Additional electrons can drastically change the bonding trend of light elements. For example, N atoms in alkali metal azides form the linear N3(-) anions instead of N2 molecules with the introduction of additional electrons. The effect of the additional electrons on the polymerization of N under pressure is important and thus far unclear. Using first principles density functional methods and the particle swarm optimization structure search algorithm, we systematically study the evolution of LiN3 structures under pressures up to 600 GPa. A stable structure featuring polymerized N under pressures higher than 375 GPa is identified for the first time. It consists of zig-zag N polymer chains that are formed by N5(-) five-member rings sharing N-N pairs. Throughout the stable pressure range, the structure is insulating and consists of N atoms in sp(3) hybridizations. Comparing with the atomic and electronic structures of previous phases, our study completes the structural evolution of LiN3 under pressure and reveals the structural changes which are accompanied and driven by the change of atomic orbital hybridization, first from sp to sp(2) and then from sp(2) to sp(3).

Pressure-driven variations of hydrogen bonding energy in ammonium azide (NH4N3): IR absorption and Raman scattering studies

Recently, lead halide perovskite nanocrystals (NCs) have gained tremendous attention in optoelectronic devices due to their excellent optical properties. However, the toxicity of lead limits their practical applications. Here, the synthesis of Zn2+-alloyed CsZnxPb1-xX3 (up to 15%) NCs is reported to achieve lead-reduced white light-emitting diodes (WLEDs). The incorporation of Zn2+ into CsPbX3 host NCs results in a lattice contraction, without altering the structure and morphology, which has a direct effect on the optical properties. The blue-shifts in the photoluminescence emission and increase in bandgap is observed while retaining high photoluminescence quantum yield. Then by engineering the different compositions of halides for 15% Zn2+-alloyed CsZnxPb1-xX3 NCs, tunable emission (411–636 nm) is obtained. Notably, the WLEDs are experimentally demonstrated employing the lead-reduced NCs (blue, green, yellow, and red). By varying the ratios of the amount of NCs, white lights with a tunable correlated-color temperature (2218–8335 K), an exemplary color-rendering index (up to 93) and high luminous efficacy of radiation (268–318 lm·W−1) are obtained. Best of our knowledge, these are superior to other reported WLEDs based on CsPbX3 NCs doped with transition metal ions. This work places the halide perovskite NCs one-step closer in designing the environmentally benign and energy-efficient WLEDs.

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