• Nolan Raynor posted an update 1 year, 5 months ago

    The combination of the increased physical adsorption capacity and ROS generation ability of 2D-MMT nanosheets would help inspire the development of MMT as a promising antimicrobial candidate in the future.We present first principle based beyond Born-Oppenheimer (BBO) theory and its applications on various models as well as realistic spectroscopic and scattering processes, where the Jahn-Teller (JT) theory is brought in conjunction with the BBO approach on the phase transition of lanthanide complexes. Over one and half decades, our development of BBO theory is demonstrated with ab initio calculations on representative molecules of spectroscopic interest (NO2 radical, Na3 and K3 clusters, NO3 radical, C6H6+ and 1,3,5-C6H3F3+ radical cations) as well as triatomic reactive scattering processes (H+ + H2 and F + H2). Such an approach exhibits the effect of JT, Renner-Teller (RT) and pseudo Jahn-Teller (PJT) type of interactions. While implementing the BBO theory, we generate highly accurate diabatic potential energy surfaces (PESs) to carry out quantum dynamics calculation and find excellent agreement with experimental photoelectron spectra of spectroscopic systems and cross-sections/rate constants of scattering processes. On the other hand, such electron-nuclear couplings incorporated through JT theory play a crucial role in dictating higher energy satellite transitions in the dielectric function spectra of the LaMnO3 complex. Overall, this article thoroughly sketches the current perspective of the BBO approach and its connection with JT theory with various applications on physical and chemical processes.Excellent luminous performance and high color rendering are the keys to white light-emitting diode (WLED) illumination. This work reports a single-phase full-visible-spectrum Y2Mg2Al2Si2O12(YMAS)Eu2+,Mn2+ phosphor for WLEDs with ultra-high color rendering. The luminescence of a single Mn2+ doped YMAS phosphor is very weak due to the spin-forbidden transition of Mn2+, while it can be dramatically enhanced in the YMASEu2+,Mn2+ system through efficient energy transfer from the sensitizer Eu2+. Meanwhile, the luminescent color of this phosphor can be tuned from cyan to cold white, to warm white, and finally close to the yellow region by controlling the activator concentration and energy transfer process. Its good thermal and chromaticity stability meet the requirements of application in WLEDs. Its stable photochromic performance at different excitation wavelengths (365-395 nm) indicates that it can be used in different ultraviolet chips. The YMAS0.03Eu2+,0.30Mn2+ phosphor-converted WLED achieves an ultra-high color rendering index (Ra = 93.3), near-standard chromaticity coordinates (CIE = (0.3343, 0.3388)) and a suitable correlated color temperature (CCT = 5417 K).Heat transfer and thermal properties at the nanoscale can be challenging to obtain experimentally. These are potentially relevant for understanding thermoregulation in cells. Experimental data from the transient heating regime in conjunction with a model based on the energy conservation enable the determination of the specific heat capacities for all components of a nanoconstruct, namely an upconverting nanoparticle and its conformal lipid bilayer coating. This approach benefits from a very simple, cost-effective and non-invasive optical setup to measure the thermal parameters at the nanoscale. The time-dependent model developed herein lays the foundation to describe the dynamics of heat transfer at the nanoscale and were used to understand the heat dissipation by lipid bilayers.Existing nanocolloidal optical resonators exhibiting strong magnetic resonances often suffer from multi-step low yield synthesis methods as well as a limited tunability, particularly in terms of spectral superposition of electric and magnetic resonances, which is the cornerstone for achieving Huygens scatterers. To overcome these drawbacks, we have synthesized clusters of gold nanoparticles using an emulsion-based formulation approach. This fabrication technique involved emulsification of an aqueous suspension of gold nanoparticles in an oil phase, followed by controlled ripening of the emulsion. The structural control of the as synthesized clusters, of mean radius 120 nm and produced in large numbers, is demonstrated with microscopy and X-ray scattering techniques. Using a polarization-resolved multi-angle light scattering setup, we conduct a comprehensive angular and spectroscopic determination of their optical resonant scattering in the visible wavelength range. We thus report on the clear experimental evidence of strong optical magnetic resonances and directional forward scattering patterns. The clusters behave as strong Huygens sources. Our findings crucially show that the electric and magnetic resonances as well as the scattering patterns can be tuned by adjusting the inner cluster structure, modifying a simple parameter of the fabrication method. This experimental approach allows for the large scale production of nanoresonators with potential uses for Huygens metasurfaces.The indispensable broad-band red phosphors for LED lighting generally show a long emission tail for wavelengths longer than 650 nm, which consumes excitation energy but contributes little luminance. Here, we report, for the first time, a broad red emission band with a steep falling edge at 652 nm, formed of widely distributed 1D2 → 3H4 emission lines of Pr3+ in Y3Si6N11 due to a large Stark splitting of the 3H4 (930 cm-1) and 1D2 (725 cm-1) levels. The red emission exhibits a 43 nm bandwidth, which is the widest in Pr3+-doped phosphors reported so far. Zidesamtinib in vivo The red Y3Si6N11Pr3+ phosphor was applied for the fabrication of 310 nm UV chip-based white LEDs, and a high color rendering index of 96 at a low correlated color temperature of 4188 K was achieved. Furthermore, a temperature-sensing scheme was proposed based on the temperature-dependent intensity ratios of the emission lines from the thermally coupled and large Stark splitting levels of the 1D2 state. Relative sensitivities as a function of temperature were studied in the range of 93-473 K. The findings of this study indicate that Y3Si6N11Pr3+ is an attractive broad-band red phosphor for both high color rendering white LEDs and temperature sensing applications.

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