Ion-Induced Surface Charge Dynamics in Freestanding Monolayers of Graphene and MoS_{2} Probed by the Emission of Electrons.

We compare the ion-induced electron emission from freestanding monolayers of graphene and MoS_{2} to find a sixfold higher number of emitted electrons for graphene even though both materials have similar work functions. An effective single-band Hubbard model explains this finding by a charge-up in MoS_{2} that prevents low energy electrons from escaping the surface within a period of a few femtoseconds after ion impact. We support these results by measuring the electron energy distribution for correlated pairs of electrons and transmitted ions. The majority of emitted primary electrons have an energy below 10 eV and are therefore subject to the dynamic charge-up effects at surfaces.

Momentum distribution function and short-range correlations of the warm dense electron gas: Ab initio quantum Monte Carlo results.

In a classical plasma the momentum distribution, n(k), decays exponentially, for large k, and the same is observed for an ideal Fermi gas. However, when quantum and correlation effects are relevant simultaneously, an algebraic decay, n_{∞}(k)∼k^{-8} has been predicted. This is of relevance for cross sections and threshold processes in dense plasmas that depend on the number of energetic particles. Here we present extensive ab initio results for the momentum distribution of the nonideal uniform electron gas at warm dense matter conditions. Our results are based on first principle fermionic path integral Monte Carlo (CPIMC) simulations and clearly confirm the k^{-8} asymptotic. This asymptotic behavior is directly linked to short-range correlations which are analyzed via the on-top pair distribution function (on-top PDF), i.e., the PDF of electrons with opposite spin. We present extensive results for the density and temperature dependence of the on-top PDF and for the momentum distribution in the entire momentum range.

Nonlinear Electronic Density Response in Warm Dense Matter.

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.

Achieving the Scaling Limit for Nonequilibrium Green Functions Simulations.

The dynamics of strongly correlated fermions following an external excitation reveals extremely rich collective quantum effects. Examples are fermionic atoms in optical lattices, electrons in correlated materials, and dense quantum plasmas. Presently, the only quantum-dynamics approach that rigorously describes these processes in two and three dimensions is the nonequilibrium Green functions (NEGF) method. However, NEGF simulations are computationally expensive due to their T^{3} scaling with the simulation duration T. Recently, T^{2} scaling was achieved with the generalized Kadanoff-Baym ansatz (GKBA), for second-order Born (SOA) selfenergies, which has substantially extended the scope of NEGF simulations. Here we demonstrate that GKBA-NEGF simulations can be performed with order T^{1} scaling, both for SOA and GW selfenergies, and point out the remarkable capabilities of this approach.

Correlated Topological States in Graphene Nanoribbon Heterostructures.

Finite graphene nanoribbon (GNR) heterostructures host intriguing topological in-gap states (Rizzo, D. J.; et al. Nature2018, 560, 204). These states may be localized either at the bulk edges or at the ends of the structure. Here we show that correlation effects (not included in previous density functional simulations) play a key role in these systems: they result in increased magnetic moments at the ribbon edges accompanied by a significant energy renormalization of the topological end states, even in the presence of a metallic substrate. Our computed results are in excellent agreement with the experiments. Furthermore, we discover a striking, novel mechanism that causes an energy splitting of the nonzero-energy topological end states for a weakly screened system. We predict that similar effects should be observable in other GNR heterostructures as well.

Doublon Formation by Ions Impacting a Strongly Correlated Finite Lattice System.

Strongly correlated systems of fermions have a number of exciting collective properties. Among them, the creation of a lattice that is occupied by doublons, i.e., two quantum particles with opposite spins, offers interesting electronic properties. In the past a variety of methods have been proposed to control doublon formation, both, spatially and temporally. Here, a novel mechanism is proposed and verified by exact diagonalization and nonequilibrium Green functions simulations-fermionic doublon creation by the impact of energetic ions. We report the formation of a nonequilibrium steady state with homogeneous doublon distribution. The effect should be particularly important for strongly correlated finite systems, such as graphene nanoribbons, and directly observable with fermionic atoms in optical lattices.

Configuration path integral Monte Carlo approach to the static density response of the warm dense electron gas.

