Local aspects of magnetism of disordered FePt are investigated by ab initio fully relativistic full potential calculations, employing the supercell approach and the coherent potential approximation (CPA). The focus is on trends of the spin and orbital magnetic moments with chemical composition and with bond lengths around the Fe and Pt atoms. A small but distinct difference between average magnetic moments obtained when using the supercells and when relying on the CPA is identified and linked to the neglect of the Madelung potential in the CPA.
On the basis of a first-principles, relativistic electronic structure theory of finite temperature metallic magnetism, we investigate the variation of magnetic anisotropy, K, with magnetisation, M, in metallic ferromagnets. We apply the theory to the high magnetic anisotropy material, L1_0-ordered FePt, and find its uniaxial K consistent with a magnetic easy axis perpendicular to the Fe/Pt layering for all M and to be proportional to M^2 for a broad range of values of M. For small M, near the Curie temperature, the calculations pick out the easy axis for the onset of magnetic order. Our result…
The kinetics of order-disorder transition of FePt nanoparticles during high temperature annealing is theoretically investigated. A model is developed to address the influence of large surface to volume ratio of nanoparticles on both the thermodynamic and kinetic aspect of the ordering process; specifically, the nucleation and growth of L10 ordered domain within disordered nanoparticles. The size- and shape-dependence of transition kinetics are quantitatively addressed by a revised Johnson-Mehl-Avrami equation that included corrections for deviations caused by the domination of surface nucleati…
We develop a self-consistent relativistic disordered local moment (RDLM) scheme aimed at describing finite temperature magnetism of itinerant metals from first principles. Our implementation in terms of the Korringa--Kohn--Rostoker multiple scattering theory and the coherent potential approximation allows to relate the orientational distribution of the spins to the electronic structure, thus a self-consistent treatment of the distribution is possible. We present applications for bulk bcc Fe, L1$_0$-FePt and FeRh ordered in the CsCl structure. The calculations for Fe show significant variation …
We have performed a theoretical study of the magnetic circular dichroism in the x-ray absorption spectra (XMCD) of the equiatomic CoPt and FePt ordered alloys as a function of the spin quantization axis. We found that the magnetization axis is along the [001] direction and the magneto-crystalline anisotropy energy (MCA) for the FePt compound is twice as large as that of the CoPt compound in agreement with experiment. The band structure and the total density of states confirm that all electronic states contribute to the MCA, and not just the states at the vicinity of the Fermi level. The orbita…
The interface between FePt--L1$_0$ and MgO(001) alloys has been studied using density functional calculations. Because the stacking of the face-centered tetragonal L1$_0$ phase is formed by alternating Fe and Pt planes, both the Fe- and Pt-terminated contact layers were studied. Furthermore, due to the large mismatch between the in-plane lattice constants of both systems, we have chosen some common $a$ values for both alloys in order to explore in detail the adsorption energy, the electronic structure and the interface magnetism. The adsorption energy has been calculated by subtracting the ene…
We have investigated the relationship between the domain structure and the magnetic interactions in a series of FePt ferromagnetic thin films of varying thickness. As-made films grow in the magnetically soft and chemically disordered A1 phase that may have two distinct domain structures. Above a critical thickness $d_{cr}\sim 30$ nm the presence of an out of plane anisotropy induces the formation of stripes, while for $d<d_{cr}$ planar domains occur. Magnetic interactions have been characterized using the well known DCD-IRM remanence protocols, $δM$ plots, and magnetic viscosity measurements. …
Electrical manipulation of magnetization is essential for integration of magnetic functionalities such as magnetic memories and magnetic logic devices into electronic circuits. The current induced spin-orbit torque (SOT) in heavy metal/ferromagnet (HM/FM) bilayers via the spin Hall effect in the HM and/or the Rashba effect at the interfaces provides an efficient way to switch the magnetization. In the meantime, current induced SOT has also been used to switch the in-plane magnetization in single layers such as ferromagnetic semiconductor (Ga,Mn)As and antiferromagnetic metal CuMnAs with global…
We present results of the magneto-crystalline anisotropy energy (MAE) calculations for chemically ordered $L1_0$ CoPt and FePt alloys taking into account the effects of strong electronic correlations and spin-orbit coupling. The local spin density + Hubbard U approximation (LSDA+U) is shown to provide a consistent picture of the magnetic ground state properties when intra-atomic Coulomb correlations are included for both 3$d$ and 5$d$ elements. Our results demonstrate significant and complex contribution of correlation effects to large MAE of these material.
