Mandy Bethkenhagen

École Polytechnique · LULI Laboratoire Pour l'Utilisation des Lasers Intenses

Laser-driven dynamic compression experiments of plastic materials have found surprisingly fast formation of nanodiamonds (ND) via X-ray probing. This mechanism is relevant for planetary models, but could also open efficient synthesis routes for tailored NDs. We investigate the release mechanics of compressed NDs by molecular dynamics simulation of...

Accurate knowledge of the properties of hydrogen at high compression is crucial for astrophysics (e.g. planetary and stellar interiors, brown dwarfs, atmosphere of compact stars) and laboratory experiments, including inertial confinement fusion. There exists experimental data for the equation of state, conductivity, and Thomson scattering spectra....

DFT-MD simulations of the CH 4 –H 2 mixture studied under icy-planetary conditions suggest a phase transition from molecular to polymer region with liberation of hydrogen leading to a non-metallic to metallic transition, fulfilling the LMA within 4%.

We report the results of the second charged-particle transport coefficient code comparison workshop, which was held in Livermore, California on 24–27 July 2023. This workshop gathered theoretical, computational, and experimental scientists to assess the state of computational and experimental techniques for understanding charged-particle transport...

We study ab initio approaches for calculating x-ray Thomson scattering spectra from density functional theory molecular dynamics simulations based on a modified Chihara formula that expresses the inelastic contribution in terms of the dielectric function. We study the electronic dynamic structure factor computed from the Mermin dielectric function...

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...

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 state⁴. Both processes sub...

We calculate reflectivities of dynamically compressed water, water-ethanol mixtures, and ammonia at infrared and optical wavelengths with density functional theory and molecular dynamics simulations. The influence of the exchange-correlation functional on the results is examined in detail. Our findings indicate that the consistent use of the HSE hy...

Hydrocarbon mixtures are extremely abundant in the Universe, and diamond formation from them can play a crucial role in shaping the interior structure and evolution of planets. With first-principles accuracy, we first estimate the melting line of diamond, and then reveal the nature of chemical bonding in hydrocarbons at extreme conditions. We final...

Accurately modeling dense plasmas over wide ranging conditions of pressure and temperature is a grand challenge critically important to our understanding of stellar and planetary physics as well as inertial confinement fusion. In this work, we employ Kohn-Sham density functional theory (DFT) molecular dynamics (MD) to compute the properties of carb...

We describe an experimental concept at the National Ignition Facility for specifically tailored spherical implosions to compress hydrogen to extreme densities (up to $\sim$800$\times$ solid density, electron number density n$_e$$\sim$4$\times$10$^{25}$ cm$^{-3}$ ) at moderate temperatures (T$\sim$200 eV), i.e., to conditions, which are relevant to...

We study state-of-the-art approaches for calculating x-ray Thomson scattering spectra from density functional theory molecular dynamics (DFT-MD) simulations based on a modified Chihara formula that expresses the inelastic contribution in terms of the dielectric function. We compare the electronic dynamic structure factor computed from the Mermin di...

The determination of the ionization of a system in the hot dense regime is a long standing issue. Recent studies have shown inconsistencies between standard predictions using average atom models and evaluations deduced from electronic transport properties computed with quantum molecular dynamics simulations [Bethkenhagen et al., Phys. Rev. Res. 2,...

Extreme conditions inside ice giants such as Uranus and Neptune can result in peculiar chemistry and structural transitions, e.g., the precipitation of diamonds or superionic water, as so far experimentally observed only for pure C─H and H 2 O systems, respectively. Here, we investigate a stoichiometric mixture of C and H 2 O by shock-compressing p...

We describe an experimental concept at the National Ignition Facility for specifically tailored spherical implosions to compress hydrogen to extreme densities (up to ~800x solid density, electron number density n e ~4x10^25 cm^-3) at moderate temperatures (T ~200 eV), i.e., to conditions, which are relevant to the interiors of red dwarf stars. The...

Most experimentally known high-pressure ice phases have a body-centred cubic (bcc) oxygen lattice. Our large-scale molecular-dynamics simulations with a machine-learning potential indicate that, amongst these bcc ice phases, ices VII, VII′ and X are the same thermodynamic phase under different conditions, whereas superionic ice VII″ has a first-ord...

