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It is demonstrated how the static electron-electron structure factor in warm dense matter can be obtained from density functional theory in combination with quantum Monte Carlo data. In contrast to theories assuming well-separated bound and free states, this ah initio approach yields also valid results for systems close to the Mott transition (pressure ionization), where bound states are strongly modified and merge with the continuum. The approach is applied to x-ray Thomson scattering and compared to predictions of the Chihara formula whereby we use the ion-ion and electron-ion structure from the same simulations. The results show significant deviations of the screening cloud from the often applied Debye-like form. [ABSTRACT FROM AUTHOR]

We present the first direct experimental test of the complex ion structure in liquid carbon at pressures around 100 GPa, using spectrally resolved x-ray scattering from shock-compressed graphite samples. Our results confirm the structure predicted by ab initio quantum simulations and demonstrate the importance of chemical bonds at extreme conditions similar to those found in the interiors of giant planets. The evidence presented here thus provides a firmer ground for modeling the evolution and current structure of carbon-bearing icy giants like Neptune, Uranus, and a number of extrasolar planets. [ABSTRACT FROM AUTHOR]

We present a reduced model for the energy transfer via coupled collective modes in two-temperature plasmas based on quantum statistical theory. The model is compared with exact numerical evaluations of the coupled-mode (CM) energy transfer rate and with alternative reduced approaches over a range of conditions in the warm dense matter (WDM) and inertial confinement fusion (ICF) regimes. Our approach shows excellent agreement with an exact treatment of the CM rate and supports the importance of the coupled-mode effect for the temperature and energy relaxation in WDM and ICF plasmas. We find that electronic damping of collective ion density fluctuations is crucial for correctly describing the mode spectrum and, thus, the energy exchange. The reduced CM approach is studied over a wide parameter space, enabling us to establish its limits of applicability. [ABSTRACT FROM AUTHOR]

The dynamics of the ion structure in warm dense matter is determined by molecular dynamics simulations using an effective ion-ion potential. This potential is obtained from ab initio simulations and has a strong short-range repulsion added to a screened Coulomb potential. Models based on static or dynamic local field corrections are found to be insufficient to describe the data. An extended Mermin approach, a hydrodynamic model, and the method of moments with local constraints are capable of reproducing the numerical results but have rather limited predictive powers as they all need some numerical data as input. The method of moments is found to be the most promising. [ABSTRACT FROM AUTHOR]

We present results for the ionic structure in hydrocarbons (polystyrene, polyethylene) that were shock compressed to pressures of up to 190 GPa, inducing rapid melting of the samples. The structure of the resulting liquid is then probed using in situ diffraction by an x-ray free electron laser beam, demonstrating the capability to obtain reliable diffraction data in a single shot, even for low-Z samples without long range order. The data agree well with ab initio simulations, validating the ability of such approaches to model mixed samples in states where complex interparticle bonds remain, and showing that simpler models are not necessarily valid. While the results clearly exclude the possibility of complete carbon-hydrogen demixing at the conditions probed, they also, in contrast to previous predictions, indicate that diffraction is not always a sufficient diagnostic for this phenomenon. [ABSTRACT FROM AUTHOR]

We present a quantum theory for the dynamic structure factors in nonequilibrium, correlated, two-component systems such as plasmas or warm dense matter. The polarization function, which is needed as the input for the calculation of the structure factors, is calculated in nonequilibrium based on a perturbation expansion in the interaction strength. To make our theory applicable for x-ray scattering, a generalized Chihara decomposition for the total electron structure factor in nonequilibrium is derived. Examples are given and the influence of correlations and exchange on the structure and the x-ray-scattering spectrum are discussed for a model nonequilibrium distribution, as often encountered during laser heating of materials, as well as for two-temperature systems. [ABSTRACT FROM AUTHOR]

The uniform electron gas at finite temperature is of key relevance for many applications in dense plasmas, warm dense matter, laser excited solids, and much more. Accurate thermodynamic data for the uniform electron gas are an essential ingredient for many-body theories, in particular, density-functional theory. Recently, first-principles restricted path integral Monte Carlo results became available, which, however, had to be restricted to moderate degeneracy, i.e., low to moderate densities with rs = r/aB ≳ 1. Here we present novel first-principles configuration path integral Monte Carlo results for electrons for rs ≤ 4. We also present quantum statistical data within the e4 approximation that are in good agreement with the simulations at small to moderate rs. [ABSTRACT FROM AUTHOR]

