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result(s) for
"Redmer, R."
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Direct observation of an abrupt insulator-to-metal transition in dense liquid deuterium
2015
Eighty years ago, it was proposed that solid hydrogen would become metallic at sufficiently high density. Despite numerous investigations, this transition has not yet been experimentally observed. More recently, there has been much interest in the analog of this predicted metallic transition in the dense liquid, due to its relevance to planetary science. Here, we show direct observation of an abrupt insulator-to-metal transition in dense liquid deuterium. Experimental determination of the location of this transition provides a much-needed benchmark for theory and may constrain the region of hydrogen-helium immiscibility and the boundary-layer pressure in standard models of the internal structure of gas-giant planets.
Journal Article
Observing the onset of pressure-driven K-shell delocalization
2023
The gravitational pressure in many astrophysical objects exceeds one gigabar (one billion atmospheres)
1
–
3
, creating extreme conditions where the distance between nuclei approaches the size of the K shell. This close proximity modifies these tightly bound states and, above a certain pressure, drives them into a delocalized state
4
. Both processes substantially affect the equation of state and radiation transport and, therefore, the structure and evolution of these objects. Still, our understanding of this transition is far from satisfactory and experimental data are sparse. Here we report on experiments that create and diagnose matter at pressures exceeding three gigabars at the National Ignition Facility
5
where 184 laser beams imploded a beryllium shell. Bright X-ray flashes enable precision radiography and X-ray Thomson scattering that reveal both the macroscopic conditions and the microscopic states. The data show clear signs of quantum-degenerate electrons in states reaching 30 times compression, and a temperature of around two million kelvins. At the most extreme conditions, we observe strongly reduced elastic scattering, which mainly originates from K-shell electrons. We attribute this reduction to the onset of delocalization of the remaining K-shell electron. With this interpretation, the ion charge inferred from the scattering data agrees well with ab initio simulations, but it is significantly higher than widely used analytical models predict
6
.
Experiments at the National Ignition Facility show how delocalization of K-shell electrons is driven by extreme pressure and temperature.
Journal Article
Ultrafast multi-cycle terahertz measurements of the electrical conductivity in strongly excited solids
2021
Key insights in materials at extreme temperatures and pressures can be gained by accurate measurements that determine the electrical conductivity. Free-electron laser pulses can ionize and excite matter out of equilibrium on femtosecond time scales, modifying the electronic and ionic structures and enhancing electronic scattering properties. The transient evolution of the conductivity manifests the energy coupling from high temperature electrons to low temperature ions. Here we combine accelerator-based, high-brightness multi-cycle terahertz radiation with a single-shot electro-optic sampling technique to probe the evolution of DC electrical conductivity using terahertz transmission measurements on sub-picosecond time scales with a multi-undulator free electron laser. Our results allow the direct determination of the electron-electron and electron-ion scattering frequencies that are the major contributors of the electrical resistivity.
The electrical conductivity is critical to understand warm dense matter, but the accurate measurement is extremely challenging. Here the authors use multi-cycle THz pulses to measure the conductivity of gold foils strongly heated by free-electron laser, determining the individual contributions of electron-electron and electron-ion scattering.
Journal Article
Heterogeneous to homogeneous melting transition visualized with ultrafast electron diffraction
by
Baldwin, J. K.
,
Glenzer, S. H.
,
Ng, A.
in
ATOMIC AND MOLECULAR PHYSICS
,
Attachment Behavior
,
Coexistence
2018
Understanding fast melting of metals is important for applications such as welding and micromachining. However, fast melting leaves simulation as the only option for probing the process. Mo et al. performed ultrafast electron diffraction experiments on laser-pulsed gold films. This allowed detailed mapping of the melting process, which proceeds through two distinct regimes while the bonding behavior changes in unexpected ways. The results require adding new physical processes to high-energy melting models. Science , this issue p. 1451 The details of how gold melts are captured with ultrafast electron diffraction experiments. The ultrafast laser excitation of matters leads to nonequilibrium states with complex solid-liquid phase-transition dynamics. We used electron diffraction at mega–electron volt energies to visualize the ultrafast melting of gold on the atomic scale length. For energy densities approaching the irreversible melting regime, we first observed heterogeneous melting on time scales of 100 to 1000 picoseconds, transitioning to homogeneous melting that occurs catastrophically within 10 to 20 picoseconds at higher energy densities. We showed evidence for the heterogeneous coexistence of solid and liquid. We determined the ion and electron temperature evolution and found superheated conditions. Our results constrain the electron-ion coupling rate, determine the Debye temperature, and reveal the melting sensitivity to nucleation seeds.
Journal Article
Melting curve of superionic ammonia at planetary interior conditions
by
Hernandez, J.-A
,
Bethkenhagen, M
,
Redmer, R
in
Ammonia
,
Electrical resistivity
,
Low temperature
2023
Under high pressures and temperatures, molecular systems with substantial polarization charges, such as ammonia and water, are predicted to form superionic phases and dense fluid states with dissociating molecules and high electrical conductivity. This behaviour potentially plays a role in explaining the origin of the multipolar magnetic fields of Uranus and Neptune, whose mantles are thought to result from a mixture of H2O, NH3 and CH4 ices. Determining the stability domain, melting curve and electrical conductivity of these superionic phases is therefore crucial for modelling planetary interiors and dynamos. Here we report the melting curve of superionic ammonia up to 300 GPa from laser-driven shock compression of pre-compressed samples and atomistic calculations. We show that ammonia melts at lower temperatures than water above 100 GPa and that fluid ammonia’s electrical conductivity exceeds that of water at conditions predicted by hot, super-adiabatic models for Uranus and Neptune, and enhances the conductivity in their fluid water-rich dynamo layers.Laser-driven shock compression experiments yield the melting curve of the superionic phase of ammonia at conditions relevant to the interiors of Uranus and Neptune.
