arXiv subjects

Jerome Daligault

Publications and source records attributed to Jerome Daligault.

At least 19 recordsLinked to original sources

arXiv2022

Direct observation of enhanced electron-phonon coupling in copper nanoparticles in the warm-dense matter regime

Warm-dense matter (WDM) is a highly-excited state that lies at the confluence of solids, plasmas, and liquids and that cannot be described by equilibrium theories. The transient nature of this state when created in a laboratory, as well as the difficulties in probing the strongly-coupled interactions between the electrons and the ions, make it challenging to develop a complete understanding of matter in this regime. In this work, by exciting isolated ~8 nm nanoparticles with a femtosecond laser below the ablation threshold, we create uniformly-excited WDM. We then use photoelectron spectroscopy to track the instantaneous electron temperature and directly extract the strongest electron-ion coupling observed experimentally to date. By directly comparing with state-of-the-art theories, we confirm that the superheated nanoparticles lie at the boundary between hot solids and plasmas, with associated strong electron-ion coupling. This is evidenced both by the fast energy loss of electrons to ions, as well as a strong modulation of the electron temperature by acoustic oscillations in the nanoparticle. This work demonstrates a new route for experimental exploration and theoretical validation of the exotic properties of WDM.

physics.plasm-ph↗

arXiv2021

Phase Separation in Ultramassive White Dwarfs

Ultramassive white dwarfs are extreme endpoints of stellar evolution. Recent findings, such as a missing multi-Gyr cooling delay for a number of ultramassive white dwarfs and a white dwarf with a quasi-Chandrasekhar mass, motivate a better understanding of their evolution. A key process still subject to important uncertainties is the crystallization of their dense cores, which are generally assumed to be constituted of $^{16}$O, $^{20}$Ne, and a mixture of several trace elements (most notably $^{23}$Na and $^{24}$Mg). In this work, we use our recently developed Clapeyron integration technique to compute accurate phase diagrams of three-component mixtures relevant to the modeling of O/Ne ultramassive white dwarfs. We show that, unlike the phase separation of $^{22}$Ne impurities in C/O cores, the phase separation of $^{23}$Na impurities in O/Ne white dwarfs cannot lead to the enrichment of their cores in $^{23}$Na via a distillation process. This severely limits the prospect of transporting large quantities of $^{23}$Na toward the center of the star, as needed in the white dwarf core collapse mechanism recently proposed by Caiazzo et al. We also show that despite representing $\approx 10\%$ of the ionic mixture, $^{23}$Na and $^{24}$Mg impurities only have a negligible impact on the O/Ne phase diagram, and the two-component O/Ne phase diagram can be safely used in white dwarf evolution codes. We provide analytic fits to our high-accuracy O/Ne phase diagram for implementation in white dwarf models.

astro-ph.SR↗

arXiv2021

Direct Evaluation of the Phase Diagrams of Dense Multicomponent Plasmas by Integration of the Clapeyron Equations

Accurate phase diagrams of multicomponent plasmas are required for the modeling of dense stellar plasmas, such as those found in the cores of white dwarf stars and the crusts of neutron stars. Those phase diagrams have been computed using a variety of standard techniques, which suffer from physical and computational limitations. Here, we present an efficient and accurate method that overcomes the drawbacks of previously used approaches. In particular, finite-size effects are avoided as each phase is calculated separately; the plasma electrons and volume changes are explicitly taken into account; and arbitrary analytic fits to simulation data are avoided. Furthermore, no simulations at uninteresting state conditions, i.e., away from the phase coexistence curves, are required, which improves the efficiency of the technique. The method consists of an adaptation of the so-called Gibbs-Duhem integration approach to electron-ion plasmas, where the coexistence curve is determined by direct numerical integration of its underlying Clapeyron equation. The thermodynamics properties of the coexisting phases are evaluated separately using Monte Carlo simulations in the isobaric semi-grand canonical ensemble. We describe this Monte Carlo-based Clapeyron integration method, including its basic principles, our extension to electron-ion plasmas, and our numerical implementation. We illustrate its applicability and benefits with the calculation of the melting curve of dense C/O plasmas under conditions relevant for white dwarf cores and provide analytic fits to implement this new melting curve in white dwarf models. While this work focuses on the liquid-solid phase boundary of dense two-component plasmas, a wider range of physical systems and phase boundaries are within the scope of the Clapeyron integration method, which had until now only been applied to simple model systems of neutral particles.