The equation of state of light elements is essential to understand the structure of Jovian planets and inertial confinement fusion research. The Omega laser was used to drive a planar shock wave in the cryogenically cooled deuterium, creating warm dense matter conditions. X-ray scattering was used to determine the spectrum near the boundary of the collective and noncollective scattering regimes using a narrow band x-ray source in backscattering geometry. Our scattering spectra are thus sensitive to the individual electron motion as well as the collective plasma behavior and provide a measurement of the electron density, temperature, and ionization state. Our data are consistent with velocity-interferometry measurements previously taken on the same shocked deuterium conditions and presented by K. Falk et al. [High Energy Density Phys. 8, 76 (2012)]. This work presents a comparison of the two diagnostic systems and offers a detailed discussion of challenges encountered. [ABSTRACT FROM AUTHOR]

The accurate description of electrons at extreme density and temperature is of paramount importance for, e.g., the understanding of astrophysical objects and inertial confinement fusion. In this context, the dynamic structure factor S(q,ω) constitutes a key quantity as it is directly measured in x-ray Thomson scattering experiments and governs transport properties like the dynamic conductivity. In this work, we present the first ab initio results for S(q,ω) by carrying out extensive path integral Monte Carlo simulations and developing a new method for the required analytic continuation, which is based on the stochastic sampling of the dynamic local field correction G(q,ω). In addition, we find that the so-called static approximation constitutes a promising opportunity to obtain high-quality data for S(q,ω) over substantial parts of the warm dense matter regime. [ABSTRACT FROM AUTHOR]

The energy loss of light ions in dense plasmas is investigated with special focus on low to medium projectile energies, i.e., at velocities where the maximum of the stopping power occurs. In this region, exceptionally large theoretical uncertainties remain and no conclusive experimental data are available. We perform simulations of beamplasma configurations well suited for an experimental test of ion energy loss in highly ionized, laser-generated carbon plasmas. The plasma parameters are extracted from two-dimensional hydrodynamic simulations, and a Monte Carlo calculation of the charge-state distribution of the projectile ion beam determines the dynamics of the ion charge state over the whole plasma profile. We show that the discrepancies in the energy loss predicted by different theoretical models are as high as 20-30%, making these theories well distinguishable in suitable experiments. [ABSTRACT FROM AUTHOR]

Detailed measurements of the electron densities, temperatures, and ionization states of compressed CH shells approaching pressures of 50 Mbar are achieved with spectrally resolved x-ray scattering. Laser-produced 9 keV x-rays probe the plasma during the transient state of three-shock coalescence. High signal-to-noise x-ray scattering spectra show direct evidence of continuum depression in highly degenerate warm dense matter states with electron densities ne>1024??cm-3. The measured densities and temperatures agree well with radiation-hydrodynamic modeling when accounting for continuum lowering in calculations that employ detailed configuration accounting. [ABSTRACT FROM AUTHOR]

The strong ion-ion correlation peak characteristic of warm dense matter (WDM) is observed for the first time using simultaneous angularly, temporally, and spectrally resolved x-ray scattering measurements in laser-driven shock-compressed aluminum. Laser-produced molybdenum x-ray line emission at an energy of 17.9 keV is employed to probe aluminum compressed to a density of ρ>8 g/cm³. We observe a well pronounced peak in the static structure factor at a wave number of k=4.0 Å-1. The measurements of the magnitude and position of this correlation peak are precise enough to test different theoretical models for the ion structure and show that only models taking the complex interaction in WDM into account agree with the data. This also demonstrates a new highly accurate diagnostic to directly measure the state of compression of warm dense matter. [ABSTRACT FROM AUTHOR]