Hydrocarbon mixtures are extremely abundant in the Universe, and diamond formation from them can play a crucial role in shaping the interior structure and evolution of planets. With first-principles accuracy, we first estimate the diamond nucleation rate in pure liquid carbon, and then reveal the nature of chemical bonding in hydrocarbons at extrem...

We investigate the thermopower and Lorenz number of hydrogen with Kohn-Sham density functional theory (DFT) across the plasma plane toward the near-classical limit, i.e., weakly degenerate and weakly coupled states. Our results are in concordance with certain limiting values for the Lorentz plasma, a model system which only considers electron-ion s...

Most experimentally known high-pressure ice phases have a body-centred cubic (bcc) oxygen lattice. Our atomistic simulations show that, amongst these bcc ice phases, ices VII, VII' and X are the same thermodynamic phase under different conditions, whereas superionic ice VII'' has a first-order phase boundary with ice VII'. Moreover, at about 300 GP...

Most water in the Universe may be superionic, and its thermodynamic and transport properties are crucial for planetary science but difficult to probe experimentally or theoretically. We use machine learning and free-energy methods to overcome the limitations of quantum mechanical simulations and characterize hydrogen diffusion, superionic transitio...

The low-density limit of the electrical conductivity σ (n, T) of hydrogen as the simplest ionic plasma is presented as a function of the temperature T and mass density n in the form of a virial expansion of the resistivity. Quantum statistical methods yield exact values for the lowest virial coefficients which serve as a benchmark for analytical ap...

Accurately modeling dense plasmas over wide ranging conditions of pressures and temperatures is a grand challenge critically important to our understanding of stellar and planetary physics as well as inertial confinement fusion. In this work, we investigate the thermodynamic, structural, and transport properties of carbon at warm and hot dense matt...

The low-density limit of the electrical conductivity $\sigma(n,T)$ of hydrogen as the simplest ionic plasma is presented as function of temperature T and mass density n in form of a virial expansion of the resistivity. Quantum statistical methods yield exact values for the lowest virial coefficients which serve as benchmark for analytical approache...

We use a nonrelativistic average-atom model to calculate carbon ionization at megabar and gigabar pressures. The pressure is calculated using the stress-tensor method. The electronic electrical conductivity is also considered using the Kubo-Greenwood approach. Comparisons are made with quantum molecular dynamic simulations. A good agreement is obta...

Most water in the universe may be superionic, and its thermodynamic and transport properties are crucial for planetary science but difficult to probe experimentally or theoretically. We use machine learning and free energy methods to overcome the limitations of quantum mechanical simulations, and characterize hydrogen diffusion, superionic transiti...

X-ray Thomson scattering (XRTS) is a powerful diagnostic technique that involves an x-ray source interacting with a dense plasma sample, resulting in a spectrum of elastically and inelastically scattered x-rays. Depending on the plasma conditions, one can measure a range of parameters from the resulting spectrum, including plasma temperature, elect...

Ammonia is predicted to be one of the major components in the depths of the ice giant planets Uranus and Neptune. Their dynamics, evolution, and interior structure are insufficiently understood and models rely imperatively on data for equation of state and transport properties. Despite its great significance, the experimentally accessed region of t...

Ammonia is predicted to be one of the major components in the depths of the ice giant planets Uranus and Neptune. Their dynamics, evolution, and interior structure are insufficiently understood and models rely imperatively on data for equation of state and transport properties. Despite its great significance, the experimentally accessed region of t...

We present an accurate and efficient real-space formulation of the Hellmann–Feynman stress tensor for O(N) Kohn–Sham density functional theory (DFT). While applicable at any temperature, the formulation is most efficient at high temperature where the Fermi–Dirac distribution becomes smoother and the density matrix becomes correspondingly more local...

The formation and evolution of stars depends on various physical aspects of stellar matter, including the equation of state (EOS) and transport properties. Although often dismissed as `ideal gas-like' and therefore simple, states occurring in stellar matter are dense plasmas, and the EOS has not been established precisely. EOS constructed using mul...

We present an accurate and efficient real-space formulation of the Hellmann-Feynman stress tensor for $\mathcal{O}(N)$ Kohn-Sham density functional theory (DFT). While applicable at any temperature, the formulation is most efficient at high temperature where the Fermi-Dirac distribution becomes smoother and density matrix becomes correspondingly mo...