By means of density functional theory we have undertaken a structural, electronic and magnetic survey of the adsorption of the Fe_xPt_y(x,y=<4) clusters on MgO (001) surface under the generalized gradient approximation. We have tested different atomic adsorption geometries with the aim of scan a wider range of adsorption sites in order to determine the preferential surface covering. Our main conclusion in this respect is that the FePt wets the surface. The intracluster (before and after the adsorption) and cluster-to-surface binding mechanisms were investigated via the adsorption energy, charg…
Using the Boltzmann formalism based on the first principles electronic structure and scattering rates, we investigate the current-induced spin accumulation and spin-orbit torques in FePt/Pt and Co/Cu bilayers in the presence of substitutional impurities. In FePt/Pt bilayers we consider the effect of intermixing of Fe and Pt atoms in the FePt layer, and find a crucial dependence of spin accumulation and spin-orbit torques on the details of the distribution of these defects. In Co/Cu bilayers we predict that the magnitude and sign of the spin-orbit torque and spin accumulation depend very sensit…
In the disordered local moment picture, we calculated the magnetization (M) and magnetic anisotropy energy (MAE) of FePt, CoPt, and MnAl ordered alloys and body-centered tegragonal FeCo (bct-FeCo) disordered alloy, assuming spatially fluctuated spin configurations at finite temperatures. All alloys exhibit the relation K1(T)/K1(0)=(M(T)/M(0))^n with the exponent (n) around 2. This is consistent with the two-ion anisotropy model, in contrast to the usual single-ion anisotropy model exhibiting n=3. Because these systems have different mechanisms of MAE, we suggest that this relation is a general…
We carry out a systematic theoretical investigation of Magneto Crystalline Anisotropy (MCA) of L10 FePt clusters with alternating Fe and Pt planes along the (001) direction. We calculate the structural relaxation and magnetic moment of each cluster by using ab initio spin-polarized density functional theory (DFT), and the MCA with both spin-polarized DFT (including spin-orbit coupling self-consistently) and the torque method. We find that the MCA of any composite structure of a given size is enhanced with respect to that of the same-sized pure Pt or pure Fe cluster as well as to that of any pa…
We here study electronic structure and magnetic properties of disordered CoPd and CoPt alloys using Augmented Space Recursion technique coupled with the tight-binding linearized muffin tin orbital (TB-LMTO) method. Effect of short range ordering present in disordered phase of alloys on electronic and magnetic properties has been discussed. We present results for magnetic moments, Curie temperatures and electronic band energies with varying degrees of short range order for different concentrations of Co and try to understand and compare the magnetic properties and ordering phenomena in these sy…
A method of using X-ray absorption spectroscopy (XAS) together with resolved grazing incidence geometry for depth profiling atomic, electronic, chemical or magnetic local structures in thin films is presented. The quantitative deconvolution of thickness-dependent spectral features is performed by fully considering both scattering and absorption formalisms. Surface oxidation and local structural depth profiles in nanometric FePt films are determined, exemplifying the application of the method.
We here study electronic structure and magnetic properties of bcc Co$_{x}$Fe$_{1-x}$, Cr$_{x}$Fe$_{1-x}$ and Mn$_{x}$Fe$_{1-x}$ in their ferromagnetic phases using Augmented Space Recursion technique coupled with tight-binding linearized muffin tin orbital (TB-LMTO) method. We make a systematic study of magnetic properties like magnetic moment and Curie temperature and try to draw some conclusions on their variation across the row of 3-{\it d} transition metal series in periodic table using arguments based on effects like charge transfer, exchange splitting and hybridization.
Crystalline Co$_{x}$Cu$_{1-x}$ alloys show interesting magnetic behavior over the entire concentration regime. We here present a fully self- consistent first principles electronic structure studies of the electronic structure and magnetic properties of the system.We present results for the variation of density of states, magnetic moment,spin susceptibility and Curie temperature.