The Fermi-degenerate plasma conditions created in liquid deuterium by a laser-ablation—driven shock wave were probed with noncollective, spectrally resolved, inelastic x-ray Thomson scattering employing CI Lyα line emission at 2.96 keV. These first x-ray Thomson scattering measurements of the microscopic properties of shocked deuterium show an inferred spatially averaged electron temperature of 8 ± 5 eV, an electron density of 2.2(±0.5) × 1023 cm-3, and an ionization of 0.8 (- 0.25, +0.15). Two-dimensional hydrodynamic simulations using equation-of-state models suited for the extreme parameters occurring in inertial confinement fusion research and planetary interiors are consistent with the experimental results. [ABSTRACT FROM AUTHOR]

We present results from the SPring-8 Angstrom Compact free electron LAser facility, where we used a high intensity (∼1020  W/cm²) x-ray pump x-ray probe scheme to observe changes in the ionic structure of silicon induced by x-ray heating of the electrons. By avoiding Laue spots in the scattering signal from a single crystalline sample, we observe a rapid rise in diffuse scattering and a transition to a disordered, liquidlike state with a structure significantly different from liquid silicon. The disordering occurs within 100 fs of irradiation, a timescale that agrees well with first principles simulations, and is faster than that predicted by purely inertial behavior, suggesting that both the phase change and disordered state reached are dominated by Coulomb forces. This method is capable of observing liquid scattering without masking signal from the ambient solid, allowing the liquid structure to be measured throughout and beyond the phase change. [ABSTRACT FROM AUTHOR]

The properties of plasmas in the low-density limit are described by virial expansions. Analytical expressions are known from Green's function approaches only for the first three virial coefficients. Accurate path-integral Monte Carlo (PIMC) simulations have recently been performed for the uniform electron gas, allowing the virial expansions to be analyzed and interpolation formulas to be derived. The exact expression for the second virial coefficient is used to test the accuracy of the PIMC simulations and the range of validity of the interpolation formula of Groth et al. [Phys. Rev. Lett. 119, 135001 (2017)0031-900710.1103/PhysRevLett.119.135001], and we discuss the fourth virial coefficient, which is not exactly known yet. Combining PIMC simulations with benchmarks from exact virial expansion results would allow us to obtain more accurate representations of the equation of state for parameter ranges of conditions which are of interest, e.g., for helioseismology.

The properties of hydrogen at warm dense matter (WDM) conditions are of high importance for the understanding of astrophysical objects and technological applications such as inertial confinement fusion. In this work, we present extensive ab initio path integral Monte Carlo results for the electronic properties in the Coulomb potential of a fixed ionic configuration. This gives us unique insights into the complex interplay between the electronic localization around the protons with their density response to an external harmonic perturbation. We find qualitative agreement between our simulation data and a heuristic model based on the assumption of a local uniform electron gas model, but important trends are not captured by this simplification. In addition to being interesting in their own right, we are convinced that our results will be of high value for future projects, such as the rigorous benchmarking of approximate theories for the simulation of WDM, most notably density functional theory.

We combine ab initio path integral Monte Carlo (PIMC) simulations with fixed ion configurations from density functional theory molecular dynamics (DFT-MD) simulations to solve the electronic problem for hydrogen under warm dense matter conditions [Böhme et al., Phys. Rev. Lett. 129, 066402 (2022)0031-900710.1103/PhysRevLett.129.066402]. The problem of path collapse due to the Coulomb attraction is avoided by utilizing the pair approximation, which is compared against the simpler Kelbg pair potential. We find very favorable convergence behavior towards the former. Since we do not impose any nodal restrictions, our PIMC simulations are afflicted with the notorious fermion sign problem, which we analyze in detail. While computationally demanding, our results constitute an exact benchmark for other methods and approximations within DFT. Our setup gives us the unique capability to study important properties of warm dense hydrogen such as the electronic static density response and exchange-correlation kernel without any model assumptions, which will be very valuable for a variety of applications such as the interpretation of experiments and the development of new XC functionals.

The properties of hydrogen under extreme conditions are important for many applications, including inertial confinement fusion and astrophysical models. A key quantity is given by the electronic density response to an external perturbation, which is probed in x-ray Thomson scattering experiments-the state of the art diagnostics from which system parameters like the free electron density n_{e}, the electronic temperature T_{e}, and the charge state Z can be inferred. In this work, we present highly accurate path integral Monte Carlo results for the static electronic density response of hydrogen. We obtain the static exchange-correlation (XC) kernel K_{XC}, which is of central relevance for many applications, such as time-dependent density functional theory. This gives us a first unbiased look into the electronic density response of hydrogen in the warm-dense matter regime, thereby opening up a gamut of avenues for future research.

