arXiv subjects

Igor A. Abrikosov

Publications and source records attributed to Igor A. Abrikosov.

At least 55 records · Page 3Linked to original sources

arXiv2017

Identification of Si-vacancy related room temperature qubits in 4H silicon carbide

Identification of microscopic configuration of point defects acting as quantum bits is a key step in the advance of quantum information processing and sensing. Among the numerous candidates, silicon vacancy related centers in silicon carbide (SiC) have shown remarkable properties owing to their particular spin-3/2 ground and excited states. Although, these centers were observed decades ago, still two competing models, the isolated negatively charged silicon vacancy and the complex of negatively charged silicon vacancy and neutral carbon vacancy [Phys. Rev. Lett.\ \textbf{115}, 247602 (2015)] are argued as an origin. By means of high precision first principles calculations and high resolution electron spin resonance measurements, we here unambiguously identify the Si-vacancy related qubits in hexagonal SiC as isolated negatively charged silicon vacancies. Moreover, we identify the Si-vacancy qubit configurations that provide room temperature optical readout.

cond-mat.mtrl-sci↗

arXiv2017

Hybrid-DFT+V$_w$ method for accurate band structure of correlated transition metal compounds: the case of cerium dioxide

Hybrid functionals' non-local exchange-correlation potential contains a derivative discontinuity that improves on standard semi-local density functional theory (DFT) band gaps. Moreover, by careful parameterization, hybrid functionals can provide self-interaction reduced description of selected states. On the other hand, the uniform description of all the electronic states of a given system is a know drawback of these functionals that causes varying accuracy in the description of states with different degrees of localization. This limitation can be remedied by the orbital dependent exact exchange extension of hybrid functionals; the hybrid-DFT+V$_w$ method [V. Iv{á}dy, et al., Phys. Rev. B 90, 035146 (2014)]. Based on the analogy of quasi-particle equations and hybrid-DFT single particle equations, here we demonstrate that parameters of hybrid-DFT+V$_w$ functional can be determined from approximate quasi-particle spectra. The proposed technique leads to a reduction of self-interaction and provides improved description for both $s$ / $p$ and $d$ / $f$-electrons of the simulated system. The performance of our charge self-consistent method is illustrated on the electronic structure calculation of cerium dioxide where good agreement with both quasi-particle and experimental spectra is achieved.

cond-mat.mtrl-sci↗

arXiv2017

The origin of the core-level binding energy shifts in nanoclusters

We investigate the shifts of the core-level binding energies in small gold nanoclusters by using {\it ab initio} density functional theory calculations. The shift of the 4$f$ states is calculated for magic number nanoclusters in a wide range of sizes and morphologies. We find a non-monotonous behavior of the core-level shift in nanoclusters depending on the size. We demonstrate that there are three main contributions to the Au 4$f$ shifts, which depend sensitively on the interatomic distances, coordination and quantum confinement. They are identified and explained by the change of the on-site electrostatic potential.

cond-mat.mes-hall↗

arXiv2016

Finite temperature elastic constants of paramagnetic materials within the disordered local moment picture from ab initio molecular dynamics calculations

We present a theoretical scheme to calculate the elastic constants of magnetic materials in the high-temperature paramagnetic state. Our approach is based on a combination of disordered local moments picture and ab initio molecular dynamics (DLM-MD). Moreover, we investigate a possibility to enhance the efficiency of the simulations of elastic properties using recently introduced method: symmetry imposed force constant temperature dependent effective potential (SIFC-TDEP). We have chosen cubic paramagnetic CrN as a model system. This is done due to its technological importance and its demonstrated strong coupling between magnetic and lattice degrees of freedom. We have studied the temperature dependent single-crystal and polycrystalline elastic constants of paramagentic CrN up to 1200 K. The obtained results at T= 300 K agree well with the experimental values of polycrystalline elastic constants as well as Poisson ratio at room temperature. We observe that the Young's modulus is strongly dependent on temperature, decreasing by ~14% from T=300 K to 1200 K. In addition we have studied the elastic anisotropy of CrN as a function of temperature and we observe that CrN becomes substantially more isotropic as the temperature increases. We demonstrate that the use of Birch law may lead to substantial errors for calculations of temperature induced changes of elastic moduli. The proposed methodology can be used for accurate predictions of mechanical properties of magnetic materials at temperatures above their magnetic order-disorder phase transition.

