SearcharxivSearch

arXiv subjects

B. Barbiellini

Publications and source records attributed to B. Barbiellini.

At least 19 recordsLinked to original sources

Recycling failed photoelectrons via tertiary photoemission

A key insight of Einstein's theory of the photoelectric effect is that a minimum energy is required for photoexcited electrons to escape from a material. For the past century it has been assumed that photoexcited electrons of lower energies make no contribution to the photoemission spectrum. Here we demonstrate the conceptual possibility that the energy of these 'failed' photoelectrons-primary or secondary-can be partially recycled to generate new 'tertiary' electrons of energy sufficient to escape. Such a 'recycling' step goes beyond the traditional three steps of the photoemission process (excitation, transport, and escape), and, as we illustrate, it can be realized through a novel Auger mechanism that involves three distinct minority electronic states in the material. We develop a phenomenological three-band model to treat this mechanism within a revised four-step framework for photoemission, which contains robust features of linewidth narrowing and population inversion under strong excitation, reminiscent of the lasing phenomena. We show that the conditions for this recycling mechanism are likely satisfied in many quantum materials with multiple flat bands properly located away from the Fermi level, and elaborate on the representative case of SrTiO3 among other promising candidates. We further discuss how this mechanism can explain the recent observation of anomalous intense coherent photoemission from a SrTiO3 surface, and predict its manifestations in related experiments, including the 'forbidden' case of photoemission with photon energies lower than the work function. Our study calls for paradigm shifts across a range of fundamental and applied research fields, especially in the areas of photoemission, photocathodes, and flat-band materials.

cond-mat.mtrl-sci

Prediction of a Heusler alloy with switchable metal-to-half-metal behavior

We propose a ferromagnetic Heusler alloy that can switch between a metal and a half-metal. Thiseffect can provide tunable spintronics properties. Using the density functional theory (DFT) withreliable implementations of the electron correlation effects, we find Mn2ScSi total energy curvesconsisting of distinct branches with a very small energy difference. The phase at low lattice crystalvolume is a low magnetic half-metallic state while the phase at high lattice crystal volume is a highmagnetic metallic state. We suggest that the transition between half-metallic and metallic statescan be triggered by a triaxial contraction/expansion of the crystal lattice or by an external magneticfield if we assume that the lattice is cubic and remains cubic under expansion/contraction. However,the phase at high volume can also undergo an austenite-martensite phase transition because of thepresence of Jahn-Teller active3delectrons on the Mn atoms.

cond-mat.mtrl-sci

Electronic structure beyond the generalized gradient approximation for Ni$_2$MnGa

The stability of the nonmodulated martensitic phase, the austenitic Fermi surface and the phonon dispersion relations for ferromagnetic Ni$_2$MnGa are studied using density functional theory. Exchange-correlation effects are considered with various degrees of precision, starting from the simplest local spin density approximation (LSDA), then adding corrections within the generalized gradient approximation (GGA) and finally, including the meta-GGA corrections within the strongly constrained and appropriately normed (SCAN). We discuss a simple procedure to reduce a possible overestimation of magnetization and underestimation of nesting vector in SCAN by parametrically decreasing self-interaction corrections.

cond-mat.mtrl-sci

Ab initio description of the Bi$_2$Sr$_2$CaCu$_2$O$_{8+δ}$ electronic structure

Bi-based cuprate superconductors are important materials for both fundamental research and applications. As in other cuprates, the superconducting phase in the Bi compounds lies close to an antiferromagnetic phase. Our density functional theory calculations based on the strongly-constrained-and-appropriately-normed (SCAN) exchange correlation functional in Bi$_2$Sr$_2$CaCu$_2$O$_{8+δ}$ reveal the persistence of magnetic moments on the copper ions for oxygen concentrations ranging from the pristine phase to the optimally hole-doped compound. We also find the existence of ferrimagnetic solutions in the heavily doped compounds, which are expected to suppress superconductivity.