Cation disorder is an important design criterion for technologically relevant transition-metal (TM) oxides, such as radiation-tolerant ceramics and Li-ion battery electrodes. In this letter, we use a combination of first-principles calculations, normal mode analysis, and band-structure arguments to pinpoint a specific electronic-structure effect that influences the stability of disordered phases. We find that the electronic configuration of a TM ion determines to which extent the structural energy is affected by site distortions. This mechanism explains the stability of disordered phases with …
By means of density functional theory (DFT) and the generalized gradient approximation (GGA) we present a structural, electronic and magnetic study of FePt, CoPt, FeAu and FePd based L1$_0$ ordered cuboctahedral nanoparticles, with total numbers of atoms, N$_{tot}$ = 13, 55, 147. After a conjugate gradient relaxation, the nanoparticles retain their L1$_0$ symmetry, but the small displacements of the atomic positions tune the electronic and magnetic properties. The value of the total magnetic moment stabilizes as the size increases. We also show that the Magnetic Anisotropy Energy (MAE) depends…
The electronic, magnetic, and thermodynamic properties of ordered and chemically disordered FeRh alloy is studied using ab-initio methods. The equiatomic Fe$_{50}$Rh$_{50}$ composition is reported for both ordered and disordered phases. Chemically disordered Fe$_x$Rh$_{100-x}$ is reported and the effect of disorder on electronic and magnetic properties is discussed. Further, We have reported the effects of stress and strain in both the order and disorder phases. The result is only for the cubic phase and no distortion has been taken into consideration. This study is motivated by the recent res…
We have investigated the electronic structure of ordered and disordered Sr$_2$FeMoO$_6$ using {\it ab-initio} band structure methods. The effect of disorder was simulated within super-cell calculations to realize several configurations with mis-site disorders. It is found that such disorder effects destroy the half-metallic ferro-magnetic state of the ordered compound. It also leads to a substantial reduction of the magnetic moments at the Fe sites in the disordered configurations. Most interestingly, it is found for the disordered configurations, that the magnetic coupling within the Fe sub-l…
We propose a self-consistent approximate solution of the disordered Kondo-lattice model (KLM) to get the interconnected electronic and magnetic properties of 'local-moment' systems like diluted ferromagnetic semiconductors. Aiming at $(A_{1-x}M_x)$ compounds, where magnetic (M) and non-magnetic (A) atoms distributed randomly over a crystal lattice, we present a theory which treats the subsystems of itinerant charge carriers and localized magnetic moments in a homologous manner. The coupling between the localized moments due to the itinerant electrons (holes) is treated by a modified RKKY-theor…
Depositing disordered Al on top of SrTiO$_3$ is a cheap and easy way to create a two-dimensional electron system in the SrTiO$_3$ surface layers. To facilitate future device applications we passivate the heterostructure by a disordered LaAlO$_3$ capping layer to study the electronic properties by complementary x-ray photoemission spectroscopy and transport measurements on the very same samples. We also tune the electronic interface properties by adjusting the oxygen pressure during film growth.