physics.plasm-ph↗

arXiv2021

$^{22}$Ne Phase Separation As A Solution To The Ultramassive White Dwarf Cooling Anomaly

The precise astrometric measurements of the Gaia Data Release 2 have opened the door to detailed tests of the predictions of white dwarf cooling models. Significant discrepancies between theory and observations have been identified, the most striking affecting ultramassive white dwarfs. Cheng et al. (2019) found that a small fraction of white dwarfs on the so-called Q branch must experience an extra cooling delay of $\sim 8\,$Gyr not predicted by current models. $^{22}$Ne phase separation in a crystallizing C/O white dwarf can lead to a distillation process that efficiently transports $^{22}$Ne toward its center, thereby releasing a considerable amount of gravitational energy. Using state-of-the-art Monte Carlo simulations, we show that this mechanism can largely resolve the ultramassive cooling anomaly if the delayed population consists of white dwarfs with moderately above-average $^{22}$Ne abundances. We also argue that $^{22}$Ne phase separation can account for the smaller cooling delay currently missing for models of white dwarfs with more standard compositions.

astro-ph.SR↗

arXiv2020

Universal Character of Atomic Motions at the Liquid-Solid Transition

We show evidence from computer simulations of a universal feature in the atoms dynamics of simple liquids that heralds the freezing transition. We develop a physically transparent model to shed light on the physics responsible for the precursory effect. We find that the freezing point is concomitant with the crossover of two characteristic time scales, namely the average period of oscillation of the liquid configuration in a minimum of the potential energy surface, and the average time separating transits between potential energy minima as a result of the continuous dynamical rearrangement of particles. When entering the undercooled regime, the transit time becomes smaller than the period of oscillation, and the delicate balance between the disordering effects of thermal agitation and the ordering effects of interactions can be destabilized in favor of the periodic order. Finally, we demonstrate that the discovered precursory feature gives rise to a new efficient method for determining the liquid-solid coexistence line of real materials from atomistic simulations, which, unlike other methods commonly used in materials science, does not require knowing the crystalline structure of the solid phase.

cond-mat.stat-mech↗

arXiv2020

Friction Force in Strongly Magnetized Plasmas

A charged particle moving through a plasma experiences a friction force that commonly acts antiparallel to its velocity. It was recently predicted that in strongly magnetized plasmas, in which the plasma particle gyro-frequency exceeds the plasma frequency, the friction also includes a transverse component that is perpendicular to both the velocity and Lorentz force. Here, this prediction is confirmed using molecular dynamics simulations, and it is shown that the relative magnitude of the transverse component increases with plasma coupling strength. This result influences single particle motion and macroscopic transport in strongly magnetized plasmas found in a broad range of applications.

physics.plasm-ph↗

arXiv2020

Nature of Non-Adiabatic Electron-Ion Forces in Liquid Metals

An accurate description of electron-ion interactions in materials is crucial for our understanding of their equilibrium and non-equilibrium properties. Here, we assess the properties of frictional forces experienced by ions in non-crystalline metallic systems, including liquid metals and warm dense plasmas, that arise from electronic excitations driven by the nuclear motion due to the presence of a continuum of low-lying electronic states. To this end, we perform detailed ab-initio calculations of the full friction tensor that characterizes the set of friction forces. The nonadiabatic electron-ion interactions introduce hydrodynamic couplings between the ionic degrees of freedom, which are sizeable between nearest neigbors. The friction tensor is generally inhomogeneous, anisotropic and non-diagonal, especially at lower densities.

cond-mat.dis-nn↗

arXiv2019

Theory of the electron-ion temperature relaxation rate spanning the hot solid metals and plasma phases

We present a theory for the rate of energy exchange between electrons and ions -- also known as the electron-ion coupling factor -- in physical systems ranging from hot solid metals to plasmas, including liquid metals and warm dense matter. The paper provides the theoretical foundations of a recent work [J. Simoni and J. Daligault, Phys. Rev. Lett. {\bf 122}, 205001 (2019)], where first-principles quantum molecular dynamics calculations based on this theory were presented for representative materials and conditions. We first derive a general expression for the electron-ion coupling factor that includes self-consistently the quantum mechanical and statistical nature of electrons, the thermal and disorder effects, and the correlations between particles. We show that our theory reduces to well-known models in limiting cases. In particular, we show that it simplifies to the standard electron-phonon coupling formula in the limit of hot solids with lattice and electronic temperatures much greater than the Debye temperature, and that it extends the electron-phonon coupling formula beyond the harmonic phonon approximation. For plasmas, we show that the theory readily reduces to well-know Spitzer formula in the hot plasma limit, to the Fermi golden rule formula in the limit of weak electron-ion interactions, and to other models proposed to go beyond the latter approximation. We explain that the electron-ion coupling is particularly well adapted to averaged atom models, which offer an effective way to include non-ideal interaction effects to the standard models and at a much reduced computational cost in comparison to first-principles quantum molecular dynamics simulations.

