Local Electronic Density Of States Research Articles

Chirality and Local Electron Density of States in a Two-Dimensional Molecular Crystal Self-Assembled by Prochiral Radical Molecules.

Creating and unveiling chiral systems is important to the development of new materials and devices. In this study, after depositing prochiral radical molecule 3-carbamoyl-2,2,5,5-tetramethyl pyrroline-1-oxyl (CTPO) on a Au(111) substrate, 2D molecular crystals with two chiralities of CTPO molecules have been discovered. A single CTPO molecule is an achiral molecule in three-dimensional space, and it can form chiral configurations after adsorbing on the substrate. The chiralities of 2D molecular crystals originate from the chiral properties of adsorbed CTPO molecules and their assembling. Molecules with different chiralities are connected with molecular recognition through hydrogen bond interactions. Through density functional theory simulations, the hydrogen bond networks and molecular structures of this system were explored. To gain a further understanding of this system, the electronic property of CTPO/Au(111) was studied with a local density of states (LDOS) characterization. A peculiar LDOS distribution related to the vibrational excitation of the molecules was mapped at the submolecular scale. These results are useful for understanding the nature of chirality formation, 2D molecular crystal construction, and radical molecule applications.

Features of hole transport and density of localized states in CuCr1-xMgxO2 and CuCr1–yMgyO2/(MgCr2O4)x–y polycrystalline ceramics

Magnesium doped polycrystalline ceramic samples of cooper chromite (I) with 0.6-4.0 at % Mg content have been synthesized. Phase composition of ceramics has been investigated by X-ray diffraction. Temperature dependencies of electrical resistivity and Seebeck coefficient have been measured by four probe method and analyzed in frame of variable range hopping conductivity. The density of localized electronic states and characteristic energy of its variation near Fermi energy have been estimated. It was obtained that the density of localized states at Fermi energy increases with an increase of Mg content, while characteristic energy of variation of localized state density near Fermi energy decreases. Obtained results show that relatively large values of Seebeck coefficient in Mg doped copper chromite (I) can be understood within variable range hopping transport of holes with rapidly increasing density toward valence band maximum.

Vliyanie primesey na adsorbtsiyu kisloroda na poverkhnosti Ti5Si3(0001)

The influence of simple and transition metal impurities, as well as interstitial impurities (B, C, and N), on the oxygen adsorption on the Ti5Si3 titanium silicide surface has been studied using the of projector augmented wave method within the electron density functional theory. It has been shown that titanium-substituting impurities belonging to the latter halves of the 3d–5d periods cause most significant changes in the adsorption energy. In addition, simple metals and interstitial impurities reduce the oxygen–surface interaction. By analyzing local electron densities of states, charge density difference distribution, charge transfer, and the overlap population of oxygen bonds to nearest-neighbor atoms, we have revealed special aspects of impurity influence on chemical bonding between the titanium silicide surface and oxygen. Factors responsible for an increase/decrease in the adsorption energy of oxygen on the doped surface are discussed. A correlation between the change in adsorption energy and the electronegativity of impurities has been found.

Modeling of Gold Adsorption by the Surface of Defect Graphene

The results of the theoretical investigation of the local structural changes and adsorption characteristics of the graphene (GP) surface in the presence of a vacancy + Auads adatom complex are presented. Based on the density functional theory (DFT), the adsorption properties of Auads at the surface of GP supercells containing 50 carbon atoms with vacancies ({text{GP}}leftlangle {{text{A}}{{{text{u}}}_{{{text{ads}}}}}} rightrangle ,{text{ G}}{{{text{P}}}_{{text{V}}}}leftlangle {{text{A}}{{{text{u}}}_{{{text{ads}}}}}} rightrangle ) are calculated. The most stable configuration of {text{G}}{{{text{P}}}_{{text{V}}}}leftlangle {{text{A}}{{{text{u}}}_{{{text{ads}}}}}} rightrangle supercells with a vacancy + Auads adatom complex is determined. The effect that an Auads adatom has on the band structure and local magnetic moment in {text{G}}{{{text{P}}}_{{text{V}}}}leftlangle {{text{A}}{{{text{u}}}_{{{text{ads}}}}}} rightrangle is calculated. The data are analyzed based on the equilibrium atomic configuration {text{G}}{{{text{P}}}_{{text{V}}}}leftlangle {{text{A}}{{{text{u}}}_{{{text{ads}}}}}} rightrangle , local density of electronic states, and spin polarization. The calculations are made using the exchange-correlation functional in a local electron-spin density approximation (LSDA).