Besides a drastic reduction in saturation magnetization of disordered Sr2FeMoO6 compared to highly ordered samples, magnetizations as a function of the temperature for different disordered samples may also show qualitatively different behaviors. We investigate the origin of such diversity by performing spatially resolved photoemission spectroscopy on various disordered samples. Our results establish that extensive electronic inhomogeneity, arising most probably from an underlying chemical inhomogeneity in disordered samples is responsible for the observed magnetic inhomogeneity. It is further …
Roadmap for electronic structure, anharmonicity, and electron-phonon calculations in locally disordered inorganic and hybrid halide perovskites
Univ Rennes, INSA Rennes, CNRS, Institut FOTON - UMR 6082（雷恩大学，雷恩国立应用科学学院，法国国家科学研究中心，FOTON研究所）；Computation-based Science and Technology Research Center, The Cyprus Institute（塞浦路斯研究院计算科学与技术研究中心）；Univ Rennes, ENSCR, INSA Rennes, CNRS, ISCR - UMR 6226（雷恩大学，雷恩高等师范学院，雷恩国立应用科学学院，法国国家科学研究中心，ISCR研究所）；Oden Institute for Computational Engineering and Sciences, The University of Texas at Austin（德克萨斯大学奥斯汀分校奥登计算工程与科学学院）；Department of Physics, The University of Texas at Austin（德克萨斯大学奥斯汀分校物理系）
We present a real-space formulation for calculating the electronic structure and optical conductivity of such random alloys based on the Kubo-Greenwood formalism interfaced with the augmented space recursion (ASR) [A. Mookerjee, J. Phys. C: Solid State Phys. {\bf 6}, 1340 (1973)] formulated with the Tight-binding Linear Muffin-tin Orbitals (TB-LMTO) basis with van Leeuwen-Baerends corrected exchange (vLB) [Singh et al, Phys. Rev B {\bf 93}, 085204, (2016)]. This approach has been used to quantitatively analyze the effect of chemical disorder on the configuration averaged electronic properties …
Following the finite-temperature ab initio calculation framework based on the relativistic disordered local moments, we computationally demonstrate the possibility of doping-enhanced coercivity at high-temperatures, taking YCo$_5$ as a working material in order to extract the $3d$-electron part of the electronic structure of the rare-earth permanent magnets. Alkaline-earth dopants are shown to be the candidates to realize the proposed phenomenon.
Disordered hyperuniform (DHU) states are recently discovered exotic states of condensed matter. DHU systems are similar to liquids or glasses in that they are statistically isotropic and lack conventional long-range translational and orientational order. On the other hand, they completely suppress normalized infinite-wavelength density fluctuations like crystals, and in this sense possess a hidden long-range order. Very recently, there are several exciting discoveries of disordered hyperuniformity in solid-state materials, including amorphous carbon nanotubes, amorphous 2D silica, amorphous gr…
Disordered elemental semiconductors, most notably a-C and a-Si, are ubiquitous in a myriad of different applications. These exploit their unique mechanical and electronic properties. In the past couple of decades, density functional theory (DFT) and other quantum mechanics-based computational simulation techniques have been successful at delivering a detailed understanding of the atomic and electronic structure of crystalline semiconductors. Unfortunately, the complex structure of disordered semiconductors sets the time and length scales required for DFT simulation of these materials out of re…
The evolution of electronic wave packets (WPs) through grain boundaries (GBs) of various structures in graphene was investigated by the numerical solution of the time-dependent Schroedinger equation. WPs were injected from a simulated STM tip placed above one of the grains. Electronic structure of the GBs was calculated by ab-initio and tight-binding methods. Two main factors governing the energy dependence of the transport have been identified: the misorientation angle of the two adjacent graphene grains and the atomic structure of the GB. In case of an ordered GB made of a periodic repetitio…
Disordered hyperuniformity (DHU) is a recently proposed new state of matter, which has been observed in a variety of classical and quantum many-body systems. DHU systems are characterized by vanishing infinite-wavelength density fluctuations and are endowed with unique novel physical properties. Here we report the first discovery of disordered hyperuniformity in atomic-scale 2D materials, i.e., amorphous silica composed of a single layer of atoms, based on spectral-density analysis of high-resolution transmission electron microscope images. Subsequent simulations suggest that the observed DHU …
Vacancy mechanism plays a dominant role in the atomic migration when a close-packed disordered alloy undergoes ordering transition. However, the calculation of thermal vacancy formation energies (VFEs) of random solid solutions is usually cumbersome due to the difficulty in considering various local atomic environments. Here, we propose a transparent way that combines coherent potential approximation and supercell-local cluster expansion to investigate VFEs of random solid solutions. This method is used to study the effects of temperature, strain and magnetism on the VFEs of random A1-FePt all…
We suggest a method for calculating electronic spectra in ordered and disordered semiconductor structures (superlattices) forming double quantum wells (QW). In our method, we represent the solution of Schrödinger equation for QW potential with the help of the solution of the corresponding diffusion equation. This is because the diffusion is the mechanism, which is primarily responsible for amorphization (disordering) of the QW structure, leading to so-called interface mixing. We show that the electron spectrum in such a structure depends on the shape of the quantum well, which, in turn, corres…
We have studied the electronic and magnetic properties of Fe-Pt, Co-Pt and Ni-Pt alloy systems in ordered and disordered phases. The influence of various exchange-correlation functionals on values of equilibrium lattice parameters and magnetic moments in ordered Fe-Pt, Co-Pt and Ni-Pt alloys have been studied using linearized muffin-tin orbital method. The electronic structure calculations for the disordered alloys have been carried out using augmented space recursion technique in the framework of tight binding linearized muffin-tin orbital method. The effect of short range order has also been…