cond-mat.mtrl-sci↗

arXiv2016

High fidelity bi-directional nuclear qubit initialization in SiC

Dynamic nuclear polarization (DNP) is an attractive method for initializing nuclear spins that are strongly coupled to optically active electron spins because it functions at room temperature and does not require strong magnetic fields. In this Letter, we demonstrate that DNP, with near-unity polarization efficiency, can be generally realized in weakly coupled hybrid registers, and furthermore that the nuclear spin polarization can be completely reversed with only sub-Gauss magnetic field variations. This mechanism offers new avenues for DNP-based sensors and radio-frequency free control of nuclear qubits.

cond-mat.mes-hall↗

arXiv2016

Structural and electronic properties of Li intercalated graphene on SiC(0001)

We investigate the structural and electronic properties of Li-intercalated monolayer graphene on SiC(0001) using combined angle-resolved photoemission spectroscopy and first-principles density functional theory. Li intercalates at room temperature both at the interface between the buffer layer and SiC and between the two carbon layers. The graphene is strongly $n$-doped due to charge transfer from the Li atoms and two $π$-bands are visible at the $\bar{K}$-point. After heating the sample to 300$^\circ$C, these $π$-bands become sharp and have a distinctly different dispersion to that of Bernal-stacked bilayer graphene. We suggest that the Li atoms intercalate between the two carbon layers with an ordered structure, similar to that of bulk LiC$_6$. An AA-stacking of these two layers becomes energetically favourable. The $π$-bands around the $\bar{K}$-point closely resemble the calculated band structure of a C$_6$LiC$_6$ system, where the intercalated Li atoms impose a super-potential on the graphene electronic structure that opens pseudo-gaps at the Dirac points of the two $π$-cones.

cond-mat.mtrl-sci↗

arXiv2016

Efficient and accurate determination of lattice-vacancy diffusion coefficients via non equilibrium ab initio molecular dynamics

We revisit the color-diffusion algorithm [P. C. Aeberhard et al., Phys. Rev. Lett. 108, 095901 (2012)] in nonequilibrium ab initio molecular dynamics (NE-AIMD), and propose a simple efficient approach for the estimation of monovacancy jump rates in crystalline solids at temperatures well below melting. Color-diffusion applied to monovacancy migration entails that one lattice atom (colored-atom) is accelerated toward the neighboring defect-site by an external constant force F. Considering bcc molybdenum between 1000 and 2800 K as a model system, NE-AIMD results show that the colored-atom jump rate k_{NE} increases exponentially with the force intensity F, up to F values far beyond the linear-fitting regime employed previously. Using a simple model, we derive an analytical expression which reproduces the observed k_{NE}(F) dependence on F. Equilibrium rates extrapolated by NE-AIMD results are in excellent agreement with those of unconstrained dynamics. The gain in computational efficiency achieved with our approach increases rapidly with decreasing temperatures, and reaches a factor of four orders of magnitude at the lowest temperature considered in the present study.

cond-mat.mtrl-sci↗

arXiv2015

Dirac points with giant spin-orbit splitting in the electronic structure of two-dimensional transition-metal carbides

Two-dimensional (2D) materials, especially their most prominent member, graphene, have greatly influenced many scientific areas. Moreover, they have become a base for investigating the relativistic properties of condensed matter within the emerging field of Dirac physics. This has ignited an intense search for new materials where charge carriers behave as massless or massive Dirac fermions. Here, we theoretically show the existence of Dirac electrons in a series of 2D transition-metal carbides, known as MXenes. They possess twelve conical crossings in the 1st Brillouin zone with giant spin-orbit splitting. Our findings indicate that the 2D band structure of MXenes is protected against external perturbations and preserved even in multilayer phases. These results, together with the broad possibilities to engineer the properties of these materials phases, make Dirac MXenes a potential candidate for studying and developing novel Dirac-physics-based technologies.