Nanoscale coherent phonon spectroscopy.

Coherent phonon spectroscopy can provide microscopic insight into ultrafast lattice dynamics and its coupling to other degrees of freedom under nonequilibrium conditions. Ultrafast optical spectroscopy is a well-established method to study coherent phonons, but the diffraction limit has hampered observing their local dynamics directly. Here, we demonstrate nanoscale coherent phonon spectroscopy using ultrafast laser–induced scanning tunneling microscopy in a plasmonic junction. Coherent phonons are locally excited in ultrathin zinc oxide films by the tightly confined plasmonic field and are probed via the photoinduced tunneling current through an electronic resonance of the zinc oxide film. Concurrently performed tip-enhanced Raman spectroscopy allows us to identify the involved phonon modes. In contrast to the Raman spectra, the phonon dynamics observed in coherent phonon spectroscopy exhibit strong nanoscale spatial variations that are correlated with the distribution of the electronic local density of states resolved by scanning tunneling spectroscopy.

Kinetic models of quantum size effect-directed nanocluster self-assembly in atomic corrals

Two simple kinetic models of quantum size effect-directed nanocluster self-assembly in circular atomic corrals are discussed. The models correspond to an adsorption (either a physisorption or a chemisorption) and an adsorption-diffusion regimes that are typical at low and high temperatures, respectively. Small magnitudes of a variation of the electronic local density of states is shown to be the prime factor that impedes self-assembly in the latter regime.

Absence of hexagonal-to-square lattice transition in LiFeAs vortex matter

We investigated magnetic vortices in two stoichiometric LiFeAs samples by means of scanning tunneling microscopy and spectroscopy. The vortices were revealed by measuring the local electronic density of states (LDOS) at zero bias conductance of samples in magnetic fields between 0.5 and 12 T. From single vortex spectroscopy we extract the Ginzburg-Landau coherence length of both samples as $4.4\pm0.5$ nm and $4.1\pm0.5$ nm, in accordance with previous findings. However, in contrast to previous reports, our study reveals that the reported hexagonal to square-like vortex lattice transition is absent up to 12 T both in field-cooling and zero-field-cooling processes. Remarkably, a highly ordered zero field cooled hexagonal vortex lattice is observed up to 8 T. We argue that several factors are likely to determine the structure of the vortex lattice in LiFeAs such as (i) details of the cooling procedure (ii) sample stoichiometry that alters the formation of nematic fluctuations, (iii) details of the order parameter and (iv) magnetoelastic coupling.

Al27 NMR local study of the Al0.5TiZrPdCuNi alloy in high-entropy alloy and metallic glass forms

We report a $^{27}\mathrm{Al}$ nuclear magnetic resonance (NMR) local spectroscopic study of the NMR lineshape and Knight shift of a six-component ${\mathrm{Al}}_{0.5}\mathrm{TiZrPdCuNi}$ metallic alloy that can be prepared either as a crystalline high-entropy alloy (HEA) or as an amorphous metallic glass (MG) at the same chemical composition. For both structural modifications of the material (HEA and MG), we have determined the distribution of electric-field-gradient (EFG) tensors and the local electronic density of states (DOS) $g({\ensuremath{\varepsilon}}_{\mathrm{F}})$ at the Fermi level at the position of $^{27}\mathrm{Al}$ nuclei. A theoretical $I=\frac{5}{2}$ quadrupole-perturbed NMR spectrum, pertinent to both cubic HEAs and amorphous MGs, has been derived using the Gaussian isotropic model of the EFG tensor distribution, and excellent fits of the experimental spectra were obtained. The EFG distribution function of the MG state is about twice broader than that of the HEA state, reflecting the existence of a (distorted) crystal lattice in the latter and its absence in the former. The ${T}^{2}$ dependence of the Knight shift indicates that the DOS is changing rapidly with energy within the Fermi level region for both structural modifications. The local DOS at the $^{27}\mathrm{Al}$ sites of the HEA sample is $\ensuremath{\sim}10%$ larger than that of the MG state, indicating comparable degrees of disorder.

