arXiv subjects

Olle Heinonen

Publications and source records attributed to Olle Heinonen.

At least 37 records · Page 2Linked to original sources

arXiv2018

Doping a Bad Metal: Origin of Suppression of Metal-Insulator Transition in Non-Stoichiometric VO$_2$

Rutile ($R$) phase VO$_2$ is a quintessential example of a strongly correlated bad-metal, which undergoes a metal-insulator transition (MIT) concomitant with a structural transition to a V-V dimerized monoclinic phase below T$_{MIT} \sim 340K$. It has been experimentally shown that one can control this transition by doping VO$_2$. In particular, doping with oxygen vacancies ($V_O$) has been shown to completely suppress this MIT {\em without} any structural transition. We explain this suppression by elucidating the influence of oxygen-vacancies on the electronic-structure of the metallic $R$ phase VO$_2$, explicitly treating strong electron-electron correlations using dynamical mean-field theory (DMFT) as well as diffusion Monte Carlo (DMC) flavor of quantum Monte Carlo (QMC) techniques. We show that $V_O$'s tend to change the V-3$d$ filling away from its nominal half-filled value, with the $e_{g}^π$ orbitals competing with the otherwise dominant $a_{1g}$ orbital. Loss of this near orbital polarization of the $a_{1g}$ orbital is associated with a weakening of electron correlations, especially along the V-V dimerization direction. This removes a charge-density wave (CDW) instability along this direction above a critical doping concentration, which further suppresses the metal-insulator transition. Our study also suggests that the MIT is predominantly driven by a correlation-induced CDW instability along the V-V dimerization direction.

cond-mat.mtrl-sci↗

arXiv2018

Zirconia and hafnia polymorphs -- ground state structural properties from diffusion Monte Carlo

Zirconia (zirconium dioxide) and hafnia (hafnium dioxide) are binary oxides used in a range of applications. Because zirconium and hafnium are chemically equivalent, they have three similar polymorphs, and it is important to understand the properties and energetics of these polymorphs. However, while density functional theory calculations can get the correct energetic ordering, the energy differences between polymorphs depend very much on the specific density functional theory approach, as do other quantities such as lattice constants and bulk modulus. We have used highly accurate quantum Monte Carlo simulations to model the three zirconia and hafnia polymorphs. We compare our results for structural parameters, bulk modulus, and cohesive energy with results obtained from density functional theory calculations. We also discuss comparisons of our results with existing experimental data, in particular for structural parameters where extrapolation to zero temperature can be attempted. We hope our results of structural parameters as well as for cohesive energy and bulk modulus can serve as benchmarks for density-functional theory based calculations and as a guidance for future experiments.

cond-mat.mtrl-sci↗

arXiv2018

Observation of out-of-plane spin texture in a SrTiO3 (111) two-dimensional electron gas

We explore the second order bilinear magnetoelectric resistance (BMER) effect in the d-electron-based two-dimensional electron gas (2DEG) at the SrTiO3 (111) surface. We find an evidence of a spin-split band structure with the archetypal spin-momentum locking of the Rashba effect for the in-plane component. Under an out-of-plane magnetic field, we find a BMER signal that breaks the six-fold symmetry of the electronic dispersion, which is a fingerprint for the presence of a momentum dependent out-of-plane spin component. Relativistic electronic structure calculations reproduce this spin-texture and indicate that the out-of-plane component is a ubiquitous property of oxide 2DEGs arising from strong crystal field effects. We further show that the BMER response of the SrTiO3 (111) 2DEG is tunable and unexpectedly large.

cond-mat.mes-hall↗

arXiv2018

Topological Hall effect in diffusive ferromagnetic thin films with spin-flip scattering

We study the topological Hall effect in a diffusive ferromagnetic metal thin film by solving a Boltzmann transport equation in the presence of spin-flip scattering. A generalized spin diffusion equation is derived, which contains an additional source term associated with the gradient of the emergent magnetic field that arises, and its solution shows that spin accumulation may build up in the vicinity of the magnetic skyrmions. We show that the spin accumulation gives rise to a spin polarized diffusion current that in general suppresses that bulk topological Hall current. Only when the spin diffusion length is much smaller than the skyrmion size, the topological Hall resistivity approaches to the one originally derived by Bruno \textit{et al.} [Phys. Rev. Lett. \textbf{93}, 096806 (2004)]. We derive a general expression of the TH resistivity that applies to thin-film geometries with spin-flip scattering, and show that the corrections to the TH resistivity become large when the size of room temperature skyrmions is further reduced to tens of nanometers.

cond-mat.mes-hall↗

arXiv2018

QMCPACK : An open source ab initio Quantum Monte Carlo package for the electronic structure of atoms, molecules, and solids

