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  1. Abstract

    In this study, we conduct extensive high‐pressure experiments to investigate phase stability in the cobalt‐nitrogen system. Through a combination of synthesis in a laser‐heated diamond anvil cell, first‐principles calculations, Raman spectroscopy, and single‐crystal X‐ray diffraction, we establish the stability fields of known high‐pressure phases, hexagonal NiAs‐type CoN, and marcasite‐type CoN2within the pressure range of 50–90 GPa. We synthesize and characterize previously unknown nitrides, Co3N2,Pnma‐CoN and two polynitrides, CoN3and CoN5, within the pressure range of 90–120 GPa. Both polynitrides exhibit novel types of polymeric nitrogen chains and networks. CoN3feature branched‐type nitrogen trimers (N3) and CoN5show π‐bonded nitrogen chain. As the nitrogen content in the cobalt nitride increases, the CoN6polyhedral frameworks transit from face‐sharing (in CoN) to edge‐sharing (in CoN2and CoN3), and finally to isolated (in CoN5). Our study provides insights into the intricate interplay between structure evolution, bonding arrangements, and high‐pressure synthesis in polynitrides, expanding the knowledge for the development of advanced energy materials

     
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    Free, publicly-accessible full text available June 6, 2025
  2. A new diamond anvil cell experimental approach has been implemented at the European x-ray Free Electron Laser, combining pulsed laser heating with MHz x-ray diffraction. Here, we use this setup to determine liquidus temperatures under extreme conditions, based on the determination of time-resolved crystallization. The focus is on a Fe-Si-O ternary system, relevant for planetary cores. This time-resolved diagnostic is complemented by a finite-element model, reproducing temporal temperature profiles measured experimentally using streaked optical pyrometry. This model calculates the temperature and strain fields by including (i) pressure and temperature dependencies of material properties, and (ii) the heat-induced thermal stress, including feedback effect on material parameter variations. Making our model more realistic, these improvements are critical as they give 7000 K temperature differences compared to previous models. Laser intensities are determined by seeking minimal deviation between measured and modeled temperatures. Combining models and streak optical pyrometry data extends temperature determination below detection limit. The presented approach can be used to infer the liquidus temperature by the appearance of SiO2 diffraction spots. In addition, temperatures obtained by the model agree with crystallization temperatures reported for Fe–Si alloys. Our model reproduces the planetary relevant experimental conditions, providing temperature, pressure, and volume conditions. Those predictions are then used to determine liquidus temperatures at experimental timescales where chemical migration is limited. This synergy of novel time-resolved experiments and finite-element modeling pushes further the interpretation capabilities in diamond anvil cell experiments.

     
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    Free, publicly-accessible full text available September 7, 2024
  3. Experiments accessing extreme conditions at x-ray free electron lasers (XFELs) involve rapidly evolving conditions of temperature. Here, we report time-resolved, direct measurements of temperature using spectral streaked optical pyrometry of x-ray and optical laser-heated states at the High Energy Density instrument of the European XFEL. This collection of typical experiments, coupled with numerical models, outlines the reliability, precision, and meaning of time dependent temperature measurements using optical emission at XFEL sources. Dynamic temperatures above 1500 K are measured continuously from spectrally- and temporally-resolved thermal emission at 450–850 nm, with time resolution down to 10–100 ns for 1–200 μs streak camera windows, using single shot and integrated modes. Targets include zero-pressure foils free-standing in air and in vacuo, and high-pressure samples compressed in diamond anvil cell multi-layer targets. Radiation sources used are 20-fs hard x-ray laser pulses at 17.8 keV, in single pulses or 2.26 MHz pulse trains of up to 30 pulses, and 250-ns infrared laser single pulses. A range of further possibilities for optical measurements of visible light in x-ray laser experiments using streak optical spectroscopy are also explored, including for the study of x-ray induced optical fluorescence, which often appears as background in thermal radiation measurements. We establish several scenarios where combined emissions from multiple sources are observed and discuss their interpretation. Challenges posed by using x-ray lasers as non-invasive probes of the sample state are addressed.

     
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    Free, publicly-accessible full text available August 7, 2024