Converting electrons into emergent fermions at a superconductor–Kitaev spin liquid interface

We study an interface between a Kitaev spin liquid (KSL) in the chiral phase and a non-chiral superconductor. When the coupling across the interface is sufficiently strong, the interface undergoes a transition into a phase characterized by a condensation of a bound state of a Bogoliubov quasiparticle in the superconductor and an emergent fermionic excitation in the spin liquid. In the condensed phase, electrons in the superconductor can coherently convert into emergent fermions in the spin liquid and vice versa. As a result, the chiral Majorana edge mode of the spin liquid becomes visible in the electronic local density of states at the interface, which can be measured in scanning tunneling spectroscopy experiments. We demonstrate the existence of this phase transition, and the non-local order parameter that characterizes it, using density matrix renormalization group simulations of a KSL strip coupled at its edge to a superconductor. An analogous phase transition can occur in a simpler system composed of a one-dimensional spin chain with a spin-flip $\mathbb{Z}_2$ symmetry coupled to a superconductor.

Revealing quantum effects in highly conductive \u03b4-layer systems

Thin, high-density layers of dopants in semiconductors, known as δ-layer systems, have recently attracted attention as a platform for exploration of the future quantum and classical computing when patterned in plane with atomic precision. However, there are many aspects of the conductive properties of these systems that are still unknown. Here we present an open-system quantum transport treatment to investigate the local density of electron states and the conductive properties of the δ-layer systems. A successful application of this treatment to phosphorous δ-layer in silicon both explains the origin of recently-observed shallow sub-bands and reproduces the sheet resistance values measured by different experimental groups. Further analysis reveals two main quantum-mechanical effects: 1) the existence of spatially distinct layers of free electrons with different average energies; 2) significant dependence of sheet resistance on the δ-layer thickness for a fixed sheet charge density.

Effects of doping substitutions on the thermal conductivity of half-Heusler compounds

The promise posed by half-Heusler compounds as thermoelectric materials depends on their thermal conductivity, which is strongly affected by doping. Here we elucidate the effect of $p$ dopants on the lattice thermal conductivity (${\ensuremath{\kappa}}_{\text{ph}}$) of seven selected half-Heusler compounds and for twelve different substitutional defects. We unveil a strong reduction in ${\ensuremath{\kappa}}_{\text{ph}}$ even for low concentrations of transition-metal substitutional atoms. Furthermore, we quantify the strength of the bond perturbation induced by substitutional impurities and interpret it in terms of the changes in the local electronic density of states. In several cases we find a significant destructive interference between the mass difference and bond perturbations which reduces the phonon scattering rates below the value expected if the two effects were treated independently. We compare our first-principles calculations with the available experimental measurements on the thermal conductivity of (${\mathrm{Zr},\mathrm{Hf})}_{\text{Nb}}$-doped NbFeSb and ${\mathrm{Sn}}_{\text{Sb}}$-doped ZrCoSb. For the latter, including the effect of independent Co vacancies and interstitials yields an almost perfect agreement with experiment.

Holey Graphene: Topological Control of Electronic Properties and Electric Conductivity

This paper studies holey graphene with various neck widths (the smallest distance between two neighbor holes). For the considered structures, the energy gap, the Fermi level, the density of electronic states, and the distribution of the local density of electronic states (LDOS) were found. The electroconductive properties of holey graphene with round holes were calculated depending on the neck width. It was found that, depending on the neck width, holey graphene demonstrated a semiconductor type of conductivity with an energy gap varying in the range of 0.01–0.37 eV. It was also shown that by changing the neck width, it is possible to control the electrical conductivity of holey graphene. The anisotropy of holey graphene electrical conductivity was observed depending on the direction of the current transfer.

Quantum transport properties of gas molecules adsorbed on Fe doped armchair graphene nanoribbons: A first principle study

Graphene, when doped with transition metals, is considered, both experimentally and theoretically, as a good candidate for the detection of gas molecules as CO, CO2, NO or NO2. This opens new perspectives for gas sensor set-ups considering that devices based on 2 dimensional graphene are more sensitive to detect molecules than solid-state gas sensors. The state of the arts on gas adsorption on Fe doped armchair graphene nanoribbons (Fe-AGNR) is still in its starting phase and thorough investigations of the mechanism of the adsorption on graphene need to be done. In the present work, the electronic and transport properties of molecules adsorbed on Fe-AGNR are scrutinized using ab-initio calculations. We observe that the adsorption of gas molecules on Fe-AGNR changes significantly the electronic properties of both the valence and the conduction band. Besides, The adsorbed molecules change the local electron density of states of the graphene nanoribbons, modifying thus the conductivity, being one of the main output quantity of the gas sensors. We also observe that the adsorbed molecules induce specific impurity bands which play a role in the transport properties. Finally, considering the observed variations of electrical conductance induced by the molecules, we propose several strategies to set-up gas sensors for CO, CO2, NO and NO2 molecules. These strategies are either based on the measurement of the conductance in the valence or the conduction band (using either p or n-doped Fe-AGNR) or to the spin polarization induced by the NO and NO2 molecules.

