{\em Ab initio} Quantum Monte Carlo simulation of the warm dense electron gas in the thermodynamic limit

We perform \emph{ab initio} quantum Monte Carlo (QMC) simulations of the warm dense uniform electron gas in the thermodynamic limit. By combining QMC data with linear response theory we are able to remove finite-size errors from the potential energy over the entire warm dense regime, overcoming the deficiencies of the existing finite-size corrections by Brown \emph{et al.}~[PRL \textbf{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 $|\Delta V|/|V|, |\Delta F_{xc}|/|F|_{xc} \sim 10^{-3}$. A comparison of our new data to the recent parametrization of $F_{xc}$ by Karasiev {\em et al.} [PRL {\bf 112}, 076403 (2014)] reveals significant deviations to the latter

Conductance anomalies in quantum wires

We study the conductance threshold of clean nearly straight quantum wires in the magnetic field. As a quantitative example we solve exactly the scattering problem for two-electrons in a wire with planar geometry and a weak bulge. From the scattering matrix we determine conductance via the Landauer-Buettiker formalism. The conductance anomalies found near 0.25(2e^2/h) and 0.75(2e^2/h) are related to a singlet resonance and a triplet resonance, respectively, and survive to temperatures of a few degrees. With increasing in-plane magnetic field the conductance exhibits a plateau at e^2/h, consistent with recent experiments.Comment: Quantum wire with planar geometry; in-plane magnetic fiel

Efficient Exploration of Microstructure-Property Spaces via Active Learning

In materials design, supervised learning plays an important role for optimization and inverse modeling of microstructure-property relations. To successfully apply supervised learning models, it is essential to train them on suitable data. Here, suitable means that the data covers the microstructure and property space sufficiently and, especially for optimization and inverse modeling, that the property space is explored broadly. For virtual materials design, typically data is generated by numerical simulations, which implies that data pairs can be sampled on demand at arbitrary locations in microstructure space. However, exploring the space of properties remains challenging. To tackle this problem, interactive learning techniques known as active learning can be applied. The present work is the first that investigates the applicability of the active learning strategy query-by-committee for an efficient property space exploration. Furthermore, an extension to active learning strategies is described, which prevents from exploring regions with properties out of scope (i.e., properties that are physically not meaningful or not reachable by manufacturing processes)

Ultrafast Heating Induced Suppression of dd-band Dominance in the Electronic Excitation Spectrum of Cuprum

The combination of isochoric heating of solids by free electron lasers (FEL) and in situ diagnostics by X-ray Thomson scattering (XRTS) allows for measurements of material properties at warm dense matter (WDM) conditions relevant for astrophysics, inertial confinement fusion, and material science. In the case of metals, the FEL beam pumps energy directly into electrons with the lattice structure of ions being nearly unaffected. This leads to a unique transient state that gives rise to a set of interesting physical effects, which can serve as a reliable testing platform for WDM theories. In this work, we present extensive linear-response time-dependent density functional theory (TDDFT) results for the electronic dynamic structure factor of isochorically heated copper with a face-centered cubic lattice. At ambient conditions, the plasmon is heavily damped due to the presence of $d$-band excitations, and its position is independent of the wavenumber. In contrast, the plasmon feature starts to dominate the excitation spectrum and has a Bohm-Gross type plasmon dispersion for temperatures $T \geq 4~{\rm eV}$, where the quasi-free electrons in the interstitial region are in the WDM regime. In addition, we analyze the thermal changes in the $d$-band excitations and outline the possibility to use future XRTS measurements of isochorically heated copper as a controlled testbed for WDM theories

Excitation signatures of isochorically heated electrons in solids at finite wavenumber explored from first principles

Ultrafast heating of solids with modern X-ray free electron lasers (XFELs) leads to a unique set of conditions that is characterized by the simultaneous presence of heated electrons in a cold ionic lattice. In this work, we analyze the effect of electronic heating on the dynamic structure factor (DSF) in bulk Aluminium (Al) with a face-centered cubic lattice and in silicon (Si) with a crystal diamond structure using first-principles linear-response time-dependent density functional theory simulations. We find a thermally induced red shift of the collective plasmon excitation in both materials. In addition, we show that the heating of the electrons in Al can lead to the formation of a double-plasmon peak due to the extension of the Landau damping region to smaller wavenumbers. Finally, we demonstrate that thermal effects generate a measurable and distinct signature (peak-valley structure) in the DSF of Si at small frequencies. Our simulations indicate that there is a variety of new features in the spectrum of X-ray-driven solids, specifically at finite momentum transfer, which can probed in upcoming X-ray Thomson scattering (XRTS) experiments at various XFEL facilities

Using the emission of muonic x-rays as a spectroscopic tool for the investigation of the local chemistry of elements

There are several techniques providing quantitative elemental analysis, but very few capable of identifying both the concentration and chemical state of elements. This study presents a systematic investigation of the properties of the X-rays emitted after the atomic capture of negatively charged muons. The probability rates of the muonic transitions possess sensitivity to the electronic structure of materials, thus making the muonic X-ray Emission Spectroscopy complementary to the X-ray Absorption and Emission techniques for the study of the chemistry of elements, and able of unparalleled analysis in case of elements bearing low atomic numbers. This qualitative method is applied to the characterization of light elements-based, energy-relevant materials involved in the reaction of hydrogen desorption from the reactive hydride composite Ca(BH4)2-Mg2NiH4. The origin of the influence of the band-structure on the muonic atom is discussed and the observed effects are attributed to the contribution of the electronic structure to the screening and to the momentum distribution in the muon cascade

Hydrogen sorption in the LiH-LiF-MgB2 system

A composite material in the LiH-LiF-MgB2 system has been synthesized by high-energy ball milling. Some peaks in addition to that of the binary 2LiH-MgB2 and 2LiF-MgB2 systems are observed for the composite material by high-pressure differential scanning calorimetry (HP-DSC), indicating the formation of intermediate phases. In situ synchrotron radiation powder X-ray diffraction (SR-PXD) performed at 60 bar of H-2 and 390 degrees C shows a superposition of both reaction pathways that are typical for 2LiH-MgB2 and 2LiF-MgB2. After hydrogen absorption of the LiH-LiF-MgB2 composite the vibrational modes of LiBH4 were observed by attenuated total reflection infrared (ATR-IR) spectroscopy. The F-19 MAS NMR spectrum of the LiF-LiBH4 sample after heat treatment in hydrogen is strongly dominated by the centerband and spinning sidebands from LiF; in addition, a low-intensity resonance, very similar to that of [BF4](-) ion, is identified

X-ray Thomson scattering absolute intensity from the f-sum rule in the imaginary-time domain

We evaluate the f-sum rule on the dynamic structure factor in the imaginary-time domain as a formally exact and simulation-free means of normalizing X-Ray Thomson Scattering (XRTS) spectra. This circumvents error-prone real-time deconvolution of the source function and facilitates calculating the static structure factor from the properly normalized imaginary-time correlation function. We apply our technique to two distinct sets of experimental data, finding that it is effective for both narrow and broad x-ray sources. This approach could be readily adapted to other scattering spectroscopies