We investigate electron and phonon transport through edge disordered zigzag graphene nanoribbons based on the same methodological tool of nonequilibrium Green functions. We show that edge disorder dramatically reduces phonon thermal transport while being only weakly detrimental to electronic conduction. The behavior of the electronic and phononic elastic mean free paths points to the possibility of realizing an electron-crystal coexisting with a phonon-glass. The calculated thermoelectric figure of merit (ZT) values qualify zigzag graphene nanoribbons as a very promising material for thermoele…
The electronic properties of one-dimensional clusters of N atoms or molecules have been studied. The model used is similar to the Kronig-Penney model with the potential offered by each ion being approximated by an attractive delta function. The energy eigenvalues, the eigenstates and the density of states are calculated exactly for a linear cluster of N atoms or molecules. The dependence of these quantities on the various parameters of the problem show interesting behavior. Effects of random distribution of the positions of the atoms and random distribution of the strengths of the potential ha…
We present and discuss an original method to synthesize disordered Nanostructured (NS) VO$_x$ films with controlled stoichiometry and tunable electronic structures. In these NS films, the original lattice symmetry of the bulk vanadium oxides is broken and atoms are arranged in a highly disordered structure . The stoichiometry-dependent disorder as a function of the oxygen concentration has been characterized by in-situ X-ray Absorption Near-Edge Structure (XANES) spectroscopy identifying the spectroscopic fingerprints. Results show structural rearrangements that deviate from the octahedral sym…
We study the magnetic Compton profile (MCP) of the disordered Fe$_{0.5}$Ni$_{0.5}$ and of the ordered FeNi alloys and discuss the interplay between structural disorder and electronic correlations. The Coherent Potential Approximation is employed to model the substitutional disorder within the single-site approximation, while local electronic correlations are captured with the Dynamical Mean Field Theory. Comparison with the experimental data reveals the limitation of local spin-density approximation in low momentum region, where we show that including local but dynamic correlations the experim…
Electronic properties of disordered binary alloys are studied via the calculation of the average Density of States (DOS) in two and three dimensions. We propose a new approximate scheme that allows for the inclusion of local order effects in finite geometries and extrapolates the behavior of infinite systems following `finite-size scaling' ideas. We particularly investigate the limit of the Quantum Site Percolation regime described by a tight-binding Hamiltonian. This limit was chosen to probe the role of short range order (SRO) properties under extreme conditions. The method is numerically hi…
Conjugated polymers are increasingly used as organic mixed ionic-electronic conductors in electrochemical devices for neuromorphic computing, bioelectronics and energy harvesting. The design of efficient applications relies on high electrochemical doping levels, high electronic conductivity, fast doping/dedoping kinetics and high ionic uptake. In this work, we establish structure-property relations and demonstrate how these parameters can be modulated by the co-existence of order and disorder. We use in-situ time-resolved spectroelectrochemistry, resonant Raman and terahertz conductivity measu…
Ultracold atom magnetic field microscopy enables the probing of current flow patterns in planar structures with unprecedented sensitivity. In polycrystalline metal (gold) films we observe long-range correlations forming organized patterns oriented at +/- 45 deg relative to the mean current flow, even at room temperature and at length scales orders of magnitude larger than the diffusion length or the grain size. The preference to form patterns at these angles is a direct consequence of universal scattering properties at defects. The observed amplitude of the current direction fluctuations scale…
The compound LiAl_yTi_(2-y)O_4 undergoes a metal-to-insulator transition for y_c ~0 .33. This system, in the absence of strong electronic correlations, is a prototypical example of quantum site percolation. However, it is known that the effects of disorder produced by such a percolating lattice are insufficient to explain this transition: a quantum site percolation model predicts y_c ~ 0.8, well above the experimental value. We have included an on-site Hubbard interaction into a model of this compound, using a real-space Hartree-Fock approach, and have found that for a Hubbard energy equal to …
Supercells are often used in ab initio calculations to model compound alloys, surfaces and defects. One of the main challenges of supercell electronic structure calculations is to recover the Bloch character of electronic eigenstates perturbed by disorder. Here we apply the spectral weight approach to unfolding the electronic structure of group III-V and II-VI semiconductor solid solutions. The illustrative examples include: formation of donor-like states in dilute Ga(PN) and associated enhancement of its optical activity, direct observation of the valence band anticrossing in dilute GaAs:Bi, …
We present an ab-initio formalism for the calculation of transport properties in compositionally disordered systems within the framework of the Korringa-Kohn-Rostoker non-local coherent potential approximation. Our formalism is based upon the single-particle Kubo-Greenwood linear response and provides a natural means of incorporating the effects of short-range order upon the transport properties. We demonstrate the efficacy of the formalism by examining the effects of short-range order and clustering upon the transport properties of disordered $AgPd$ and $CuZn$ alloys.
