Searcharxiv⌕ Search

arXiv subjects

S. B. Dugdale

Publications and source records attributed to S. B. Dugdale.

At least 19 recordsLinked to original sources

Electron momentum densities from QSGW and $G^0W^0$: Revealing the role of many-body effects within the reduced density matrix

The ground-state many-body electron momentum density, which can be probed by x-ray Compton scattering, holds insights into the electronic structure of materials. Comparisons between the measured so-called Compton profiles and the theoretical ones are invaluable in assessing the successes and failures of the methodology used to generate the theoretical ground-state electronic structure. Here, we present calculations of the Compton profiles of Li, Si, Cr, and Ni using the state-of-the-art QSGW method within the Questaal package compared with density functional theory (DFT), one-shot $GW$ ($G^0W^0$) predictions and with experiment. This comparison reveals significant differences between the QSGW and $G^0W^0$ methods which we attribute to the distinction between the single particle density provided by the QSGW method and the many-body density that we construct from the $G^0W^0$ theory; although in general the QSGW description of the electronic structure is superior to that of $G^0W^0$, we find the use of the many-body reduced density matrix is key to improving the agreement of the Compton profile with experiment.

cond-mat.str-el↗

Investigating the magnetism of Ni from a momentum space perspective

For more than three decades, clear discrepancies have existed between spin densities in momentum space revealed by Magnetic Compton scattering experiments and theoretical calculations based on density functional theory (DFT). Here by making a wide comparison between different theoretical methods, including DFT, DFT combined with dynamical mean field theory, and Hedin's $GW$ approximation, we discover how the magnetic Compton profiles of Ni can be predicted remarkably well. We find that the essential ingredients missing in DFT are (i) local spin fluctuations and (ii) a non-local treatment of electron correlations.

cond-mat.str-el↗

Local electron correlation effects on the Fermiology of the weak itinerant ferromagnet ZrZn$_2$

The Fermi surface topology plays an important role in the macroscopic properties of metals. It can be particularly sensitive to electron correlation, which appears to be especially significant for the weak itinerant ferromagnet ZrZn$_{2}$. Here, we look at the differences in the predicted Fermi surface sheets of this metallic compound in its paramagnetic phase for both density functional theory (DFT) and the combination of DFT with dynamical mean field theory (DFT+DMFT). The theoretical spectral functions evaluated at the Fermi level were used along with calculations of the electron-positron momentum density (also known as the two-photon momenutm density) in $k$-space to provide insights into the origin of certain features of the Fermi surface topology. We compare this two photon momentum density to that extracted from the positron annihilation experimental data (Phys. Rev. Lett. 92, 107003 (2004)). The DFT+DMFT densities are in better agreement with the experiment than the DFT, particularly with regard to the flat bands around the $L$ and $W$ high symmetry points. The experimental neck around $L$, which relates to a van Hove singularity, is present in DFT+DMFT but not in the DFT. We find that these flat bands, and as such the Fermi surface topology, are sensitive to the many body electron correlation description, and show that the positron annihilation technique is able to probe this. This description is significant for the observed behavior such as the Lifshiftz transition around the quantum critical point.

cond-mat.str-el↗

$L$-hole Pockets of the Palladium Fermi Surface Revealed by Positron Annihilation Spectroscopy

Using the combined Density Functional and Dynamical Mean Field theory we study relativistic corrections to the Fermi surface of palladium. We find indeed that relativistic corrections create a small hole pockets at the $L$-symmetry points. Furthermore we show that the computed two dimensional Angular Correlation of Electron Positron Annihilation Radiation (the so called $2D$-ACAR) clearly demonstrates the existence of these $L$-hole pockets, which remains robust against electronic correlations. A $2D$-ACAR experiment should therefore provide the "smoking-gun" proof for the existence of the $L$-hole pockets in the palladium Fermi surface.

cond-mat.str-el↗

An investigation of the sensitivity of the Fermi surface to the treatment of exchange and correlation