We carry out extensive direct path integral Monte Carlo (PIMC) simulations of the uniform electron gas (UEG) at finite temperature for different values of the spin-polarization ξ. This allows us to unambiguously quantify the impact of spin effects on the momentum distribution function n(k) and related properties. We find that interesting physical effects like the interaction-induced increase in the occupation of the zero-momentum state n(0) substantially depend on ξ. Our results further advance the current understanding of the UEG as a fundamental model system, and are of practical relevance for the description of transport properties of warm dense matter in an external magnetic field. All PIMC results are freely available online and can be used as a benchmark for the development of methods and applications.

We present an effective static approximation (ESA) to the local field correction (LFC) of the electron gas that enables highly accurate calculations of electronic properties like the dynamic structure factor S(q,ω), the static structure factor S(q), and the interaction energy v. The ESA combines the recent neural-net representation by T. Dornheim et al., [J. Chem. Phys. 151, 194104 (2019)JCPSA60021-960610.1063/1.5123013] of the temperature-dependent LFC in the exact static limit with a consistent large wave-number limit obtained from quantum Monte Carlo data of the on-top pair distribution function g(0). It is suited for a straightforward integration into existing codes. We demonstrate the importance of the LFC for practical applications by reevaluating the results of the recent x-ray Thomson scattering experiment on aluminum by Sperling et al. [Phys. Rev. Lett. 115, 115001 (2015)PRLTAO0031-900710.1103/PhysRevLett.115.115001]. We find that an accurate incorporation of electronic correlations in terms of the ESA leads to a different prediction of the inelastic scattering spectrum than obtained from state-of-the-art models like the Mermin approach or linear-response time-dependent density functional theory. Furthermore, the ESA scheme is particularly relevant for the development of advanced exchange-correlation functionals in density functional theory.

We systematically investigate finite-size effects in the dynamic structure factor S(q,ω) of the uniform electron gas obtained via the analytic continuation of ab initio path integral Monte Carlo data for the imaginary-time density-density correlation function F(q,τ). Using the recent scheme by Dornheim et al. [Phys. Rev. Lett. 121, 255001 (2018)PRLTAO0031-900710.1103/PhysRevLett.121.255001], we find that the reconstructed spectra are not afflicted with any finite-size effects for as few as N=14 electrons both at warm dense matter (WDM) conditions and at the margins of the strongly correlated electron liquid regime. Our results further corroborate the high quality of our current description of the dynamic density response of correlated electrons, which is of high importance for many applications in WDM theory and beyond.

Warm dense matter (WDM)-an extreme state with high temperatures and densities that occurs, e.g., in astrophysical objects-constitutes one of the most active fields in plasma physics and materials science. These conditions can be realized in the lab by shock compression or laser excitation, and the most accurate experimental diagnostics is achieved with lasers and free electron lasers which is theoretically modeled using linear response theory. Here, we present first ab initio path integral Monte Carlo results for the nonlinear density response of correlated electrons in WDM and show that for many situations of experimental relevance nonlinear effects cannot be neglected.

The static density response of the uniform electron gas is of fundamental importance for numerous applications. Here we employ the recently developed ab initio permutation blocking path integral Monte Carlo (PB-PIMC) technique [T. Dornheim et al., New J. Phys. 17, 073017 (2015)10.1088/1367-2630/17/7/073017] to carry out extensive simulations of the harmonically perturbed electron gas at warm dense matter conditions. In particular, we investigate in detail the validity of linear response theory and demonstrate that PB-PIMC allows us to obtain highly accurate results for the static density response function and, thus, the static local field correction. A comparison with dielectric approximations to our new ab initio data reveals the need for an exact treatment of correlations. Finally, we consider a superposition of multiple perturbations and discuss the implications for the calculation of the static response function.