Unveiling Odd-Frequency Pairing around a Magnetic Impurity in a Superconductor.

We study the unconventional superconducting correlations caused by a single isolated magnetic impurity in a conventional s-wave superconductor. Because of the local breaking of time-reversal symmetry, the impurity induces unconventional superconductivity, which is even in both space and spin variables but odd under time inversion. We derive an exact proportionality relation between the even-frequency component of the local electron density of states and the imaginary part of the odd-frequency local pairing function. By applying this relation to scanning tunneling microscopy spectra taken on top of magnetic impurities immersed in a Pb/Si(111) monolayer, we show experimental evidence of the occurrence of the odd-frequency pairing in these systems and explicitly extract its superconducting function from the data.

Quantum Transport in a Silicon Nanowire FET Transistor: Hot Electrons and Local Power Dissipation.

A review and perspective is presented of the classical, semi-classical and fully quantum routes to the simulation of electro-thermal phenomena in ultra-scaled silicon nanowire field-effect transistors. It is shown that the physics of ultra-scaled devices requires at least a coupled electron quantum transport semi-classical heat equation model outlined here. The importance of the local density of states (LDOS) is discussed from classical to fully quantum versions. It is shown that the minimal quantum approach requires self-consistency with the Poisson equation and that the electronic LDOS must be determined within at least the self-consistent Born approximation. To bring in this description and to provide the energy resolved local carrier distributions it is necessary to adopt the non-equilibrium Green function (NEGF) formalism, briefly surveyed here. The NEGF approach describes quantum coherent and dissipative transport, Pauli exclusion and non-equilibrium conditions inside the device. There are two extremes of NEGF used in the community. The most fundamental is based on coupled equations for the Green functions electrons and phonons that are computed at the atomically resolved level within the nanowire channel and into the surrounding device structure using a tight binding Hamiltonian. It has the advantage of treating both the non-equilibrium heat flow within the electron and phonon systems even when the phonon energy distributions are not described by a temperature model. The disadvantage is the grand challenge level of computational complexity. The second approach, that we focus on here, is more useful for fast multiple simulations of devices important for TCAD (Technology Computer Aided Design). It retains the fundamental quantum transport model for the electrons but subsumes the description of the energy distribution of the local phonon sub-system statistics into a semi-classical Fourier heat equation that is sourced by the local heat dissipation from the electron system. It is shown that this self-consistent approach retains the salient features of the full-scale approach. For focus, we outline our electro-thermal simulations for a typical narrow Si nanowire gate all-around field-effect transistor. The self-consistent Born approximation is used to describe electron-phonon scattering as the source of heat dissipation to the lattice. We calculated the effect of the device self-heating on the current voltage characteristics. Our fast and simpler methodology closely reproduces the results of a more fundamental compute-intensive calculations in which the phonon system is treated on the same footing as the electron system. We computed the local power dissipation and “local lattice temperature” profiles. We compared the self-heating using hot electron heating and the Joule heating, i.e., assuming the electron system was in local equilibrium with the potential. Our simulations show that at low bias the source region of the device has a tendency to cool down for the case of the hot electron heating but not for the case of Joule heating. Our methodology opens the possibility of studying thermoelectricity at nano-scales in an accurate and computationally efficient way. At nano-scales, coherence and hot electrons play a major role. It was found that the overall behaviour of the electron system is dominated by the local density of states and the scattering rate. Electrons leaving the simulated drain region were found to be far from equilibrium.

