MgSiO 3 melt toward deeper part of the Earth's lower mantle.
We report spectroscopic evidence for the pressure-induced structural changes in glass quenched from melts at pressures up to 6 GPa using solid-state NMR. While all borons are tri-coordinated at 1 atm, the fraction of tetra-coordinated boron increases with pressure, being about 5% and 27% in the glass quenched from melts at 2 and 6 GPa, respectively. The fraction of boroxol ring species increases with pressure up to 2 GPa and apparently decreases with further compression up to 6 GPa. Two densification mechanisms are proposed to explain the variation of boron species with pressure.