Precise knowledge of the static density response function (SDRF) of the uniform electron gas serves as key input for numerous applications, most importantly for density functional theory beyond generalized gradient approximations. Here we extend the configuration path integral Monte Carlo (CPIMC) formalism that was previously applied to the spatially uniform electron gas to the case of an inhomogeneous electron gas by adding a spatially periodic external potential. This procedure has recently been successfully used in permutation blocking path integral Monte Carlo simulations (PB-PIMC) of the warm dense electron gas [T. Dornheim et al., Phys. Rev. E 96, 023203 (2017)], but this method is restricted to low and moderate densities. Implementing this procedure into CPIMC allows us to obtain highly accurate finite temperature results for the SDRF of the electron gas at high to moderate densities closing the gap left open by the PB-PIMC data. In this paper, we demonstrate how the CPIMC formalism can be efficiently extended to the spatially inhomogeneous electron gas and present the first data points. Finally, we discuss finite size errors involved in the quantum Monte Carlo results for the SDRF in detail and present a solution how to remove them that is based on a generalization of ground state techniques.

Permutation-blocking path-integral Monte Carlo approach to the static density response of the warm dense electron gas.

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.

Ab initio Exchange-Correlation Free Energy of the Uniform Electron Gas at Warm Dense Matter Conditions.

In a recent Letter [T. Dornheim et al., Phys. Rev. Lett. 117, 156403 (2016)PRLTAO0031-900710.1103/PhysRevLett.117.156403], we presented the first quantum Monte Carlo (QMC) results for the warm dense electron gas in the thermodynamic limit. However, a complete parametrization of the exchange-correlation free energy with respect to density, temperature, and spin polarization remained out of reach due to the absence of (i) accurate QMC results below θ=k_{B}T/E_{F}=0.5 and (ii) QMC results for spin polarizations different from the paramagnetic case. Here we overcome both remaining limitations. By closing the gap to the ground state and by performing extensive QMC simulations for different spin polarizations, we are able to obtain the first completely ab initio exchange-correlation free energy functional; the accuracy achieved is an unprecedented ∼0.3%. This also allows us to quantify the accuracy and systematic errors of various previous approximate functionals.

Ab Initio Quantum Monte Carlo Simulation of the Warm Dense Electron Gas in the Thermodynamic Limit.

We perform ab initio quantum Monte Carlo (QMC) simulations of the warm dense uniform electron gas in the thermodynamic limit. By combining QMC data with the linear response theory, we are able to remove finite-size errors from the potential energy over the substantial parts of the warm dense regime, overcoming the deficiencies of the existing finite-size corrections by Brown et al. [Phys. Rev. Lett. 110, 146405 (2013)]. Extensive new QMC results for up to N=1000 electrons enable us to compute the potential energy V and the exchange-correlation free energy F_{xc} of the macroscopic electron gas with an unprecedented accuracy of |ΔV|/|V|,|ΔF_{xc}|/|F|_{xc}∼10^{-3}. A comparison of our new data to the recent parametrization of F_{xc} by Karasiev et al. [Phys. Rev. Lett. 112, 076403 (2014)] reveals significant deviations to the latter.

Permutation blocking path integral Monte Carlo approach to the uniform electron gas at finite temperature.

The uniform electron gas (UEG) at finite temperature is of high current interest due to its key relevance for many applications including dense plasmas and laser excited solids. In particular, density functional theory heavily relies on accurate thermodynamic data for the UEG. Until recently, the only existing first-principle results had been obtained for N = 33 electrons with restricted path integral Monte Carlo (RPIMC), for low to moderate density, rs=r¯/aB≳1. These data have been complemented by configuration path integral Monte Carlo (CPIMC) simulations for rs ≤ 1 that substantially deviate from RPIMC towards smaller rs and low temperature. In this work, we present results from an independent third method-the recently developed permutation blocking path integral Monte Carlo (PB-PIMC) approach [T. Dornheim et al., New J. Phys. 17, 073017 (2015)] which we extend to the UEG. Interestingly, PB-PIMC allows us to perform simulations over the entire density range down to half the Fermi temperature (θ = kBT/EF = 0.5) and, therefore, to compare our results to both aforementioned methods. While we find excellent agreement with CPIMC, where results are available, we observe deviations from RPIMC that are beyond the statistical errors and increase with density.

