arXiv subjects

Walter R. L. Lambrecht

Publications and source records attributed to Walter R. L. Lambrecht.

54 records · Page 3Linked to original sources

arXiv2019

Quasiparticle self-consistent $GW$ band structures of Mg-IV-N$_2$ compounds: the role of semicore $d$ states

We present improved band structure calculations of the Mg-IV-N$_2$ compounds in the quasiparticle self-consistent $GW$ approximation. Compared to previous calculations (Phys. Rev. B 94, 125201 (2016)) we here include the effects of the Ge-3$d$ and Sn-4$d$ semicore states and find that these tend to reduce the band gap significantly. This places the band gap of MgSnN$_2$ in the difficult to reach green region of the visible spectrum. The stability of the materials with respect to competing binary compounds is also evaluated and details of the valence band maximum manifold splitting and effective masses are provided.

cond-mat.mtrl-sci↗

arXiv2019

Computational study of Electron Paramagnetic Resonance parameters for Mg and Zn impurities in $β$-Ga$_2$O$_3$

A computational study of the electron paramagnetic resonance (EPR) $g$-tensors and hyperfine tensors in Mg and Zn doped $β$-Ga$_2$O$_3$ is presented. While Mg has been found previously to prefer the octahedral site, we find here that Zn prefers the tetrahedral substitutional site. The EPR signatures are found to be distinct for the two sites. Good agreement with experiment is found for the $g$-tensor and hyperfine interaction for Mg$_\mathrm{Ga2}$ and predictions are made for the Zn case.

cond-mat.mtrl-sci↗

arXiv2019

Computational identification of Ga-vacancy related electron paramagnetic resonance centers in $β$-Ga$_2$O$_3$

A combined experimental/theoretical study of the EPR in irradiated $β$-Ga$_2$O$_3$ is presented. Four EPR spectra, two $S=1/2$ and two $S=1$, are observed after high-energy proton or electron irradiation. One of the S=1/2 spectra (EPR1) can be observed at room temperature and below and is characterized by the spin Hamiltonian parameters $g_b=2.0313$, $g_c=2.0079$, $g_{a*}=2.0025$ and a quasi isotropic hyperfine interaction with two equivalent Ga neighbors of $~\sim$14 G on $^{69}$Ga. The second (EPR2) is observed after photoexcitation (with threshold 2.8 eV) at low temperature and is characterized by $g_b=2.0064$, $g_c=2.0464$, $g_{a*}=2.0024$ and a quasi isotropic hyperfine interaction with two equivalent Ga neighbors of 10 G. A spin $S=1$ spectrum with a similar g-tensor and a 50\% reduced hyperfine splitting accompanies each of these, which is indicative of a defect of two weakly coupled $S=1/2$ centers. DFT calculations of the magnetic resonance fingerprint of a wide variety of native defect models are carried out to identify these EPR centers in terms of specific defect configurations. The EPR1 center is proposed to correspond to a complex of two tetrahedral $V_\mathrm{Ga1}$ with an interstitial Ga in between them. This model was previously shown to have lower energy than the simple tetrahedral Ga vacancy and has a $2-/3-$ transition level higher than other $V_\mathrm{Ga}$ related models, which would explain why the other ones are already in their diamagnetic $3-$ state and are thus not observed if the Fermi level is pinned approximately at this level. The EPR2 spectra are proposed to correspond to the octahedral $V_\mathrm{Ga2}$. Models based on self-trapped holes and oxygen interstitials are ruled out because they would have hyperfine interaction with more than two Ga nuclei and because they can not support a corresponding $S=1$ center.

cond-mat.mtrl-sci↗

arXiv2019

Quasiparticle self-consistent $GW$ electronic band structures of Be-IV-N$_2$ compounds

The electronic band structures of BeSiN$_2$ and BeGeN$_2$ compounds are calculated using the quasiparticle self-consistent $GW$ method. The lattice parameters are calculated for the wurtzite based crystal structure commonly found in other II-IV-N$_2$ compounds with the $Pbn$2$_1$ space group. They are determined both in the local density approximation (LDA) and generalized gradient approximation (GGA), which provide lower and upper limits. At the GGA lattice constants, which gives lattice constants closer to the experimental ones, BeSiN$_2$ is found to have an indirect band gap of 6.88 eV and its direct gap at $Γ$ is 7.77 eV, while in BeGeN$_2$ the gap is direct at $Γ$ and equals 5.03 eV. To explain the indirect gap in BeSiN$_2$, comparisons are made with the parent III-N compound w-BN band structure. The effective mass parameters are also evaluated and found to decrease from BeSiN$_2$ to BeGeN$_2$.