The Group V and VI transition metals share a common Fermi surface feature of hole ellipsoids at the N point in the Brillouin zone. In clear contrast to the other Fermi surface sheets, which are purely of d character, these arise from a band that has a significant proportion of p character. By performing local density approximation (LDA), generalized gradient approximation (GGA), strongly constrained and appropriately normed (SCAN) meta-GGA, and GW approximation calculations, we find that the p character part of this band (and therefore the Fermi surface) is particularly sensitive to the exchange-correlation approximation. LDA and GGA calculations inadequately describe this feature, predicting N hole ellipsoid sizes that are consistently too large in comparison to various experimental measurements, whereas quasiparticle self-consistent GW calculations predict a size that is slightly too small (and non-self-consistent GW calculations that use an LDA starting point predict a size that is much too small). Overall, for the metals tested here, SCAN provides the most accurate Fermi surface predictions, mostly correcting the discrepancies between measurements and calculations that were observed when LDA calculations were used. However, none of the tested exchange-correlation approximations succeeds in simultaneously bringing all of the measurable properties of these metals into good experimental agreement, particularly where magnetism is concerned. The SCAN calculations predict antiferromagnetic moments for Cr that are 3 times larger than the experimental value (1.90 $μ_B$ compared to 0.62 $μ_B$).

cond-mat.str-el↗

Magnetic Compton profiles of Ni beyond the one-particle picture: numerically exact and perturbative solvers of dynamical mean-field theory

We calculated the magnetic Compton profiles (MCPs) of Ni using density functional theory supplemented by electronic correlations treated within dynamical mean-field theory (DMFT). We present comparisons between the theoretical and experimental MCPs. The theoretical MCPs were calculated using the KKR method with the perturbative spin-polarized T-matrix fluctuation exchange approximation DMFT solver, as well as with the full potential linear augmented planewave method with the numerically exact continuous-time quantum Monte Carlo DMFT solver. We show that the total magnetic moment decreases with the intra-atomic Coulomb repulsion $U$, which is also reflected in the corresponding MCPs. The total magnetic moment obtained in experimental measurements can be reproduced by intermediate values of $U$. The spectral function reveals that the minority X$_2$ Fermi surface pocket shrinks and gets shallower with respect to the density functional theory calculations.

cond-mat.str-el↗

Wavefunctions, electronic localization and bonding properties for correlated materials beyond the Kohn-Sham formalism

Many-body theories such as dynamical mean field theory (DMFT) have enabled the description of the electron exchange-correlation interactions that are missing in current density functional theory (DFT) calculations. However, there has been relatively little focus on the wavefunctions from these theories. We present the methodology of the newly developed Elk-TRIQS interface and how to calculate the DFT with DMFT (DFT+DMFT) wavefunctions, which can be used to calculate DFT+DMFT wavefunction dependent quantities. We illustrate this by calculating the electron localized function (ELF) in monolayer SrVO$_3$ and CaFe$_2$As$_2$, which provides a means of visualizing their chemical bonds. Monolayer SrVO$_3$ ELFs are sensitive to the charge redistribution between the DFT, one-shot DFT+DMFT and fully charge self-consistent DFT+DMFT calculations. In both tetragonal and collapsed tetragonal CaFe$_2$As$_2$ phases, the ELF changes weakly with correlation induced charge redistribution of the hybridized As-p and Fe-d states. Nonetheless, the interlayer As-As bond in the collapsed tetragonal structure is robust to the changes at and around the Fermi level.

cond-mat.str-el↗

Bulk and element specific magnetism of the medium and high entropy Cantor-Wu alloys

Magnetic Compton scattering, x-ray magnetic circular dichroism spectroscopy and bulk magnetometry measurements are performed on a set of medium (NiFeCo and NiFeCoCr) and high (NiFeCoCrPd and NiFeCoCrMn) entropy Cantor-Wu alloys. The bulk spin momentum densities determined by magnetic Compton scattering are remarkably isotropic, and this is a consequence of the smearing of the electronic structure by disorder scattering of the electron quasiparticles. Non-zero x-ray magnetic circular dichroism signals are observed for every element in every alloy indicating differences in the populations of the majority and minority spin states implying finite magnetic moments. When Cr is included in the solid solution, the Cr spin moment is unambiguously antiparallel to the total magnetic moment, while a vanishingly small magnetic moment is observed for Mn, despite calculations indicating a large moment. Some significant discrepancies are observed between the experimental bulk and surface magnetic moments. Despite the lack of quantitative agreement, the element specific surface magnetic moments seem to be qualitatively reasonable.

cond-mat.str-el↗

Determination of spin and orbital magnetization in the ferromagnetic superconductor UCoGe

