350 research outputs found
Green's function multiple-scattering theory with a truncated basis set: An Augmented-KKR formalism
Korringa-Kohn-Rostoker (KKR) Green's function, multiple-scattering theory is
an efficient site-centered, electronic-structure technique for addressing an
assembly of scatterers. Wave-functions are expanded in a spherical-wave
basis on each scattering center and indexed up to a maximum orbital and
azimuthal number , while scattering matrices, which
determine spectral properties, are truncated at where phase
shifts are negligible. Historically, is set equal
to ; however, a more proper procedure retains free-electron and
single-site contributions for with set to
zero [Zhang and Butler, Phys. Rev. B {\bf 46}, 7433]. We present a numerically
efficient and accurate \emph{augmented}-KKR Green's function formalism that
solves the KKR secular equations by matrix inversion [ process
with rank ] and includes higher-order contributions via
linear algebra [ process with rank ].
Augmented-KKR yields properly normalized wave-functions, numerically cheaper
basis-set convergence, and a total charge density and electron count that
agrees with Lloyd's formula. For fcc Cu, bcc Fe and L CoPt, we present the
formalism and numerical results for accuracy and for the convergence of the
total energies, Fermi energies, and magnetic moments versus for a
given .Comment: 7 pages, 5 figure
Origin of magnetic anisotropy in doped Ce2Co17 alloys
Magnetocrystalline anisotropy (MCA) in doped Ce2Co17 and other competing structures was investigated using density functional theory. We confirmed that the MCA contribution from dumbbell Co sites is very negative. Replacing Co dumbbell atoms with a pair of Fe or Mn atoms greatly enhance the uniaxial anisotropy, which agrees quantitatively with experiment, and this enhancement arises from electronic-structure features near the Fermi level, mostly associated with dumbbell sites. With Co dumbbell atoms replaced by other elements, the variation of anisotropy is generally a collective effect and contributions from other sublattices may change significantly. Moreover, we found that Zr doping promotes the formation of 1-5 structure that exhibits a large uniaxial anisotropy, such that Zr is the most effective element to enhance MCA in this system
Better band gaps for wide-gap semiconductors from a locally corrected exchange-correlation potential that nearly eliminates self-interaction errors
This work constitutes a comprehensive and improved account of
electronic-structure and mechanical properties of silicon-nitride (Si3N4)
polymorphs via van Leeuwen and Baerends (LB) exchange-corrected local density
approximation (LDA) that enforces the exact exchange potential asymptotic
behavior. The calculated lattice constant, bulk modulus, and electronic band
structure of Si3N4 polymorphs are in good agreement with experimental results.
We also show that, for a single electron in a hydrogen atom, spherical well, or
harmonic oscillator, the LB-corrected LDA reduces the (self-interaction) error
to exact total energy to ~10%, a factor of three to four lower than standard
LDA, due to a dramatically improved representation of the exchange-potential.Comment: 6 pages, 3 figure
Better Band Gaps with Asymptotically Corrected Local Exchange Potentials
We formulate a spin-polarized van Leeuwen and Baerends (vLB) correction to
the local density approximation (LDA) exchange potential [Phys. Rev. A 49, 2421
(1994)] that enforces the ionization potential (IP) theorem following Stein et
al. [Phys. Rev. Lett. 105, 266802 (2010)]. For electronic-structure problems,
the vLB-correction replicates the behavior of exact-exchange potentials, with
improved scaling and well-behaved asymptotics, but with the computational cost
of semi-local functionals. The vLB+IP corrections produces large improvement in
the eigenvalues over that from LDA due to correct asympotic behavior and atomic
shell structures, as shown on rare-gas, alkaline-earth, zinc-based oxides,
alkali-halides, sulphides, and nitrides. In half-Heusler alloys, this
asymptotically-corrected LDA reproduces the spin-polarized properties
correctly, including magnetism and half-metallicity. We also considered
finite-sized systems [e.g., ringed boron-nitirde (BN) and
graphene (C)] to emphasize the wide applicability of the method.Comment: 9 pages, 3 figure
Intrinsic magnetic properties in R(Fe1−xCox)11TiZ(R=Yand Ce;Z=H,C,and N)
To guide improved properties coincident with reduction of critical materials in permanent magnets, we investigate via density functional theory (DFT) the intrinsic magnetic properties of a promising system, R(Fe1−xCox)11TiZ with R=Y, Ce and interstitial doping (Z=H,C,N). The magnetization M, Curie temperature TC, and magnetocrystalline anisotropy energy K calculated in local density approximation to DFT agree well with measurements. Site-resolved contributions to K reveal that all three Fe sublattices promote uniaxial anisotropy in YFe11Ti, while competing anisotropy contributions exist in YCo11Ti. As observed in experiments on R(Fe1−xCox)11Ti, we find a complex nonmonotonic dependence of K on Co content and show that anisotropy variations are a collective effect of MAE contributions from all sites and cannot be solely explained by preferential site occupancy. With interstitial doping, calculated TC enhancements are in the sequence of N\u3eC\u3eH, with volume and chemical effects contributing to the enhancement. The uniaxial anisotropy of R(Fe1−xCox)11TiZ generally decreases with C and N; although, for R=Ce, C doping is found to greatly enhance it for a small range of 0.