cond-mat.mtrl-sci↗

arXiv2018

Proton Irradiation Induced Defects in \b{eta}-Ga2O3: a combined EPR and Theory Study

Proton irradiation of both n-type and semi-insulating bulk samples of \b{eta}-Ga2O3 leads to the formation of one paramagnetic defect with spin S=1/2, monoclinic point symmetry, a g-tensor with principal values of gb=2.0313, gc=2.0079, ga*= 2.0025 and quasi isotropic superhyperfine interaction of 13G with two equivalent Ga neigbours. Its high introduction rate indicates it to be a primary irradiation induced defect. At low temperature, photoexcitation transforms this defect into a different metastable S=1/2 center with principal g-values of gb=2.0064, gc=2.0464, ga*= 2.0024 and a reduced hyperfine interaction of 9G. This metastable defect is stable up to T=100K, when it switches back to the previous configuration. Density functional theory calculations of the Spin Hamiltonian parameters of various intrinsic defects are carried out using the Gauge Including Projector Augmented Wave method in order to determine the microscopic structure of these defects.Our results do not support the intuitive model of the isolated octahedral or tetrahedral gallium vacancy, VGa2-, but favor the model of a gallium vacancy complex VGa-Gai-VGa.

cond-mat.mtrl-sci↗

arXiv2018

Instability of the layered orthorhombic post-perovskite phase of SrTiO$_3$ and other candidate orthorhombic phases under pressure

While the tetragonal antiferro-electrically distorted (AFD) phase with space group $I4/mcm$ is well known for SrTiO$_3$ to occur below 105 K, there are also some hints in literature of an orthorhombic phase, either at lower temperature at high pressure. A previously proposed orthorhombic layered structure of SrTiO$_3$, known as the post-perovskite or CaIrO$_3$ structure with space group $Cmcm$ is shown to have significantly higher energy than the cubic or tetragonal phase and to have its minimum volume at larger volume than cubic perovskite. It thus cannot correspond to a high-pressure phase of SrTiO$_3$. We also study an alternative $Pnma$ phase obtained by two octahedral rotations about different axes. This phase is found to have slightly lower energy than the $I4/mcm$ phase in spite of the fact that its parent, in-phase tilted $P4/mbm$ phase is not found to occur. Alternative ferro-electric tetragonal and orthorhombic structures are also considered. These are not found to occur in our zero temperature calculations but have been suggested in previous literature to occur at higher temperature.

cond-mat.mtrl-sci↗

arXiv2017

Native interstitial defects in ZnGeN$_2$

A density functional study is presented of the interstitial Zn$_i$, Ge$_i$, and N$_i$ in ZnGeN$_2$. Corrections to the band gap are included by means of the LDA+U method. The Zn and Ge interstitials are both found to strongly prefer the larger octahedral site compared to the two types of tetrahedral sites. The Zn interstitial is found to be a shallow double donor but has higher energy than previously studied antisite defects. It has a resonance in the conduction band which is Zn-$s$ like. The Ge interstitial is an even higher energy of formation defect and also behaves as a shallow double donor but has also a deep level in the gap, corresponding to a Ge-$s$ orbital character while the Ge-$p$ forms a resonance in the conduction band. The nitrogen interstitial forms a split-interstitial configuration, as also occurs in GaN. Its electronic levels can be related to that of a N$_2$ molecule. The defect levels in the gap correspond to the $π_g$-like lowest unoccupied molecular orbital (LUMO) of the molecule, which here becomes filled with 3 electrons in the defect's neutral charge state. They are found to prefer a high-spin configuration in the $q=+1$ state. The corresponding transition levels are obtained and show that this is an amphoteric trap level occurring in $+2$, $+1$, 0 and $-1$ charge states. The two possible sites for this split interstitial, on top of Zn or on top of Ge differ slightly in N$_2$ bond-length. While the N$_i$ defects have the lowest formation energy among the interstitials, it is still higher than that of the antisites. Hence they are not expected to occur in sufficient concentration to affect the intrinsic Fermi level position. In particular, they do not contribute to the unintentional n-type background doping.

cond-mat.mtrl-sci↗

arXiv2017

All-electron quasi-particle self-consistent $GW$ band structures for SrTiO$_3$ including lattice polarization corrections in different phase