physics.plasm-ph↗

arXiv2019

Mean Force Kinetic Theory: a Convergent Kinetic Theory for Weakly and Strongly Coupled Plasmas

A new closure of the BBGKY hierarchy is developed, which results in a convergent kinetic equation that provides a rigorous extension of plasma kinetic theory into the regime of strong Coulomb coupling. The approach is based on a single expansion parameter which enforces that the exact equilibrium limit is maintained at all orders. Because the expansion parameter does not explicitly depend on the range or the strength of the interaction potential, the resulting kinetic theory does not suffer from the typical divergences at short and long length scales encountered when applying the standard kinetic equations to Coulomb interactions. The approach demonstrates that particles effectively interact via the potential of mean force and that the range of this force determines the size of the collision volume. When applied to a plasma, the collision operator is shown to be related to the effective potential theory [Baalrud and Daligault, Phys. Rev. Lett 110, 235001 (2013)]. The relationship between this and previous kinetic theories is discussed.

physics.plasm-ph↗

arXiv2019

Effects of Coulomb Coupling on Stopping Power and a Link to Macroscopic Transport

Molecular dynamics simulations are used to assess the influence of Coulomb coupling on the energy evolution of charged projectiles in the classical one-component plasma. The average projectile kinetic energy is found to decrease linearly with time when $ν_α/ω_{p} \lesssim 10^{-2}$, where $ν_{α}$ is the Coulomb collision frequency between the projectile and the medium, and $ω_{p}$ is the plasma frequency. Stopping power is obtained from the slope of this curve. In comparison to the weakly coupled limit, strong Coulomb coupling causes the magnitude of the stopping power to increase, the Bragg peak to shift to several times the plasma thermal speed, and for the stopping power curve to broaden substantially. The rate of change of the total projectile kinetic energy averaged over many independent simulations is shown to consist of two measurable components: a component associated with a one-dimensional friction force, and a thermal energy exchange rate. In the limit of a slow and massive projectile, these can be related to the macroscopic transport rates of self-diffusion and temperature relaxation in the plasma. Simulation results are compared with available theoretical models for stopping power, self-diffusion coefficients, and temperature relaxation rates.

physics.plasm-ph↗

arXiv2018

Non-Adiabatic Quantum Molecular Dynamics with Detailed Balance

We present an approach for carrying out non-adiabatic molecular dynamics simulations of systems in which non-adiabatic transitions arise from the coupling between the classical atomic motions and a quasi-continuum of electronic quantum states. Such conditions occur in many research areas, including chemistry at metal surfaces, radiation damage of materials, and warm dense matter physics. The classical atomic motions are governed by stochastic Langevin-like equations, while the quantum electron dynamics is described by a master equation for the populations of the electronic states. These working equations are obtained from a first-principle derivation. Remarkably, unlike the widely used Ehrenfest and surface-hopping methods, the approach naturally satisfies the principle of detailed balance at equilibrium and, therefore, can describe the evolution to thermal equilibrium from an arbitrary initial state. In addition, unlike other schemes, there is no need to explicitly propagate wave functions in time.

physics.comp-ph↗

arXiv2017

Transport Regimes Spanning Magnetization-Coupling Phase Space

The manner in which transport properties vary over the entire parameter-space of coupling and magnetization strength is explored for the first time. Four regimes are identified based on the relative size of the gyroradius compared to other fundamental length scales: the collision mean free path, Debye length, distance of closest approach and interparticle spacing. Molecular dynamics simulations of self-diffusion and temperature anisotropy relaxation spanning the parameter space are found to agree well with the predicted boundaries. Comparison with existing theories reveals regimes where they succeed, where they fail, and where no theory has yet been developed.

physics.plasm-ph↗

arXiv2017

Influence of coupling on thermal forces and dynamic friction in plasmas with multiple ion species