cond-mat.supr-con

Examining the surface phase diagram of IrTe$_2$ with photoemission

In the transition metal dichalcogenide IrTe$_2$, low-temperature charge-ordered phase transitions involving Ir dimers lead to the occurrence of stripe phases of different periodicities, and nearly degenerate energies. Bulk-sensitive measurements have shown that, upon cooling, IrTe$_2$ undergoes two such first-order transitions to $(5\times1\times5)$ and $(8\times1\times8)$ reconstructed phases at $T_{c_1}\sim 280$~K and $T_{c_2}\sim 180$~K, respectively. Here, using surface sensitive probes of the electronic structure of IrTe$_2$, we reveal the first-order phase transition at $T_{c_3}=165$~K to the $(6\times1)$ stripes phase, previously proposed to be the surface ground state. This is achieved by combining x-ray photoemission spectroscopy and angle-resolved photoemission spectroscopy, which give access to the evolution of stripe domains and a particular surface state, the energy of which is dependent on the Ir dimer length. By performing measurements over a full thermal cycle, we also report the complete hysteresis of all these phases.

cond-mat.str-el

Correlation effects on ground-state properties of ternary Heusler alloys: first-principles study

The strongly constrained and appropriately normed (SCAN) semi-local functional for exchange-correlation is deployed to study the ground-state properties of ternary Heusler alloys transforming martensitically. The calculations are performed for ferromagnetic, ferrimagnetic, and antiferromagnetic phases. Comparisons between SCAN and generalized gradient approximation (GGA) are discussed. We find that SCAN yields smaller lattice parameters and higher magnetic moments compared to the GGA corresponding values for both austenite and martensite phases. Furthermore, in the case of ferromagnetic and non-magnetic Heusler compounds, GGA and SCAN display similar trends in the total energy as a function of lattice constant and tetragonal ratio. However, for some ferrimagnetic Mn-rich Heusler compounds, different magnetic ground states are found within GGA and SCAN.

cond-mat.mtrl-sci

Gate-tunable magnetism of C adatoms on graphene

We have performed density functional theory calculations of graphene decorated with carbon adatoms, which bind at the bridge site of a C--C bond. Earlier studies have shown that the C adatoms have magnetic moments and have suggested the possibility of ferromagnetism with high Curie temperature. Here we propose to use a gate voltage to fine tune the magnetic moments from zero to 1$μ_B$ while changing the magnetic coupling from antiferromagnetism to ferromagnetism and again to antiferromagnetism. These results are rationalized within the Stoner and RKKY models. When the SCAN meta-GGA correction is used, the magnetic moments for zero gate voltage are reduced and the Stoner band ferromagnetism is slightly weakened in the ferromagnetic region.

cond-mat.mes-hall

Characterization of Thin Film Materials using SCAN meta-GGA, an Accurate Nonempirical Density Functional

We discuss self-consistently obtained ground-state electronic properties of monolayers of graphene and a number of beyond graphene compounds, including films of transition-metal dichalcogenides (TMDs), using the recently proposed strongly constrained and appropriately normed (SCAN) meta-generalized gradient approximation (meta-GGA) to the density functional theory. The SCAN meta-GGA results are compared with those based on the local density approximation (LDA) as well as the generalized gradient approximation (GGA). As expected, the GGA yields expanded lattices and softened bonds in relation to the LDA, but the SCAN meta-GGA systematically improves the agreement with experiment. Our study suggests the efficacy of the SCAN functional for accurate modeling of electronic structures of layered materials in high-throughput calculations more generally.

cond-mat.mtrl-sci

Direct observation of electron emission as a result of a VVV Auger transition in the valence band of Graphene

We report the first direct observation of electron emission into the vacuum as a result of a VVV Auger transition resulting from the relaxation of a deep hole in the valence band. A beam of low energy (<1.25eV) positrons was used to deposit positrons onto the surface of samples consisting of single layer graphene, multi-layer graphene and graphite. The distribution of electrons emitted from the samples as a result of the annihilation of the positron showed peak extending up to ~12 eV with a maximum at ~4eV. The observed peak was ~17 times larger than the previously observed annihilation induced C KVV peak. An analysis based upon a density functional theory calculation of the positron annihilation rates indicates that the width and intensity of the peak is consistent with electron emission resulting from VVV Auger transition excited by the annihilation of valence band electrons. Good agreement was found between the data from the single layer graphene on Cu surface with a theoretical line shape found from a self-folding of the density of states for a free standing graphene layer. The agreement between the theoretical and measured intensities for the KVV and VVV transitions indicates that the branching ratio for holes to decay via an Auger transition is nearly the same in both cases (i.e. close to 100%). Our results suggest the possibility of using annihilation induced VVV Auger spectroscopy to study the properties of the local density of states and the hole decay processes in materials in which the valence band width exceeds the work function.