The electronic band structure of SrTiO$_3$ is investigated in the all-electron QS$GW$ approximation. Unlike previous pseudopotential based QS$GW$ or single-shot $G_0W_0$ calculations, the gap is found to be significantly overestimated compared to experiment. After putting in a correction for the underestimate of the screening by the random phase approximation in terms of a 0.8$Σ$ approach, the gap is still overestimated. The 0.8$Σ$ approach is discussed and justified in terms of various recent literature results including electron-hole corrections. Adding a lattice polarization correction (LPC) in the ${\bf q}\rightarrow0$ limit for the screening of $W$, agreement with experiment is recovered. The LPC is alternatively estimated using a polaron model. We apply our approach to the cubic and tetragonal phases as well as a hypothetical layered post-perovskite structure and find that the LDA (local density approximation) to $GW$ gap correction is almost independent of structure.

cond-mat.mtrl-sci↗

arXiv2017

Lattice polarization effects on the screened Coulomb interaction $W$ of the GW approximation

In polar insulators where longitudinal and transverse optical phonon modes differ substantially, the electron-phonon coupling affects the energy-band structure primarily through the long-range Fröhlich contribution to the Fan term. This diagram has the same structure as the $GW$ self-energy where $W$ originates from the electron part of the screened coulomb interaction. The two can be conveniently combined by combining electron and lattice contributions to the polarizability. Both contributions are nonanalytic at the origin, and diverge as $1/q^2$ so that the predominant contribution comes from a small region around $q{=}0$. Here we adopt a simple estimate for the Fröhlich contribution by assuming that the entire phonon part can be attributed to a small volume of $q$ near $q{=}0$. We estimate the magnitude for $\mathbf{q}{\rightarrow}0$ from a generalized Lyddane-Sachs-Teller relation, and the radius from the inverse of the polaron length scale. The gap correction is shown to agree with Fröhlich's simple estimate $-α_Pω_L/2$ of the polaron effect.

cond-mat.mtrl-sci↗

arXiv2016

Raman study of the vibrational modes in ZnGeN2 (0001)

A Raman spectroscopy study was carried out for ZnGeN2 with direction of propagation along the (0001) crystallographic direction on hexagonal single crystal platelets obtained by reaction of gaseous ammonia with a Zn-Ge-Sn liquid alloy at 758 degree C. The sample geometry allowed measurement of the a2 and a1 Raman modes. First-principles calculations were carried out of the spectra. Measurements with crossed polarizers yielded spectra that agreed well with first-principles calculations of the a2 modes. Measurements with parallel polarizers should in principle provide the a1L modes. However, for most of the Raman modes, the LO-TO splitting was calculated to be very small, and for the few modes which were predicted to have larger LO-TO splittings, the LO mode was not observed. This absence is tentatively explained in terms of overdamped LO-plasmon coupling. LO-TO mode crossing was identified by comparing the calculated eigenvectors and intensities of individual modes. Some features in the experimental spectra were identified as arising from critical points in the phonon density of states and are indicative of the degree of disorder on the cation lattice.

cond-mat.mtrl-sci↗

arXiv2013

Strain effects on the spin-orbit induced band structure splittings in monolayer MoS2 and graphene

The strain effects on the spin-orbit induced splitting of the valence band maximum and conduction band minimum in monolayer MoS2 and the gap in graphene are calculated using first-principles calculations. The dependence of these splittings on the various symmetry types of strain is described by means of an effective Hamiltonian based on the method of invariants and the parameters in the model are extracted by fitting to the theory. These splittings are related to acoustic phonon deformation potentials, or electron-phonon coupling matrix elements which enter the spin-dependent scattering theory of conduction in these materials.

cond-mat.mtrl-sci↗

arXiv2012

Rare-earth mononitrides

When the rare earth mononitrides (RENs) first burst onto the scientific scene in the middle of last century, there were feverish dreams that their strong magnetic moment would afford a wide range of applications. For decades research was frustrated by poor stoichiometry and the ready reaction of the materials in ambient conditions, and only recently have these impediments finally been overcome by advances in thin film fabrication with ultra-high vacuum based growth technology. Currently, the field of research into the RENs is growing rapidly, motivated by the materials demands of proposed electronic and spintronic devices. Both semiconducting and ferromagnetic properties have been established in some of the RENs which thus attract interest for the potential to exploit the spin of charge carriers in semiconductor technologies for both fundamental and applied science. In this review, we take stock of where progress has occurred within the last decade in both theoretical and experimental fields, and which has led to the point where a proof-of-concept spintronic device based on RENs has already been demonstrated. The article is organized into three major parts. First, we describe the epitaxial growth of REN thin films and their structural properties, with an emphasis on their prospective spintronic applications. Then, we conduct a critical review of the different advanced theoretical calculations utilised to determine both the electronic structure and the origins of the magnetism in these compounds. The rest of the review is devoted to the recent experimental results on optical, electrical and magnetic properties and their relation to current theoretical descriptions. These results are discussed particularly with regard to the controversy about the exact nature of the magnetic state and conduction processes in the RENs.