A realistic description of partially ionized matter in extreme thermodynamic states is critical to model the interior and evolution of the multiplicity of high-density astrophysical objects. Current predictions of its essential property, the ionization degree, rely widely on analytical approximations that have been challenged recently by a series o...

Atom-in-jellium calculations of the Einstein frequency were used to calculate the mean displacement of an ion over a wide range of compression and temperature. Expressed as a fraction of the Wigner-Seitz radius, the displacement is a measure of the asymptotic freedom of the ion at high temperature, and thus of the change in heat capacity from six t...

A realistic description of partially-ionized matter in extreme thermodynamic states is critical to model the interior and evolution of the multiplicity of high-density astrophysical objects. Current predictions of its essential property, the ionization degree, rely widely on analytical approximations that have been challenged recently by a series o...

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 c...

Recent path-integral Monte Carlo and quantum molecular dynamics simulations have shown that computationally efficient average-atom models can predict thermodynamic states in warm dense matter to within a few percent. One such atom-in-jellium model has typically been used to predict the electron-thermal behavior only, although it was previously deve...

Atom-in-jellium calculations of the Einstein frequency were used to calculate the mean displacement of an ion over a wide range of compression and temperature. Expressed as a fraction of the Wigner-Seitz radius, the displacement is a measure of the asymptotic freedom of the ion at high temperature, and thus of the change in heat capacity from 6 to...

Recent path-integral Monte Carlo and quantum molecular dynamics simulations have shown that computationally efficient average-atom models can predict thermodynamic states in warm dense matter to within a few percent. One such atom-in-jellium model has typically been used to predict the electron-thermal behavior only, although it was previously deve...

We have developed and fielded a new x-ray pinhole-imaging snout that exploits time-resolved penumbral imaging of low-emission hot spots in capsule implosion experiments at the National Ignition Facility. We report results for a series of indirectly driven Be capsule implosions that aim at measuring x-ray Thomson scattering (XRTS) spectra at extreme...

We present thermodynamic material and transport properties for the extreme conditions prevalent in the interiors of massive giant planets and brown dwarfs. They are obtained from extensive ab initio simulations of hydrogen-helium mixtures along the isentropes of three representative objects. In particular, we determine the heat capacities, the ther...

We present thermodynamic material and transport properties for the extreme conditions prevalent in the interiors of massive giant planets and brown dwarfs. They are obtained from extensive \textit{ab initio} simulations of hydrogen-helium mixtures along the isentropes of three representative objects. In particular, we determine the heat capacities,...

The validity of the widely used linear mixing approximation for the equations of state (EOS) of planetary ices is investigated at pressure-temperature conditions typical for the interior of Uranus and Neptune. The basis of this study are ab initio data ranging up to 1000 GPa and 20 000 K calculated via density functional theory molecular dynamics s...

The strikingly low luminosity of Uranus (Teff ~ Teq) constitutes a long-standing challenge to our understanding of Ice Giant planets. Here we present the first Uranus structure and evolution models that are constructed to agree with both the observed low luminosity and the gravity field data. Our models make use of modern ab initio equations of sta...

We have performed finite-temperature density functional theory molecular dynamics simulations on dense methane, ammonia, and water mixtures (CH4:NH3:H2O) for various compositions and temperatures (2000 K ≤ T ≤ 10 000 K) that span a set of possible conditions in the interiors of ice-giant exoplanets. The equation-of-state, pair distribution function...

We report four structures for the 1:1 water-ammonia mixture showing superionic behavior at high temperature with the space groups P4/nmm, Ima2, Pma2 and Pm, which have been identified from evolutionary random structure search calculations at 0~K. Analyzing the respective pair distribution functions and diffusive properties the superionic phase is f...

We present an equation of state as well as a phase diagram of ammonia at high pressures and high temperatures derived from ab initio molecular dynamics simulations. The predicted phases of ammonia are characterized by analyzing diffusion coefficients and structural properties. Both the phase diagram and the subsequently computed Hugoniot curves are...

We determine basic thermodynamic and transport properties of hydrogen-helium-water mixtures for the extreme conditions along Jupiter's adiabat via ab initio simulations, which are compiled in an accurate and consistent data set. In particular, we calculate the electrical and thermal conductivity, the shear and longitudinal viscosity, and diffusion...