Ion potential in warm dense matter: wake effects due to streaming degenerate electrons.

The effective dynamically screened potential of a classical ion in a stationary flowing quantum plasma at finite temperature is investigated. This is a key quantity for thermodynamics and transport of dense plasmas in the warm-dense-matter regime. This potential has been studied before within hydrodynamic approaches or based on the zero temperature Lindhard dielectric function. Here we extend the kinetic analysis by including the effects of finite temperature and of collisions based on the Mermin dielectric function. The resulting ion potential exhibits an oscillatory structure with attractive minima (wakes) and, thus, strongly deviates from the static Yukawa potential of equilibrium plasmas. This potential is analyzed in detail for high-density plasmas with values of the Brueckner parameter in the range 0.1≤r(s)≤1 for a broad range of plasma temperature and electron streaming velocity. It is shown that wake effects become weaker with increasing temperature of the electrons. Finally, we obtain the minimal electron streaming velocity for which attraction between ions occurs. This velocity turns out to be less than the electron Fermi velocity. Our results allow for reliable predictions of the strength of wake effects in nonequilibrium quantum plasmas with fast streaming electrons showing that these effects are crucial for transport under warm-dense-matter conditions, in particular for laser-matter interaction, electron-ion temperature equilibration, and stopping power.

Dynamics of strongly correlated and strongly inhomogeneous plasmas.

Kinetic and fluid equations are derived for the dynamics of classical inhomogeneous trapped plasmas in the strong coupling regime. The starting point is an extended Singwi-Tosi-Land-Sjölander (STLS) ansatz for the dynamic correlation function, which is allowed to depend on time and both particle coordinates separately. The time evolution of the correlation function is determined from the second equation of the Bogolyubov-Born-Green-Kirkwood-Yvon hierarchy. We study the equations in the linear limit and derive a nonlocal equation for the fluid displacement field. Comparisons to first-principles molecular dynamics simulations reveal an excellent quality of our approach thereby overcoming the limitations of the broadly used STLS scheme.

Magnetoplasmons in rotating dusty plasmas.

A rotating dusty plasma apparatus was constructed to provide the possibility of experimental emulation of extremely high magnetic fields by means of the Coriolis force, observable in a corotating measurement frame. We present collective excitation spectra for different rotation rates with a magnetic induction equivalent of up to 3200 T. We identify the onset of magnetoplasmon-equivalent mode dispersion in the rotating macroscopic two-dimensional single-layer dusty plasma. The experimental results are supported by molecular dynamics simulations of 2D magnetized Yukawa systems.

Melting scenarios for three-dimensional dusty plasma clusters.

The melting transition of finite three-dimensional dust clouds (Yukawa balls) from a solid-like to a liquid-like state is systematically studied with high spatial and temporal resolution of the individual grains by means of stereoscopy. Two different melting scenarios are reported: Melting is induced first by an increase of plasma power, and second by laser-induced heating. The experiments confirm that melting starts with a loss of orientational correlation, followed by a loss of the radial order upon further heating. While the plasma-power melting is driven via the ion wakefield, laser heating provides a more equilibrium scenario. The internal loss of correlations is well captured by the triple correlation function (TCF) which is insensitive to particle exchanges and the rotation of the cluster as a whole. The critical Coulomb coupling parameter for N=35 is determined as Γ(crit)≈570. The experimental findings are in good agreement with thermodynamic Monte Carlo simulations.

Two-photon ionization of helium studied with the multiconfigurational time-dependent Hartree-Fock method.

The multiconfigurational time-dependent Hartree-Fock method (MCTDHF) is applied for simulations of the two-photon ionization of helium. We present results for the single and double ionizations from the ground state for photon energies in the nonsequential regime and compare them to direct solutions of the Schrödinger equation using the time-dependent (full) configuration interaction (TDCI) method. We find that the single ionization is accurately reproduced by MCTDHF, whereas the double ionization results correctly capture the main trends of TDCI.