Half-metallic Co-based quaternary Heusler alloys for spintronics: Defect- and pressure-induced transitions and properties
Heusler compounds offer potential as spintronic devices due to their spin polarization and half-metallicity properties, where electron spin-majority (minority) manifold exhibits states (band gap) at the electronic chemical potential, yielding full spin polarization in a single manifold. Yet, Heuslers often exhibit intrinsic disorder that degrades its half-metallicity and spin polarization. Using density-functional theory, we analyze the electronic and magnetic properties of equiatomic Heusler (L21) CoMnCrAl and CoFeCrGe alloys for effects of hydrostatic pressure and intrinsic disorder (thermal antisites, binary swaps, and vacancies). Under pressure, CoMnCrAl undergoes a metallic transition, while half-metallicity in CoFeCrGe is retained for a limited range. Antisite disorder between Cr-Al pair in CoMnCrAl alloy is energetically the most favorable, and retains half-metallic character in Cr-excess regime. However, Co-deficient samples in both alloys undergo a transition from half-metallic to metallic, with a discontinuity in the saturation magnetization. For binary swaps, configurations that compete with the ground state are identified and show no loss of half-metallicity; however, the minority-spin band gap and magnetic moments vary depending on the atoms swapped. For single binary swaps, there is a significant energy cost in CoMnCrAl but with no loss of half-metallicity. Although a few configurations in CoFeCrGe energetically compete with the ground state, the minority-spin band gap and magnetic moments vary depending on the atoms swapped. This information should help in controlling these potential spintronic materials
Short-range order in archetypal disordered Cu3Au: effects on thermodynamic, structural, and mechanical properties
Density-functional theory based electronic-structure method was used to
demonstrate the effect of chemical short-range order (SRO) on thermodynamic,
structural, electronic, and mechanical properties of archetypal
face-centered-cubic CuAu alloy. We show that SRO can be tuned to modify
bonding characteristics, lattice dynamics (i.e., phonons), and electronic
structure of disordered CuAu with direct impact on thermodynamic and
mechanical properties. The formation energy of disordered phase (-34.3
meV-atom) was found to increase by nearly 34 meV-atom in presence
of SRO (-68.2 meV-atom). The vibrational entropy estimated form phonon
dispersions decreases with increasing short-range order, which shows
significant drop below room temperature, e.g., from 9 at 300 K to
6 at 100 K. The SRO shows weak effect on average mechanical properties
(Bulk, Young's, and Shear moduli), however, the directional dependence of
Young's and Shear moduli was increased substantially in presence of SRO. We
established through detailed analysis of archetypal CuAu that ignoring
SRO may lead to a skewed view of the actual properties of the disordered phase
of more chemically complex alloys. More generally, our results indicate SRO can
be used as a control parameter that can be tuned to achieve desirable
properties.Comment: 17 pages, 12 figures, 3 table
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