The magnetism in the ferromagnetic superconductor UCoGe has been studied using a combination of magnetic Compton scattering, bulk magnetization, X-ray magnetic circular dichroism and electronic structure calculations, in order to determine the spin and orbital moments. The experimentally observed total spin moment, $M_s$, was found to be -0.24 $\pm$ 0.05~$μ_B$ at 5~T. By comparison with the total moment of 0.16 $\pm$ 0.01~$μ_B$, the orbital moment, $M_l$, was determined to be 0.40 $\pm$ 0.05~$μ_B$. The U and Co spin moments were determined to be antiparallel. We find that the U 5\textit{f} electrons carry a spin moment of U$_s \approx$ -0.30~$μ_B$ and that there is a Co spin moment of Co$_s \approx$ 0.06~$μ_B$ induced via hybridization. The ratio U$_l/$U$_s$, of $-1.3 \pm 0.3$, shows the U moment to be itinerant. In order to ensure an accurate description of the properties of 5\textit{f} systems, and to provide a critical test of the theoretical approaches, it is clearly necessary to obtain experimental data for both the spin and orbital moments, rather than just the total magnetic moment. This can be achieved simply by measuring the spin moment with magnetic Compton scattering and comparing this to the total moment from bulk magnetization.

cond-mat.str-el↗

Calculating electron momentum densities and Compton profiles using the linear tetrahedron method

A method for computing electron momentum densities and Compton profiles from ab initio calculations is presented. Reciprocal space is divided into optimally-shaped tetrahedra for interpolation, and the linear tetrahedron method is used to obtain the momentum density and its projections such as Compton profiles. Results are presented and evaluated against experimental data for Be, Cu, Ni, Fe3Pt, and YBa2Cu4O8, demonstrating the accuracy of our method in a wide variety of crystal structures.

cond-mat.mtrl-sci↗

Temperature-dependent electron-phonon coupling in La$_{2-x}$Sr$_x$CuO$_4$ probed by femtosecond X-ray diffraction

The strength of the electron-phonon coupling parameter and its evolution throughout a solid's phase diagram often determines phenomena such as superconductivity, charge- and spin-density waves. Its experimental determination relies on the ability to distinguish thermally activated phonons from those emitted by conduction band electrons, which can be achieved in an elegant way by ultrafast techniques. Separating the electronic from the out-of-equilibrium lattice subsystems, we probed their re-equilibration by monitoring the transient lattice temperature through femtosecond X-ray diffraction in La$_{2-x}$Sr$_x$CuO$_4$ single crystals with $x$=0.1 and 0.21. The temperature dependence of the electron-phonon coupling is obtained experimentally and shows similar trends to what is expected from the \textit{ab-initio} calculated shape of the electronic density-of-states near the Fermi energy. This study evidences the important role of band effects in the electron-lattice interaction in solids, in particular in superconductors.

cond-mat.supr-con↗

Electronic topological transition in LaSn$_3$ under pressure

The electronic structure, Fermi surface and elastic properties of the iso-structural and iso-electronic LaSn$_3$ and YSn$_3$ intermetallic compounds are studied under pressure within the framework of density functional theory including spin-orbit coupling. The LaSn$_3$ Fermi surface consists of two sheets, of which the second is very complex. Under pressure a third sheet appears around compression $V/V_0=0.94$, while a small topology change in the second sheet is seen at compression $V/V_0=0.90$. This may be in accordance with the anomalous behaviour in the superconducting transition temperature observed in LaSn$_3$, which has been suggested to reflect a Fermi surface topological transition, along with a non-monotonic pressure dependence of the density of states at the Fermi level. The same behavior is not observed in YSn$_3$, the Fermi surface of which already includes three sheets at ambient conditions, and the topology remains unchanged under pressure. The reason for the difference in behaviour between LaSn$_3$ and YSn$_3$ is the role of spin-orbit coupling and the hybridization of La - $4f$ states with the Sn - $p$ states in the vicinity of the Fermi level, which is well explained using the band structure calculation. The elastic constants and related mechanical properties are calculated at ambient as well as at elevated pressures. The elastic constants increase with pressure for both compounds and satisfy the conditions for mechanical stability under pressure.

cond-mat.mtrl-sci↗

Measurement of Magnetic Exchange in Ferromagnet-Superconductor La2/3Ca1/3MnO3/YBa2Cu3O7 Bilayers

The existence of coherent magnetic correlations in the normal phase of cuprate high-temperature superconductors has proven difficult to measure directly. Here we report on a study of ferromagnetic-superconductor bilayers of La2/3Ca1/3MnO3/YBa2Cu3O7 (LCMO/YBCO) with varying YBCO layer thicknesses. Using x-ray magnetic circular dichroism, we demonstrate that the ferromagnetic layer induces a Cu magnetic moment in the adjacent high-temperature superconductor. For thin samples, this moment exists at all temperatures below the Curie temperature of the LCMO layer. However, for a YBCO layer thicker than 12 unit cells, the Cu moment is suppressed for temperatures above the superconducting transition, suggesting this to be a direct measurement of magnetic coherence in the normal state of a superconducting oxide.