Laser-produced proton beams have been used to achieve ultrafast volumetric heating of carbon samples at solid density. The isochoric melting of carbon was probed by a scattering of x rays from a secondary laser-produced plasma. From the scattering signal, we have deduced the fraction of the material that was melted by the inhomogeneous heating. The results are compared to different theoretical approaches for the equation of state which suggests modifications from standard models.

We employ a pseudopotential approach to investigate the screening of ionic cores in partially ionized plasmas. Here, the effect of the tightly bound electrons is condensed into an effective potential between the (free) valence electrons and the ionic cores. Even for weak electron-ion coupling, the corresponding screening clouds show strong modifications from the Debye result for elements heavier than helium. Modifications of the theoretically predicted x-ray scattering signal and implications on measurements are discussed.

A quantum kinetic approach for the energy relaxation in strongly coupled plasmas with different electron and ion temperatures is presented. Based on the density operator formalism, we derive a balance equation for the energies of electrons and ions connecting kinetic, correlation, and exchange energies with a quite general expression for the electron-ion energy-transfer rate. The latter is given in terms of the correlation function of density fluctuations which allows for a derivation of increasingly realistic approximation schemes including a coupled-mode expression. The equilibration of the contributions of the total energy including the species temperatures in dense hydrogen and beryllium relevant for inertial confinement fusion is investigated as an example.

We present the first ultrafast temporally, spectrally, and angularly resolved x-ray scattering measurements from shock-compressed matter. The experimental spectra yield the absolute elastic and inelastic scattering intensities from the measured density of free electrons. Laser-compressed lithium-hydride samples are well characterized by inelastic Compton and plasmon scattering of a K-alpha x-ray probe providing independent measurements of temperature and density. The data show excellent agreement with the total intensity and structure when using the two-species form factor and accounting for the screening of ion-ion interactions.

We have performed short-pulse x-ray scattering measurements on laser-driven shock-compressed plastic samples in the warm dense matter regime, providing instantaneous snapshots of the system evolution. Time-resolved and angularly resolved scattered spectra sensitive to the correlation effects in the plasma show the appearance of short-range order within a few interionic separations. Comparison with radiation-hydrodynamic simulations indicates that the shocked plastic is compressed with a temperature of a few electron volts. These results are important for the understanding of the thermodynamic behavior of strongly correlated matter for conditions relevant to both laboratory astrophysics and inertial confinement fusion research.

We investigate the microscopic structure of strongly coupled ions in warm dense matter using ab initio simulations and hypernetted chain (HNC) equations. We demonstrate that an approximate treatment of quantum effects by weak pseudopotentials fails to describe the highly degenerate electrons in warm dense matter correctly. However, one-component HNC calculations for the ions agree well with first-principles simulations if a linearly screened Coulomb potential is used. These HNC results can be further improved by adding a short-range repulsion that accounts for bound electrons. Examples are given for recently studied light elements, lithium and beryllium, and for aluminum where the extra short-range repulsion is essential.

We investigate the capabilities of dynamic compression by intense heavy ion beams to yield information about the high pressure phases of hydrogen. Employing ab initio simulations and experimental data, a new wide range equation of state for hydrogen is constructed. The results show that the melting line up to its maximum as well as the transition from molecular fluids to fully ionized plasmas can be tested with the beam parameters soon to be available. We demonstrate that x-ray scattering can distinguish between phases and dissociation states.

We calculate thermodynamic properties for a dense hydrogen plasma and a quantum electron gas using thermodynamic Green's function techniques. Our perturbation approach is appropriate to give reliable results in the weak coupling regime. In particular, the contribution of the exchange term of the order e(4) is fully included for the nondegenerate case as well as for the dense highly degenerate quantum region. We compare our results for the equation of state with data obtained by different numerical simulations.

The mean value of the kinetic energy of a quantum plasma is investigated in Hartree-Fock and Montroll-Ward approximations using the method of thermodynamic Green's functions. Usually, one finds the kinetic energy to be larger than that of an ideal plasma due to the interaction between the particles in the system. However, also the opposite case is possible, i.e., a decrease of the kinetic energy compared to that of the ideal gas. This special correlation effect is found for temperatures of about 10(6) K and densities between 10(21) and 10(26) cm(-3). Here, the single-particle distribution function is shifted towards smaller momenta, and the binary distribution is changed.