cond-mat.mes-hall

Identifying a descriptor for d-orbital delocalization in cathodes of Li batteries based on x-ray Compton scattering

We discuss how x-ray Compton scattering spectra can be used for investigating the evolution of electronic states in cathode materials of Li batteries under the lithiation/delithiation process. In particular, our analysis of the Compton spectra taken from polycrystalline LixCoO2 samples shows that the spectra are dominated by the contribution of the O-2p redox orbital. We identify a distinct signature of d-orbital delocalization, which is tied directly to the conductivity of the material, providing a descriptor based on Compton spectra for monitoring the lithiation range with improved conductivity and kinetics for electrochemical operation. Our study demonstrates that Compton scattering spectroscopy can provide a window for probing complex electronic mechanisms underlying the charging and discharging processes in Li-battery materials.

cond-mat.mtrl-sci

3D Dirac cone carrier dynamics in Na3Bi and Cd3As2

Optical measurements and band structure calculations are reported on 3D Dirac materials. The electronic properties associated with the Dirac cone are identified in the reflectivity spectra of Cd$_3$As$_2$ and Na$_3$Bi single crystals. In Na$_3$Bi, the plasma edge is found to be strongly temperature dependent due to thermally excited free carriers in the Dirac cone. The thermal behavior provides an estimate of the Fermi level $E_F=25$ meV and the z-axis Fermi velocity $v_z = 0.3 \text{ eV} Å$ associated with the heavy bismuth Dirac band. At high energies above the $Γ$-point Lifshitz gap energy, a frequency and temperature independent $ε_2$ indicative of Dirac cone interband transitions translates into an ab-plane Fermi velocity of $3 \text{ eV} Å$. The observed number of IR phonons rules out the $\text{P}6_3\text{/mmc}$ space group symmetry but is consistent with the $\text{P}\bar{3}\text{c}1$ candidate symmetry. A plasmaron excitation is discovered near the plasmon energy that persists over a broad range of temperature. The optical signature of the large joint density of states arising from saddle points at $Γ$ is strongly suppressed in Na$_3$Bi consistent with band structure calculations that show the dipole transition matrix elements to be weak due to the very small s-orbital character of the Dirac bands. In Cd$_3$As$_2$, a distinctive peak in reflectivity due to the logarithmic divergence in $ε_1$ expected at the onset of Dirac cone interband transitions is identified. The center frequency of the peak shifts with temperature quantitatively consistent with a linear dispersion and a carrier density of $n=1.3\times10^{17}\text{ cm}^{-3}$. The peak width gives a measure of the Fermi velocity anisotropy of $10\%$, indicating a nearly spherical Fermi surface. The lineshape gives an upper bound estimate of 7 meV for the potential fluctuation energy scale.

cond-mat.str-el

Self-consistent scheme for optical response of large hybrid networks of semiconductor quantum dots and plasmonic metal nanoparticles

We discuss a self-consistent scheme for treating the optical response of large, hybrid networks of semiconducting quantum dots (SQDs) and plasmonic metallic nanoparticles (MNPs). Our method is efficient and scalable and becomes exact in the limiting case of weakly interacting SQDs. The self-consistent equations obtained for the steady state are analogous to the von Neumann equations of motion for the density matrix of a SQD placed in an effective electric field computed within the discrete dipole approximation. Illustrative applications of the theory to square and honeycomb SQD, MNP, and hybrid SDQ-MNP lattices as well as SQD-MNP dimers are presented. Our results demonstrate that hybrid SQD-MNP lattices can provide flexible platforms for light manipulation with tunable resonant characteristics.

cond-mat.mes-hall

Non-destructive measurement of in-operando lithium concentration in batteries via x-ray Compton scattering