The recently proposed effective potential theory [Phys. Rev. Lett. 110, 235001 (2013)] is used to investigate the influence of coupling on inter-ion-species diffusion and momentum exchange in multi-component plasmas. Thermo-diffusion and the thermal force are found to diminish rapidly as strong coupling onsets. For the same coupling parameters, the dynamic friction coefficient is found to tend to unity. These results provide an impetus for addressing the role of coupling on diffusive processes in inertial confinement fusion experiments.

physics.plasm-ph↗

arXiv2017

Temperature Anisotropy Relaxation of the One-Component Plasma

The relaxation rate of a Maxwellian velocity distribution function that has an initially anisotropic temperature $(T_\parallel \neq T_\perp)$ is an important physical process in space and laboratory plasmas. It is also a canonical example of an energy transport process that can be used to test theory. Here, this rate is evaluated using molecular dynamics simulations of the one-component plasma. Results are compared with the predictions of four kinetic theories; two treating the weakly coupled regime (1) the Landau equation, and (2) the Lenard-Balescu equation, and two that attempt to extend the theory into the strongly coupled regime (3) the effective potential theory and (4) the generalized Lenard-Balescu theory. The role of dynamic screening is studied, and is found to have a negligible influence on this transport rate. Oscillations and a delayed relaxation onset in the temperature profiles are observed at strong coupling, which are not described by the kinetic theories.

physics.plasm-ph↗

arXiv2015

Modified Enskog Kinetic Theory for Strongly Coupled Plasmas

Concepts underlying the Enskog kinetic theory of hard-spheres are applied to include short-range correlation effects in a model for transport coefficients of strongly coupled plasmas. The approach is based on an extension of the effective potential transport theory [S.~D.~Baalrud and J.~Daligault, Phys.~Rev.~Lett.~{\bf 110}, 235001 (2013)] to include an exclusion radius surrounding individual charged particles that is associated with Coulomb repulsion. This is obtained by analogy with the finite size of hard spheres in Enskog's theory. Predictions for the self-diffusion and shear viscosity coefficients of the one-component plasma are tested against molecular dynamics simulations. The theory is found to accurately capture the kinetic contributions to the transport coefficients, but not the potential contributions that arise at very strong coupling ($Γ\gtrsim 30$). Considerations related to a first-principles generalization of Enskog's kinetic equation to continuous potentials are also discussed.

physics.plasm-ph↗

arXiv2014

Effective Potential Theory: A Practical Way to Extend Plasma Transport Theory to Strong Coupling

The effective potential theory is a physically motivated method for extending traditional plasma transport theories to stronger coupling. It is practical in the sense that it is easily incorporated within the framework of the Chapman-Enskog or Grad methods that are commonly applied in plasma physics and it is computationally efficient to evaluate. The extension is to treat binary scatterers as interacting through the potential of mean force, rather than the bare Coulomb or Debye-screened Coulomb potential. This allows for aspects of many-body correlations to be included in the transport coefficients. Recent work has shown that this method accurately extends plasma theory to orders of magnitude stronger coupling when applied to the classical one-component plasma model. The present work shows that similar accuracy is realized for the Yukawa one-component plasma model and it provides a comparison with other approaches.

physics.plasm-ph↗

arXiv2014

Gradient corrections to the exchange-correlation free energy

We develop the first order gradient correction to the exchange-correlation free energy of the homogeneous electron gas for use in finite temperature density functional calculations. Based on this we propose and implement a simple temperature dependent extension for functionals beyond the local density approximation. These finite temperature functionals show improvement over zero temperature functionals as compared to path integral Monte Carlo calculations for deuterium and perform without computational cost increase compared to zero temperature functionals and so should be used for finite temperature calculations.

physics.comp-ph↗

arXiv2014

Fast and accurate quantum molecular dynamics of dense plasmas across temperature regimes

We have developed and implemented a new quantum molecular dynamics approximation that allows fast and accurate simulations of dense plasmas from cold to hot conditions. The method is based on a carefully designed orbital-free implementation of density functional theory (DFT). The results for hydrogen and aluminum are in very good agreement with Kohn-Sham (orbital-based) DFT and path integral Monte Carlo (PIMC) for microscopic features such as the electron density as well as equation of state. The present approach does not scale with temperature and hence extends to higher temperatures than is accessible in Kohn-Sham method and lower temperatures than is accessible by PIMC, while being significantly less computationally expensive than either of those two methods

physics.plasm-ph↗