cond-mat.str-el↗

Evidence for a Peierls phase-transition in a three-dimensional multiple charge-density waves solid

The effect of dimensionality on materials properties has become strikingly evident with the recent discovery of graphene. Charge ordering phenomena can be induced in one dimension by periodic distortions of a material's crystal structure, termed Peierls ordering transition. Charge-density waves can also be induced in solids by strong Coulomb repulsion between carriers, and at the extreme limit, Wigner predicted that crystallization itself can be induced in an electrons gas in free space close to the absolute zero of temperature. Similar phenomena are observed also in higher dimensions, but the microscopic description of the corresponding phase transition is often controversial, and remains an open field of research for fundamental physics. Here, we photoinduce the melting of the charge ordering in a complex three-dimensional solid and monitor the consequent charge redistribution by probing the optical response over a broad spectral range with ultrashort laser pulses. Although the photoinduced electronic temperature far exceeds the critical value, the charge-density wave is preserved until the lattice is sufficiently distorted to induce the phase transition. Combining this result with it ab initio} electronic structure calculations, we identified the Peierls origin of multiple charge-density waves in a three-dimensional system for the first time.

cond-mat.str-el↗

Maximum entropy deconvolution of resonant inelastic x-ray scattering spectra

Resonant inelastic x-ray scattering (RIXS) has become a powerful tool in the study of the electronic structure of condensed matter. Although the linewidths of many RIXS features are narrow, the experimental broadening can often hamper the identification of spectral features. Here, we show that the Maximum Entropy technique can successfully be applied in the deconvolution of RIXS spectra, improving the interpretation of the loss features without a severe increase in the noise ratio.

cond-mat.str-el↗

Experimental determination of the state-dependent enhancement of the electron-positron momentum density in solids

The state-dependence of the enhancement of the electron-positron momentum density is investigated for some transition and simple metals (Cr, V, Ag and Al). Quantitative comparison with linearized muffin-tin orbital calculations of the corresponding quantity in the first Brillouin zone is shown to yield a measurement of the enhancement of the s, p and d states, independent of any parameterizations in terms of the electron density local to the positron. An empirical correction that can be applied to a first-principles state-dependent model is proposed that reproduces the measured state-dependence very well, yielding a general, predictive model for the enhancement of the momentum distribution of positron annihilation measurements, including those of angular correlation and coincidence Doppler broadening techniques.

cond-mat.str-el↗

Fermi surface of an important nano-sized metastable phase: Al$_3$Li

Nanoscale particles embedded in a metallic matrix are of considerable interest as a route towards identifying and tailoring material properties. We present a detailed investigation of the electronic structure, and in particular the Fermi surface, of a nanoscale phase ($L1_2$ Al$_3$Li) that has so far been inaccessible with conventional techniques, despite playing a key role in determining the favorable material properties of the alloy (Al\nobreakdash-9 at. %\nobreakdash-Li). The ordered precipitates only form within the stabilizing Al matrix and do not exist in the bulk; here, we take advantage of the strong positron affinity of Li to directly probe the Fermi surface of Al$_3$Li. Through comparison with band structure calculations, we demonstrate that the positron uniquely probes these precipitates, and present a 'tuned' Fermi surface for this elusive phase.

cond-mat.mtrl-sci↗

Bulk electronic structure of optimally doped Ba(Fe$_{1-x}$Co$_{x}$)$_2$As$_2$

We report high-resolution, bulk Compton scattering measurements unveiling the Fermi surface of an optimally-doped iron-arsenide superconductor, Ba(Fe$_{0.93}$Co$_{0.07}$)$_2$As$_2$. Our measurements are in agreement with first-principles calculations of the electronic structure, revealing both the $X$-centered electron pockets and the $Γ$-centered hole pockets. Moreover, our data are consistent with the strong three-dimensionality of one of these sheets that has been predicted by electronic structure calculations at the local-density-approximation-minimum As position. Complementary calculations of the noninteracting susceptibility, $χ_0({\bf q}, ω)$, suggest that the broad peak that develops due to interband Fermi-surface nesting, and which has motivated several theories of superconductivity in this class of material, survives the measured three dimensionality of the Fermi surface in this family.

cond-mat.str-el↗