QMCPACK is an open source quantum Monte Carlo package for ab-initio electronic structure calculations. It supports calculations of metallic and insulating solids, molecules, atoms, and some model Hamiltonians. Implemented real space quantum Monte Carlo algorithms include variational, diffusion, and reptation Monte Carlo. QMCPACK uses Slater-Jastrow type trial wave functions in conjunction with a sophisticated optimizer capable of optimizing tens of thousands of parameters. The orbital space auxiliary field quantum Monte Carlo method is also implemented, enabling cross validation between different highly accurate methods. The code is specifically optimized for calculations with large numbers of electrons on the latest high performance computing architectures, including multicore central processing unit (CPU) and graphical processing unit (GPU) systems. We detail the program's capabilities, outline its structure, and give examples of its use in current research calculations. The package is available at http://www.qmcpack.org .

physics.comp-ph↗

arXiv2017

Benchmarks and reliable DFT results for spin-crossover complexes

DFT is used throughout nanoscience, especially when modeling spin-dependent properties that are important in spintronics. But standard quantum chemical methods (both CCSD(T) and self-consistent semilocal density functional calculations) fail badly for the spin adiabatic energy difference in Fe(II) spin-crossover complexes. We show that all-electron fixed-node diffusion Monte Carlo can be converged at significant computational cost, and that the B3LYP single-determinant has sufficiently accurate nodes, providing benchmarks for these systems. We also find that density-corrected DFT, using Hartree-Fock densities (HF-DFT), greatly improves accuracy and reduces dependence on approximations for these calculations. The small gap in the self-consistent DFT calculations for the high-spin state is consistent with this. For the spin adiabatic energy differences in these complexes, HF-DFT is both accurate and reliable, and we make a strong prediction for the Fe-Porphyrin complex. The "parameter-dilemma" of needing different amounts of mixing for different properties is eliminated by HF-DFT.

physics.chem-ph↗

arXiv2017

Topologically non-trivial magnon bands in artificial square spin ices subject to Dzyaloshinskii-Moriya interaction

Systems that exhibit topologically protected edge states are interesting both from a fundamental point of view as well as for potential applications, the latter because of the absence of back-scattering and robustness to perturbations. It is desirable to be able to control and manipulate such edge states. Here, we show that artificial square ices can incorporate both features: an interfacial Dzyaloshinksii-Moriya gives rise to topologically non-trivial magnon bands, and the equilibrium state of the spin ice is reconfigurable with different configurations having different magnon dispersions and topology. The topology is found to develop as odd-symmetry bulk and edge magnon bands approach each other, so that constructive band inversion occurs in reciprocal space. Our results show that topologically protected bands are supported in square spin ices.

cond-mat.mes-hall↗

arXiv2017

The Nature of Interlayer Binding and Stacking of $sp$-$sp^{2}$ Hybridized Carbon Layers: A Quantum Monte Carlo Study

$α$-graphyne is a two-dimensional sheet of $sp$-$sp^2$ hybridized carbon atoms in a honeycomb lattice. While the geometrical structure is similar to that of graphene, the hybridized triple bonds give rise to electronic structure that is different from that of graphene. Similar to graphene, $α$-graphyne can be stacked in bilayers with two stable configurations, but the different stackings have very different electronic structures: one is predicted to have gapless parabolic bands and the other a tunable band gap which is attractive for applications. In order to realize applications, it is crucial to understand which stacking is more stable. This is difficult to model, as the stability is a result of weak interlayer van der Waals interactions which are not well captured by density functional theory (DFT). We have used quantum Monte Carlo simulations that accurately include van der Waals interactions to calculate the interlayer binding energy of bilayer graphyne and to determine its most stable stacking mode. Our results show that interlayer bindings of $sp$- and $sp^{2}$-bonded carbon networks are significantly underestimated in a Kohn-Sham DFT approach, even with an exchange-correlation potential corrected to include, in some approximation, van der Waals interactions. Finally, our quantum Monte Carlo calculations reveal that the interlayer binding energy difference between the two stacking modes is only 0.9(4) meV/atom. From this we conclude that the two stable stacking modes of bilayer $α$-graphyne are almost degenerate with each other, and both will occur with about the same probability at room temperature unless there is a synthesis path that prefers one stacking over the other.

