Direct imaging of shock wave splitting in diamond at Mbar pressure

Understanding the behavior of matter at extreme pressures of the order of a megabar(Mbar)is essential to gain insight into various physical phenomena at macroscales—the formation of planets,young stars,and the cores of super-Earths,and at microscales—damage to ceramic materials and high-pressure plastic transformation and phase transitions in solids.Under dynamic compression of solids up to Mbar pressures,even a solid with high strength exhibits plastic properties,causing the induced shock wave to split in two:an elastic precursor and a plastic shock wave.This phenomenon is described by theoretical models based on indirect measurements of material response.The advent of x-ray free-electron lasers(XFELs)has made it possible to use their ultrashort pulses for direct observations of the propagation of shock waves in solid materials by the method of phase-contrast radiography.However,there is still a lack of comprehensive data for verification of theoretical models of different solids.Here,we present the results of an experiment in which the evolution of the coupled elastic-plastic wave structure in diamond was directly observed and studied with submicrometer spatial resolution,using the unique capabilities of the x-ray free-electron laser(XFEL).The direct measurements allowed,for the first time,the fitting and validation of the 2D failure model for diamond in the range of several Mbar.Our experimental approach opens new possibilities for the direct verification and construction of equations of state of matter in the ultra-high-stress range,which are relevant to solving a variety of problems in high-energy-density physics.

Development of new diagnostics based on LiF detector for pump-probe experiments

We present new diagnostics for use in optical laser pump-X-ray Free Electron Laser(XFEL)probe experiments to monitor dimensions,intensity profile and focusability of the XFEL beam and to control initial quality and homogeneity of targets to be driven by optical laser pulse.By developing X-ray imaging,based on the use of an LiF crystal detector,we were able to measure the distribution of energy inside a hard X-ray beam with unprecedented high spatial resolution(~1 mm)and across a field of view larger than some millimetres.This diagnostic can be used in situ,provides a very high dynamic range,has an extremely limited cost,and is relatively easy to be implemented in pump-probe experiments.The proposed methods were successfully applied in pump-probe experiments at the SPring-8 Angstrom Compact free electron LAser(SACLA)XFEL facility and its potential was demonstrated for current and future High Energy Density Science experiments.

Optimization of a laser plasma-based x-ray source according to WDM absorption spectroscopy requirements

X-ray absorption spectroscopy is a well-accepted diagnostic for experimental studies of warm dense matter.It requires a short-lived X-ray source of sufficiently high emissivity and without characteristic lines in the spectral range of interest.In the present work,we discuss how to choose an optimum material and thickness to get a bright source in the wavelength range 2A–6A(∼2 keV to 6 keV)by considering relatively low-Z elements.We demonstrate that the highest emissivity of solid aluminum and silicon foil targets irradiated with a 1-ps high-contrast sub-kJ laser pulse is achieved when the target thickness is close to 10μm.An outer plastic layer can increase the emissivity even further.

Ru complex and N,P-containing polymers confined within mesoporous hollow carbon spheres for hydrogenation of CO_(2)to formate

The development of reliable catalysts with both excellent activity and recyclability for carbon dioxide(CO_(2))hydrogenation is challenging.Herein,a ternary hybrid heterogeneous catalyst,involving mononuclear Ru complex,N,P-containing porous organic polymers(POPs),and mesoporous hollow carbon spheres(Ru^(3+)-POPs@MHCS)is reported for CO_(2)hydrogenation to formate.Based on comprehensive structural analyses,we demonstrated that Ru^(3+)-POPs were successfully immobilized within MHCS.The optimized Ru^(3+)-0.5POPs@MHCS catalyst,which was obtained with about 5 wt.%Ru^(3+)and 0.5 mmol POPs polymers confined into 0.3 g MHCS,exhibited high catalytic activity for CO_(2)hydrogenation to formate(turnover number(TON)>1,200 for 24 h under mild reaction conditions(4.0 MPa,120℃))and improved durability,compared to Ru^(3+)catalysts without POPs polymers(Ru^(3+)-MHCS)and unencapsulated MHCS(Ru^(3+)-0.5POPs)catalysts.The improved catalytic performance is attributed to the high surface area and large pore volume of MHCS which favors dispersion and stabilization of Ru^(3+)-POPs.Furthermore,the MHCS and POPs showed high CO_(2)adsorption ability.Ru^(3+)-POPs encapsulated into MHCS reduces the activation energy barrier for CO_(2)hydrogenation to formate.