Regular nanoscale perforations in graphene (graphene antidot lattices, GAL) are known to lead to a gap in the energy spectrum, thereby paving a possible way towards many applications. This theoretical prediction relies on a perfect placement of identical perforations, a situation not likely to occur in the laboratory. Here, we present a systematic study of the effects of disorder in GALs. We consider both geometric and chemical disorder, and evaluate the density-of-states as well as the optical conductivity of disordered GALs. The theoretical method is based on an efficient algorithm for solvi…
We present KITE, a general purpose open-source tight-binding software for accurate real-space simulations of electronic structure and quantum transport properties of large-scale molecular and condensed systems with tens of billions of atomic orbitals (N~10^10). KITE's core is written in C++, with a versatile Python-based interface, and is fully optimised for shared memory multi-node CPU architectures, thus scalable, efficient and fast. At the core of KITE is a seamless spectral expansion of lattice Green's functions, which enables large-scale calculations of generic target functions with unifo…
Motivated by the increasing number of systems featuring multiple bands at low energy, we address the Boltzmann approach to transport in a multiband weakly disordered noninteracting crystal subject to a small electric field. In general, the multiband structure leads to a considerable complication of the Boltzmann equation. Indeed, even in the presence of elastic impurity scattering, one needs to compute for each band and momentum the dressed velocities, which account for scattering events. Here we provide a semianalytical solution to the Boltzmann equation that reduces such a challenging numeri…
Charge and thermal conductivities are the most important parameters of carbon nanomaterials as candidates for future electronics. In this paper we address the effects of Anderson type disorder in long semiconductor carbon nanotubes (CNTs) to electron charge conductivity and lattice thermal conductivity using the atomistic Green function approach. The electron and phonon transmissions are analyzed as a function of the length of the disordered nanostructures. The thermal conductance as a function of temperature is calculated for different lengths. Analysis of the transmission probabilities as a …
Accurate prediction of chemical short-range order and its effect on thermodynamic, structural, and electronic properties of disordered alloys: exemplified in Cu$_{3}$Au
The Kronig-Penney model is used to Study the effect of nonlinear interaction on the transmissive properties of both ordered and disordered chains. In the ordered case, the nonlinearity can either localize or delocalize the electronic states depending on both its sign and strength but there is a critical strength above which all the states are localized. In the disordered case, however, we found that the transmission decays as $T\sim L^{-γ}$ around the band edge of the corresponding periodic system. The exponent $γ$ is independent of the strength of the nonlinearity in the case of disordered ba…
We comment on article by Yi Zhang , Hanna Terletska, Ka-Ming Tam, Yang Wang, Markus Eisenbach, Liviu Chioncel, and Mark Jarrell [Phys. Rev. B {\bf 100}, 054205 (2019)]\cite{Zhang} in which to study substitution disordered systems, they presented an embedding scheme for the locally self-consistent method. Here we show that their methods is a truncated case of our super-cell approximation, achieved by neglecting super-cell wave vectors dependence on self-energy $Σ_{sc}({\bf K}_{n},E)$ and replacing them by a local on-site self-energy, $Σ_{sc}({\bf K}_{n},E)=Σ_{sc}(L,L,E)$ in our articles\cite{Mo…