Non-destructive determination of lithium distribution in a working battery is key for addressing both efficiency and safety issues. Although various techniques have been developed to map the lithium distribution in electrodes, these methods are mostly applicable to test cells. Here we propose the use of high-energy x-ray Compton scattering spectroscopy to measure the local lithium concentration in closed electrochemical cells. A combination of experimental measurements and parallel first-principles computations is used to show that the shape parameter S of the Compton profile is linearly proportional to lithium concentration and thus provides a viable descriptor for this important quantity. The merits and applicability of our method are demonstrated with illustrative examples of LixMn2O4 cathodes and a working commercial lithium coin battery CR2032.

cond-mat.mtrl-sci

Explaining the x-ray nonlinear susceptibility of diamond and silicon near absorption edges

We report the observation and the theoretical explanation of the parametric down-conversion nonlinear susceptibility at the $K$-absorption edge of diamond and at the $L_{23}$-absorption edge of a silicon crystal. Using arguments similar to those invoked to successfully predict resonant inelastic x-ray spectra, we derive an expression for the renormalization term of the non-linear susceptibility at the x-ray edges, which can be evaluated by using first-principles calculations of the atomic scattering factor $f_1$. Our model is shown to reproduce the observed enhancement of the parametric down-conversion at the diamond $K$ and the Si $L_{23}$ edges rather than the suppression previously claimed.

cond-mat.mtrl-sci

Visualizing the mixed bonding properties of liquid boron with high resolution Compton scattering

Bonding characteristics of liquid boron at 2500K are studied by using high resolution Compton scattering. An excellent agreement is found between the measurements and the corresponding Car-Parinello molecular dynamics simulations. Covalent bond pairs are clearly shown to dominate in liquid boron along with the coexistence of diffuse pairs. Our study reveals the complex bonding pattern of liquid boron, and gives insight into the unusual properties of this high temperature liquid.

cond-mat.mtrl-sci

Extracting the Redox Orbitals in Li Battery Materials with High-Resolution X-Ray Compton Scattering Spectroscopy

We present an incisive spectroscopic technique for directly probing redox orbitals based on bulk electron momentum density measurements via high-resolution x-ray Compton scattering. Application of our method to spinel LixMn2O4, a lithium ion battery cathode material, is discussed. The orbital involved in the lithium insertion and extraction process is shown to mainly be the oxygen 2p orbital. Moreover, the manganese 3d states are shown to experience spatial delocalization involving 0.16 electrons per Mn site during the battery operation. Our analysis provides a clear understanding of the fundamental redox process involved in the working of a lithium ion battery.

cond-mat.mtrl-sci

A Minimal tight-binding model for ferromagnetic canted bilayer manganites

Half-metallicity in materials has been a subject of extensive research due to its potential for applications in spintronics. Ferromagnetic manganites have been seen as a good candidate, and aside from a small minority-spin pocket observed in La$_{2-2x}$Sr$_{1+2x}$Mn$_{2}$O$_{7}$ $(x=0.38)$, transport measurements show that ferromagnetic manganites essentially behave like half metals. Here we develop robust tight-binding models to describe the electronic band structure of the majority as well as minority spin states of ferromagnetic, spin-canted antiferromagnetic, and fully antiferromagnetic bilayer manganites. Both the bilayer coupling between the MnO$_2$ planes and the mixing of the $|x^2 - y^2>$ and $|3z^2 - r^2>$ Mn 3d orbitals play an important role in the subtle behavior of the bilayer splitting. Effects of $k_z$ dispersion are included.

cond-mat.str-el

Gradient correction scheme for bulk and defect positron states in materials: New developments

As local density approximation positron calculations systematically underestimate positron lifetimes when they are compared with their experimental counterparts, the generalized gradient approximation (GGA) for positrons was introduced in the 1990s, in analogy with the GGA for electrons. New developments in the GGA for positrons are summarized and presented here and it is also discussed how they affect and possibly improve calculated positron lifetimes. In particular, these new GGA approaches are based on the recent perturbed hypernetted-chain and quantum Monte Carlo results.

cond-mat.mtrl-sci