cond-mat.mtrl-sci↗

arXiv2017

Tunable mode coupling in nano-contact spin torque oscillators

Recent experiments on spin torque oscillators have revealed interactions between multiple magnetodynamic modes, including mode-coexistence, mode-hopping, and temperature-driven cross-over between modes. Initial multimode theory has indicated that a linear coupling between several dominant modes, arising from the interaction of the subdynamic system with a magnon bath, plays an essential role in the generation of various multimode behaviors, such as mode hopping and mode coexistence. In this work, we derive a set of rate equations to describe the dynamics of coupled magnetodynamic modes in a nano-contact spin torque oscillator. Expressions for both linear and nonlinear coupling terms are obtained, which allow us to analyze the dependence of the coupled dynamic behaviors of modes on external experimental conditions as well as intrinsic magnetic properties. For a minimal two-mode system, we further map the energy and phase difference of the two modes onto a two-dimensional phase space, and demonstrate in the phase portraits, how the manifolds of periodic orbits and fixed points vary with external magnetic field as well as with temperature.

cond-mat.mes-hall↗

arXiv2017

Topological phase transformations and intrinsic size effects in ferroelectric nanoparticles

Composite materials comprised of ferroelectric nanoparticles in a dielectric matrix are being actively investigated for a variety of functional properties attractive for a wide range of novel electronic and energy harvesting devices. However, the dependence of these functionalities on shapes, sizes, orientation and mutual arrangement of ferroelectric particles is currently not fully understood. In this study, we utilize a time-dependent Ginzburg-Landau approach combined with coupled-physics finite-element-method based simulations to elucidate the behavior of polarization in isolated spherical PbTiO3 or BaTiO3 nanoparticles embedded in a dielectric medium, including air. The equilibrium polarization topology is strongly affected by particle diameter, as well as the choice of inclusion and matrix materials, with monodomain, vortex-like and multidomain patterns emerging for various combinations of size and materials parameters. This leads to radically different polarization vs electric field responses, resulting in highly tunable size-dependent dielectric properties that should be possible to observe experimentally. Our calculations show that there is a critical particle size below which ferroelectricity vanishes. For the PbTiO3 particle, this size is 2 and 3.4 nm, respectively, for high- and low-permittivity media. For the BaTiO3 particle, it is ~3.6 nm regardless of the medium dielectric strength.

cond-mat.mes-hall↗

arXiv2016

Phase Stability of TiO$_2$ Polymorphs from Diffusion Quantum Monte Carlo

Titanium dioxide, TiO$_2$, has multiple applications in catalysis, energy conversion and memristive devices because of its electronic structure. Most of these applications utilize the naturally existing phases: rutile, anatase and brookite. Despite the simple form of TiO$_2$ and its wide uses, there is long-standing disagreement between theory and experiment on the energetic ordering of these phases that has never been resolved. We present the first analysis of phase stability at zero temperature using the highly accurate many-body fixed node diffusion Quantum Monte Carlo (QMC) method. We also include the effects of temperature by calculating the Helmholtz free energy including both internal energy and vibrational contributions from density functional perturbation theory based quasi harmonic phonon calculations. Our QMC calculations find that anatase is the most stable phase at zero temperature, consistent with many previous mean-field calculations. However, at elevated temperatures, rutile becomes the most stable phase. For all finite temperatures, brookite is always the least stable phase.

cond-mat.mtrl-sci↗

arXiv2016

Oxygen modulated quantum conductance for ultra-thin HfO$_2$-based memristive switching devices

Memristive switching devices, candidates for resistive random access memory technology, have been shown to switch off through a progression of states with quantized conductance and subsequent non-integer conductance (in terms of conductance quantum $G_0$). We have performed calculations based on density functional theory to model the switching process for a Pt-HfO$_2$-Pt structure, involving the movement of one or two oxygen atoms. Oxygen atoms moving within a conductive oxygen vacancy filament act as tunneling barriers, and partition the filament into weakly coupled quantum wells. We show that the low-bias conductance decreases exponentially when one oxygen atom moves away from interface. Our results demonstrate the high sensitivity of the device conductance to the position of oxygen atoms.

cond-mat.mes-hall↗

arXiv2016

An O(N) and parallel approach to integral problems by a kernel-independent fast multipole method: Application to polarization and magnetization of interacting particles

Large classes of materials systems in physics and engineering are governed by magnetic and electrostatic interactions. Continuum or mesoscale descriptions of such systems can be cast in terms of integral equations, whose direct computational evaluation requires O(N^2) operations, where N is the number of unknowns. Such a scaling, which arises from the many-body nature of the relevant Green's function, has precluded wide-spread adoption of integral methods for solution of large-scale scientific and engineering problems. In this work, a parallel computational approach is presented that relies on using scalable open source libraries and utilizes a kernel-independent Fast Multipole Method to evaluate the integrals in O(N) operations, with O(N) memory cost, thereby substantially improving the scalability and efficiency of computational integral methods. We demonstrate the accuracy, efficiency, and scalability of our approach in the contest of two examples. In the first, we solve a boundary value problem for a ferroelectric/ferromagnetic volume in free space. In the second, we solve an electrostatic problem involving polarizable dielectric bodies in an unbounded dielectric medium. The results from these test cases show that our parallel approach, which is built on a kernel-independent FMM, can enable highly efficient and accurate simulations and allow for considerable flexibility in a broad range of applications.