cond-mat.mtrl-sci↗

arXiv2015

Pressure induced crossing of the core-levels in 5d metals

Pressure induced interaction between core electrons, the core level crossing (CLC) transition has been observed in hcp Os at P~400 GPa [L. Dubrovinksy, et al., Nature 525, 226-229 (2015)]. In this work, we carry out a systematic study of the influence of pressure on the electronic structure in all metals of the 5d series (Hf,Ta,W,Re,Os,Ir,Pt,Au) using first-principles electronic structure calculations. We have found that CLC is a general effect for this series of metals. While in Pt it occurs at ~1500 GPa, at a pressure substantially higher than in Os, in Ir it occurs already at 80 GPa. Moreover, we predict that in Re the CLC transition may appear at ambient pressure. We analyze the shifts of the CLC transition pressure across the series within the Thomas-Fermi model, and show that the effect has many common features to the atomic collapse in the rare-earth elements.

cond-mat.mtrl-sci↗

arXiv2015

Anharmonicity changes the solid solubility of an alloy at high temperatures

We have developed a method to accurately and efficiently determine the vibrational free energy as a function of temperature and volume for substitutional alloys from first principles. Taking Ti$_{1-x}$Al$_x$N alloy as a model system, we calculate the isostructural phase diagram by finding the global minimum of the free energy, corresponding to the true equilibrium state of the system. We demonstrate that the anharmonic contribution and temperature dependence of the mixing enthalpy have a decisive impact on the calculated phase diagram of a Ti$_{1-x}$Al$_x$N alloy, lowering the maximum temperature for the miscibility gap from 6560 K to 2860 K. Our local chemical composition measurements on thermally aged Ti$_{0.5}$Al$_{0.5}$N alloys agree with the calculated phase diagram.

cond-mat.mtrl-sci↗

arXiv2015

Theoretical model of the dynamic spin polarization of nuclei coupled to paramagnetic point defects in diamond and silicon carbide

Dynamic nuclear spin polarization (DNP) mediated by paramagnetic point defects in semiconductors is a key resource for both initializing nuclear quantum memories and producing nuclear hyperpolarization. DNP is therefore an important process in the field of quantum-information processing, sensitivity-enhanced nuclear magnetic resonance, and nuclear-spin-based spintronics. DNP based on optical pumping of point defects has been demonstrated by using the electron spin of nitrogen-vacancy (NV) center in diamond, and more recently, by using divacancy and related defect spins in hexagonal silicon carbide (SiC). Here, we describe a general model for these optical DNP processes that allows the effects of many microscopic processes to be integrated. Applying this theory, we gain a deeper insight into dynamic nuclear spin polarization and the physics of diamond and SiC defects. Our results are in good agreement with experimental observations and provide a detailed and unified understanding. In particular, our findings show that the defects' electron spin coherence times and excited state lifetimes are crucial factors in the entire DNP process.

cond-mat.mes-hall↗

arXiv2015

The morphology transition mechanism from icosahedral to decahedral phase during growth of nanoclusters

The morphology transition from the thermodynamically favorable to the unfavorable phase during growth of free-standing copper nanoclusters is studied by molecular dynamics simulations. We give a detailed description of the kinetics and thermodynamics of the process. A universal mechanism of a solid-solid transition, from icosahedral to decahedral morphology in nanoclusters, is proposed. We show that a formation of distorted NC during the growth process with islands of incoming atoms localized in certain parts of the grown particle may shift the energy balance between Ih and Dh phases in favour of the latter leading to the morphology transition deep within the thermodynamic stability field of the former. The role of diffusion in the morphology transition is revealed. In particular, it is shown that fast diffusion should suppress the morphology transition and favour homogeneous growth of the nanoclusters.

cond-mat.mes-hall↗

arXiv2014

The role of N defects in paramagnetic CrN at finite temperatures from first-principles