cond-mat.str-el↗

arXiv2006

Electronic structure of Gd pnictides

A computational study of the electronic structure and magnetic properties of Gd-pnictides is reported. The calculations were performed using a full-potential linear muffin-tin orbital (LMTO) method within the so-called LSDA+U approach, which adds Hubbard-U correlation effects to specified narrow bands in a mean-field approach to the local spin density approximation (LSDA). Here both the Gd 4f and 5d states are subject to such corrections. The U(f) values were determined semi-empirically by using photo-emission and inverse photoemission data for GdP, GdAs, GdSb and GdBi. In contrast to U(f) which represents narrow band physics, U(d) represents a quasiparticle self-energy correction of the LSDA gap underestimate. The U(d) value was adjusted using optical absorption data for semiconducting GdN above its Curie temperature. Below the Curie temperature, however, in the ferromagnetic state, the gap becomes almost zero. The other Gd pnictides are found to have a small overlap of the conduction band at the X point and the valence band at the Gamma point in the majority-spin channel. A small gap opens in the spin-minority channel of GdP and GdAs, which are thus half-metallic. This spin-minority gap closes in semimetallic GdSb and GdBi. While GdN is found to be ferromagnetic, the other Gd-pnictides are found to be antiferromagnetic, with ordering along [111]. From calculations with different magnetic configurations, a Heisenberg model with first and second nearest neighbor exchange parameters is extracted. The Heisenberg model is then used to predict Curie-Weiss and N'eel temperatures and critical magnetic fields within mean field and compared with experimental data. The trends are found to be in good agreement with the experimental data.

cond-mat.mtrl-sci↗

arXiv1998

Second harmonic generation and birefringence of some ternary pnictide semiconductors

A first-principles study of the birefringence and the frequency dependent second harmonic generation (SHG) coefficients of the ternary pnictide semiconductors with formula ABC$_2$ (A = Zn, Cd; B = Si, Ge; C = As, P) with the chalcopyrite structures was carried out. We show that a simple empirical observation that a smaller value of the gap is correlated with larger value of SHG is qualitatively true. However, simple inverse power scaling laws between gaps and SHG were not found. Instead, the real value of the nonlinear response is a result of a very delicate balance between different intraband and interband terms.

cond-mat.mtrl-sci↗

arXiv1997

Second harmonic generation in SiC polytypes

LMTO calculations are presented for the frequency dependent second harmonic generation (SHG) in the polytypes 2H, 4H, 6H, 15R and 3C of SiC. All independent tensor components are calculated. The spectral features and the ratios of the 333 to 311 tensorial components are studied as a function of the degree of hexagonality. The relationship to the linear optical response and the underlying band structure are investigated. SHG is suggested to be a sensitive tool for investigating the near band edge interband excitations.

cond-mat↗

arXiv1997

Total energy differences between SiC polytypes revisited

The total energy differences between various SiC polytypes (3C, 6H, 4H, 2H, 15R and 9R) were calculated using the full-potential linear muffin-tin orbital method using the Perdew-Wang-(91) generalized gradient approximation to the exchange-correlation functional in the density functional method. Numerical convergence versus k-point sampling and basis set completeness are demonstrated to be better than 1 meV/atom. The parameters of several generalized anisotropic next-nearest-neighbor Ising models are extracted and their significance and consequences for epitaxial growth are discussed.

cond-mat.mtrl-sci↗

arXiv1997

Efficient ab-initio method for the calculation of frequency dependent non-linear optical response in semiconductors: application to second harmonic generation

A LMTO implementation of Aversa and Sipe's length-gauge formalism for calculating the full frequency dependent second-harmonic generation in the independent particle approximation is presented. It is applied to GaAs, GaP, 3C-SiC, c-BN and wurtzite and zincblende GaN and AlN. The use of the scissor's operator for correcting LDA errors is discussed and compared to an alternative approach in which the Hamiltonian is corrected. The latter is found to be superior. Decomposition in omega and 2 omega resonances and in intra- and inter-band contributions and in specific band-to-band contributions are presented.

cond-mat.mtrl-sci↗

arXiv1995

Band structure analysis of the conduction-band mass anisotropy in 6H and 4H SiC

The band structures of 6H and 4H SiC calculated by means of the FP-LMTO method are used to determine the effective mass tensors for their conduction-band minima. The results are shown to be consistent with recent optically detected cyclotron resonance measurements and predict an unusual band filling dependence for 6H-SiC.

mtrl-th↗