physics.comp-ph↗

arXiv2016

Quantum Monte Carlo analysis of a charge ordered insulating antiferromagnet: the Ti$_4$O$_7$ Magnéli phase

The Magnéli phase Ti$_4$O$_7$ is an important transition metal oxide with a wide range of applications because of its interplay between charge, spin, and lattice degrees of freedom. At low temperatures, it has non-trivial magnetic states very close in energy, driven by electronic exchange and correlation interactions. We have examined three low-lying states, one ferromagnetic and two antiferromagnetic, and calculated their energies as well as Ti spin moment distributions using highly accurate Quantum Monte Carlo methods. We compare our results to those obtained from density functional theory-based methods that include approximate corrections for exchange and correlation. Our results confirm the nature of the states and their ordering in energy, as compared with density-functional theory methods. However, the energy differences and spin distributions differ. A detailed analysis suggests that non-local exchange-correlation functionals, in addition to other approximations such as LDA+U to account for correlations, are needed to simultaneously obtain better estimates for spin moments, distributions, energy differences and energy gaps.

cond-mat.mtrl-sci↗

arXiv2016

Direct Observation of the Skyrmion Hall Effect

The well-known Hall effect describes the transverse deflection of charged particles (electrons or holes) in an electric-current carrying conductor under the influence of perpendicular magnetic fields, as a result of the Lorentz force. Similarly, it is intriguing to examine if quasi-particles without an electric charge, but with a topological charge, show related transverse motion. Chiral magnetic skyrmions with a well-defined spin topology resulting in a unit topological charge serve as good candidates to test this hypothesis. In spite of the recent progress made on investigating magnetic skyrmions, direct observation of the skyrmion Hall effect in real space has, remained elusive. Here, by using a current-induced spin Hall spin torque, we experimentally observe the skyrmion Hall effect by driving skyrmions from creep motion into the steady flow motion regime. We observe a Hall angle for the magnetic skyrmion motion as large as 15 degree for current densities smaller than 10 MA/cm^(2) at room temperature. The experimental observation of transverse transport of skyrmions due to topological charge may potentially create many exciting opportunities for the emerging field of skyrmionics, including novel applications such as topological selection.

cond-mat.mes-hall↗

arXiv2016

Generation of magnetic skyrmion bubbles by inhomogeneous spin Hall currents

Recent experiments have shown that magnetic skyrmion bubbles can be generated and injected at room temperature in thin films [W. Jiang et al, Science vol. 349, 283 (2015)]. Here, we demonstrate, using micromagnetic modeling, that such skyrmions can be generated by an inhomogeneous spin Hall torque in the presence of Dzyaloshinskii-Moriya interactions (DMIs). In the experimental Ta/Co$_{20}$Fe$_{60}$B$_{20}$ thin films, the DMI is rather small; nevertheless, the skyrmion bubbles are stable, or at least metastable on observational time scales.

cond-mat.mes-hall↗

arXiv2016

Reconfigurable spin wave band structure of artificial square spin ice

Artificial square spin ices are structures composed of magnetic elements arranged on a geometrically frustrated lattice and located on the sites of a two-dimensional square lattice, such that there are four interacting magnetic elements at each vertex. Using a semi-analytical approach, we show that square spin ices exhibit a rich spin wave band structure that is tunable both by external magnetic fields and the configuration of individual elements. Internal degrees of freedom can give rise to equilibrium states with bent magnetization at the edges leading to characteristic excitations; in the presence of magnetostatic interactions these form separate bands analogous to impurity bands in semiconductors. Full-scale micromagnetic simulations corroborate our semi-analytical approach. Our results show that artificial square spin ices can be viewed as reconfigurable and tunable magnonic crystals that can be used as metamaterials for spin-wave-based applications at the nanoscale.

cond-mat.mes-hall↗

arXiv2016

Mobile Néel skyrmions at room temperature: status and future

Magnetic skyrmions are topologically protected spin textures that exhibit many fascinating features. As compared to the well-studied cryogenic Bloch skyrmions in bulk materials, we focus on the room-temperature Néel skyrmions in thin-film systems with an interfacial broken inversion symmetry in this article. Specifically, we show the stabilization, the creation, and the implementation of Néel skyrmions that are enabled by the electrical current-induced spin-orbit torques. Towards the nanoscale Néel skyrmions, we further discuss the challenges from both material optimization and imaging characterization perspectives.

cond-mat.mes-hall↗