Simulations of defects in paramagnetic materials at high temperature constitute a formidable challenge to solid state theory due to the interaction of magnetic disorder, vibrations, and structural relaxations. CrN is a material where these effects are particularly large due to a strong magneto-lattice coupling and a tendency for deviations from the nominal 1:1 stoichiometry. In this work we present a first-principles study of nitrogen vacancies and nitrogen interstitals in CrN at elevated temperature. We report on formation energetics, the geometry of interstital nitrogen dimers, and impact on the electronic structure caused by the defects. We find a vacancy formation energy of 2.28 eV with a small effect of temperature, a formation energy for N interstitial in the form of a $\big<111\big>$ oriented split-bond of 3.77 eV with an increase to 3.97 at 1000 K. Vacancies are found to add three electrons while split bond interstitial adds one electron to the conduction band. The band gap of defect-free CrN is smeared out due to vibrations, though it is difficult to draw conclusion about the exact temperature at which the band gap closes from our calculations. However, it is clear that at 900 K there is a non-zero density of electronic states at the Fermi level. At 300 K our results indicate a boarder case were the band-gap is about to close.

cond-mat.str-el↗

arXiv2014

Molecular dynamics simulation of growth of Cu nanoclusters from Cu-ions in a plasma

A recently developed method of nanoclusters growth in a pulsed plasma is studied by means of molecular dynamics. A model that allows one to consider high-energy charged particles in classical molecular dynamics is suggested, and applied for studies of single impact events in nanoclusters growth. In particular, we provide a comparative analysis of the well-studied inert gas aggregation method and the growth from ions in a plasma. The importance to consider of the angular distribution of incoming ions in the simulations of the nanocluster growth is underlined. A detailed study of the energy transfer from the incoming ions to a nanocluster, as well as the diffusion of incoming ions on the cluster surface is carried out. Our results are important for understanding and control of the nanocluster growth process.

cond-mat.mes-hall↗

arXiv2014

Theoretical unification of hybrid-DFT and DFT+U methods for the treatment of localized orbitals

We formulate the on-site occupation dependent exchange correlation energy and effective potential of hybrid functionals for localized states and connect them to the on-site correction term of the DFT+U method. Our derivation provides a theoretical justification for adding a DFT+U-like onsite potential in hybrid DFT calculations to resolve issues caused by overscreening of localized states. The resulting scheme, hybrid- DFT+Vw, is tested for chromium impurity in wurtzite AlN and vanadium impurity in 4H-SiC, which are paradigm examples of systems with different degree of localization between host and impurity orbitals.

cond-mat.str-el↗

arXiv2014

Vibrational free energy and phase stability of paramagnetic and antiferromagnetic CrN from ab-initio molecular dynamics

We present a theoretical first-principles method to calculate the free energy of a magnetic system in its high-temperature paramagnetic phase, including vibrational, electronic, and magnetic contributions. The method for calculating free energies is based on ab-initio molecular dynamics and combines a treatment of disordered magnetism using disordered local moments molecular dynamics (DLM-MD) with the temperature dependent effective potential (TDEP) method to obtain the vibrational contribution to the free energy. We illustrate the applicability of the method by obtaining the anharmonic free energy for the paramagnetic cubic and the antiferromagnetic orthorhombic phases of chromium nitride. The influence of lattice dynamics on the transition between the two phases is demonstrated by constructing the temperature-pressure phase diagram.

cond-mat.mtrl-sci↗

arXiv2013

Electrically and mechanically tunable electron spins in silicon carbide color centers

The electron spins of semiconductor defects can have complex interactions with their host, particularly in polar materials like SiC where electrical and mechanical variables are intertwined. By combining pulsed spin resonance with ab-initio simulations, we show that spin-spin interactions within SiC neutral divacancies give rise to spin states with an enhanced Stark effect, sub-10**-6 strain sensitivity, and highly spin-dependent photoluminescence with intensity contrasts of 15-36%. These results establish SiC color centers as compelling systems for sensing nanoscale fields.

cond-mat.mes-hall↗

arXiv2013

Temperature dependent effective third order interatomic force constants from first principles

The temperature dependent effective potential (TDEP) method is generalized beyond pair interactions. The second and third order force constants are determined consistently from ab initio molecular dynamics simulations at finite temperature. The reliability of the approach is demonstrated by calculations of the Mode Grüneisen parameters for Si. We show that the extension of TDEP to higher order allows for an efficient calculation of the phonon life time, in Si as well as in $ε$-FeSi, a system that exhibits anomalous softening with temperature.

cond-mat.mtrl-sci↗