Synthesis and Properties of a Through-Space Interacting Diradicaloid

Knowledge about electronic structures is important to gain an understanding of the unique functional properties of diradicaloids.In this study,we synthesized and characterized a diradicaloid in which two phenalenyl radical sites are coupled antiferromagnetically via a through-space interaction.The results of quantum chemical,physicochemical(^(1)H NMR,electronic absorption,cyclic voltammetry,SQUID,ESR),and chemical reactivity studies show that this diradicaloid has singlet diradical character.An assessment of the nature of the bonding interaction between two radical sites in this species using DFT calculations demonstrates that a small spatial overlap between the two SOMOs in this diradicaloid provides an efficient electron exchange path for the singlet state to be substantially lower in energy than the triplet state.

Turbulent hydrodynamics experiments in high energy density plasmas： scientific case and preliminary results of the TurboHEDP project

The physics of compressible turbulence in high energy density(HED) plasmas is an unchartered experimental area.Simulations of compressible and radiative flows relevant for astrophysics rely mainly on subscale parameters. Therefore,we plan to perform turbulent hydrodynamics experiments in HED plasmas(TurboHEDP) in order to improve our understanding of such important phenomena for interest in both communities: laser plasma physics and astrophysics. We will focus on the physics of supernovae remnants which are complex structures subject to fluid instabilities such as the Rayleigh–Taylor and Kelvin–Helmholtz instabilities. The advent of megajoule laser facilities, like the National Ignition Facility and the Laser Megajoule, creates novel opportunities in laboratory astrophysics, as it provides unique platforms to study turbulent mixing flows in HED plasmas. Indeed, the physics requires accelerating targets over larger distances and longer time periods than previously achieved. In a preparatory phase, scaling from experiments at lower laser energies is used to guarantee the performance of future MJ experiments. This subscale experiments allow us to develop experimental skills and numerical tools in this new field of research, and are stepping stones to achieve our objectives on larger laser facilities. We review first in this paper recent advances in high energy density experiments devoted to laboratory astrophysics. Then we describe the necessary steps forward to commission an experimental platform devoted to turbulent hydrodynamics on a megajoule laser facility. Recent novel experimental results acquired on LULI2000, as well as supporting radiative hydrodynamics simulations, are presented. Together with the development of LiF detectors as transformative X-ray diagnostics, these preliminary results are promising on the way to achieve micrometric spatial resolution in turbulent HED physics experiments in the near future.

Optical nature of non-substituted triphenylmethyl cation:Crystalline state emission,thermochromism,and phosphorescence

Since the discovery of the triphenylmethyl(trityl)cation 120 years ago,a variety of aromatic cations having various colors and luminescence properties have been rigorously studied.Many,differently substituted trityl cations have been synthesized,and their optical properties have been elucidated.However,the optical properties of the parent,non-substituted and highly reactive trityl cation,which was observed to be very weakly luminescent,have not been subjected to detailed investigation.In the effort described herein,we explored the optical nature of non-substituted trityl hexafluorophosphate(PF_(6))in the crystalline state.Trityl PF_(6) was found to exist as two crystal polymorphs including a yellow(Y)and an orange(O)form.Moreover,we observed that these crystalline forms display crystalline-state emission with different colors.The results of X-ray crystallographic analysis showed that the two polymorphs have totally different molecular packing arrangements.Furthermore,an investigation of their optical properties revealed that the O-crystal undergoes a distinct color change to yellow upon cooling as a consequence of a change in the nature of the charge transfer interaction between the cation and PF6 anion,and that both the Y-and O-crystal exhibit phosphorescence.

X-ray absorption spectroscopy study of energy transport in foil targets heated by petawatt laser pulses

X-ray absorption spectroscopy is proposed as a method for studying the heating of solid-density matter excited by secondary X-ray radiation from a relativistic laser-produced plasma. The method was developed and applied to experiments involving thin silicon foils irradiated by 0.5–1.5 ps duration ultrahigh contrast laser pulses at intensities between 0.5 × 10^(20) and 2.5 × 10^(20) W∕cm^2. The electron temperature of the material at the rear side of the target is estimated to be in the range of 140–300 eV. The diagnostic approach enables the study of warm dense matter states with low self-emissivity.