Journal Article
Laser-driven shock compression of “synthetic planetary mixtures” of water, ethanol, and ammonia
2019
Water, methane, and ammonia are commonly considered to be the key components of the interiors of Uranus and Neptune. Modelling the planets’ internal structure, evolution, and dynamo heavily relies on the properties of the complex mixtures with uncertain exact composition in their deep interiors. Therefore, characterising icy mixtures with varying composition at planetary conditions of several hundred gigapascal and a few thousand Kelvin is crucial to improve our understanding of the ice giants. In this work, pure water, a water-ethanol mixture, and a water-ethanol-ammonia “synthetic planetary mixture” (SPM) have been compressed through laser-driven decaying shocks along their principal Hugoniot curves up to 270, 280, and 260 GPa, respectively. Measured temperatures spanned from 4000 to 25000 K, just above the coldest predicted adiabatic Uranus and Neptune profiles (3000–4000 K) but more similar to those predicted by more recent models including a thermal boundary layer (7000–14000 K). The experiments were performed at the GEKKO XII and LULI2000 laser facilities using standard optical diagnostics (Doppler velocimetry and optical pyrometry) to measure the thermodynamic state and the shock-front reflectivity at two different wavelengths. The results show that water and the mixtures undergo a similar compression path under single shock loading in agreement with Density Functional Theory Molecular Dynamics (DFT-MD) calculations using the Linear Mixing Approximation (LMA). On the contrary, their shock-front reflectivities behave differently by what concerns both the onset pressures and the saturation values, with possible impact on planetary dynamos.
Journal Article
Towards performing high‐resolution inelastic X‐ray scattering measurements at hard X‐ray free‐electron lasers coupled with energetic laser drivers
by
Baldwin, J. K.
,
Glenzer, S. H.
,
Descamps, A.
in
Coherent light
,
Design of experiments
,
Energy resolution
2022
High‐resolution inelastic X‐ray scattering is an established technique in the synchrotron community, used to investigate collective low‐frequency responses of materials. When fielded at hard X‐ray free‐electron lasers (XFELs) and combined with high‐intensity laser drivers, it becomes a promising technique for investigating matter at high temperatures and high pressures. This technique gives access to important thermodynamic properties of matter at extreme conditions, such as temperature, material sound speed, and viscosity. The successful realization of this method requires the acquisition of many identical laser‐pump/X‐ray‐probe shots, allowing the collection of a sufficient number of photons necessary to perform quantitative analyses. Here, a 2.5‐fold improvement in the energy resolution of the instrument relative to previous works at the Matter in Extreme Conditions (MEC) endstation, Linac Coherent Light Source (LCLS), and the High Energy Density (HED) instrument, European XFEL, is presented. Some aspects of the experimental design that are essential for improving the number of photons detected in each X‐ray shot, making such measurements feasible, are discussed. A careful choice of the energy resolution, the X‐ray beam mode provided by the XFEL, and the position of the analysers used in such experiments can provide a more than ten‐fold improvement in the photometrics. The discussion is supported by experimental data on 10 µm‐thick iron and 50 nm‐thick gold samples collected at the MEC endstation at the LCLS, and by complementary ray‐tracing simulations coupled with thermal diffuse scattering calculations. High‐resolution inelastic X‐ray scattering measurements at hard X‐ray free‐electron lasers coupled with energetic laser drivers have shown a 2.5‐fold improved energy resolution compared with previous experiments at similar XFEL instruments. Aspects of the experimental design that can be adjusted to improve the number of recorded photons on the detector are discussed.
Journal Article
X-ray scattering measurements of dissociation-induced metallization of dynamically compressed deuterium
2016
Hydrogen, the simplest element in the universe, has a surprisingly complex phase diagram. Because of applications to planetary science, inertial confinement fusion and fundamental physics, its high-pressure properties have been the subject of intense study over the past two decades. While sophisticated static experiments have probed hydrogen’s structure at ever higher pressures, studies examining the higher-temperature regime using dynamic compression have mostly been limited to optical measurement techniques. Here we present spectrally resolved x-ray scattering measurements from plasmons in dynamically compressed deuterium. Combined with Compton scattering, and velocity interferometry to determine shock pressure and mass density, this allows us to extract ionization state as a function of compression. The onset of ionization occurs close in pressure to where density functional theory-molecular dynamics (DFT-MD) simulations show molecular dissociation, suggesting hydrogen transitions from a molecular and insulating fluid to a conducting state without passing through an intermediate atomic phase.
High-pressure experiments play a critical role in understanding planetary interiors, but are notoriously difficult to carry out. Here, the authors demonstrate a laboratory platform for the controlled exploration of deuterium, with results that challenge existing models of ionization under compression.
Journal Article
An approach for the measurement of the bulk temperature of single crystal diamond using an X-ray free electron laser
2020
We present a method to determine the bulk temperature of a single crystal diamond sample at an X-Ray free electron laser using inelastic X-ray scattering. The experiment was performed at the high energy density instrument at the European XFEL GmbH, Germany. The technique, based on inelastic X-ray scattering and the principle of detailed balance, was demonstrated to give accurate temperature measurements, within
8
%
for both room temperature diamond and heated diamond to 500 K. Here, the temperature was increased in a controlled way using a resistive heater to test theoretical predictions of the scaling of the signal with temperature. The method was tested by validating the energy of the phonon modes with previous measurements made at room temperature using inelastic X-ray scattering and neutron scattering techniques. This technique could be used to determine the bulk temperature in transient systems with a temporal resolution of 50 fs and for which accurate measurements of thermodynamic properties are vital to build accurate equation of state and transport models.
Journal Article