Band topology, Hubbard model, Heisenberg model, and Dzyaloshinskii-Moriya interaction in twisted bilayer WSe2

We present a theoretical study of single-particle and many-body properties of twisted bilayer WSe$_2$. For single-particle physics, we calculate the band topological phase diagram and electron local density of states (LDOS), which are found to be correlated. By comparing our theoretical LDOS with those measured by scanning tunneling microscopy, we comment on the possible topological nature of the first moir\'e valence band. For many-body physics, we construct a generalized Hubbard model on a triangular lattice based on the calculated single-particle moir\'e bands. We show that a layer potential difference, arising, for example, from an applied electric field, can drastically change the non-interacting moir\'e bands, tune the spin-orbit coupling in the Hubbard model, control the charge excitation gap of the Mott insulator at half filling, and generate an effective Dzyaloshinskii-Moriya interaction in the effective Heisenberg model for the Mott insulator. Our theoretical results agree with transport experiments on the same system in several key aspects, and establish twisted bilayer WSe$_2$ as a highly tunable system for studying and simulating strongly correlated phenomena in the Hubbard model.

Studies of surface states in Bi2Se3 induced by the BiSe substitution in the crystal subsurface structure

We present a systematic theoretical study of bismuth selenide electronic structure in the presence of spin-orbit interaction. It is confirmed that the inversion of Bi pz and Se pz states in the bulk band structure is induced by spin-orbit coupling. The energy gap in the bulk electronic structure is closed by pz states associated mainly with Bi atoms from the first quintuple layer. We elucidate the influence of Bi substitution in the fifth atomic layer on the local density of electronic states in the top quintuple layer. Finally, we describe how it develops into the additional p states in the surface electronic structure, which produce the triangular protrusion observed in Scanning Tunnelling Microscopy measurements and characteristic narrow features in Scanning Tunnelling Spectroscopy results.

The effect of size quantization on the electron spectra of graphene nanoribbons

The total electron densities of states for graphene nanoribbons with edges of different chirality, as well as the electron local densities of states for individual atoms in these nanoribbons, are calculated and analyzed. There are sharp resonance peaks near the Fermi level in the total electron densities of states of graphene nanoribbons with zigzag edges, which emerge only in the local densities of atoms from the sublattice that goes directly to the nearest edge (i.e., whose atoms have dangling bonds). Semiconducting gaps appear in the spectra of graphene nanobands with armchair chirality edges having a number of constituent atomic lines that is either a multiple of three, or gives a remainder of one when divided by three. The width of this gap only depends on the width of the nanoribbon, and is the same for all its atoms. The electron spectra of graphene nanoribbons with armchair-chirality edges have a metallic behavior if the number of atomic lines gives a remainder of two when divided by three. However, semiconducting gaps still manifest on the local densities of the atoms belonging to some lines of such nanoribbons.

Revealing the Local Electronic Structure of a Single-Layer Covalent Organic Framework through Electronic Decoupling.

Covalent organic frameworks (COFs) are molecule-based 2D and 3D materials that possess a wide range of mechanical and electronic properties. We have performed a joint experimental and theoretical study of the electronic structure of boroxine-linked COFs grown under ultrahigh vacuum conditions and characterized using scanning tunneling spectroscopy on Au(111) and hBN/Cu(111) substrates. Our results show that a single hBN layer electronically decouples the COF from the metallic substrate, thus suppressing substrate-induced broadening and revealing new features in the COF electronic local density of states (LDOS). The resulting sharpening of LDOS features allows us to experimentally determine the COF band gap, bandwidths, and the electronic hopping amplitude between adjacent COF bridge sites. These experimental parameters are consistent with the results of first-principles theoretical predictions.

Exactly solvable Majorana-Anderson impurity models

Motivated by recent experimental progress in the realization of hybrid structures with a topologically superconducting nanowire coupled to a quantum dot, viewed through the lens of the emerging field of correlated Majorana fermions, we introduce a class of interacting Majorana-Anderson impurity models which admit an exact solution for a wide range of parameters, including on-site repulsive interactions of arbitrary strength. The model is solved by mapping it via the $\mathbb{Z}_2$ slave-spin method to a noninteracting resonant level model for auxiliary Majorana degrees of freedom. The resulting gauge constraint is eliminated by exploiting the transformation properties of the Hamiltonian under a special local particle-hole transformation. For a spin-polarized Kitaev chain coupled to a quantum dot, we obtain exact expressions for the dot spectral functions at both zero and finite temperature. We study how the interaction strength and localization length of the end Majorana zero mode affect physical properties of the dot, such as quasiparticle weight, double occupancy, and odd-frequency pairing correlations, as well as the local electronic density of states in the superconducting chain.