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cond-mat.mtrl-sci

11957 works46100 researchers

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24 paper(s) to start with

preprint2016arXiv

Strong anisotropy within a Heisenberg model in the J=1/2 insulating state of Sr2Ir0.8Ru0.2O4

The dispersive magnetic excitations in Sr2IrO4 have previously been well described within an isospin-1/2 Heisenberg model on a square lattice that revealed parallels with La2CuO4. Here we investigate the inelastic spectra of Sr2Ir0.8Ru0.2O4 with resonant inelastic x-ray scattering (RIXS) at the Ir L3-edge. The results are well described using linear spin-wave theory within a similar Heisenberg model applicable to Sr2IrO4, however the disorder induced by the substitution of 20% Ir4+ ions for Ru4+ removes longer range exchange interactions. A large spin-gap (40 meV) is measured indicating strong anisotropy from spin-orbit coupling that is manifest due to the altered magnetic structure in Sr2Ir0.8Ru0.2O4 with c-axis aligned moments compared to the basal plane moments in the parent. Collectively the results indicate the robustness of a Heisenberg model description even when the magnetic structure is altered and the J=1/2 moments diluted.

preprint2016arXiv

Effects of electron-impurity scattering on density of states in silicene: impurity bands and band-gap narrowing

Considering the interband correlation, we present a generalized multiple-scattering approach of Green's function to investigate the effects of electron-impurity scattering on the density of states in silicene. The reduction of energy gaps in the case of relatively high chemical potential and the transformation of split-off impurity bands into band tails for low chemical potential are found. The dependency of optical conductivity on the impurity concentration is also discussed for frequency within the terahertz regime.

preprint2017arXiv

Room temperature dynamic correlation between methylammonium molecules in lead-iodine based perovskites: An ab-initio molecular dynamics perspective

The high efficiency of lead organo-metal-halide perovskite solar cells has raised many questions about the role of the methylammonium (MA) molecules in the Pb-I framework. Experiments indicate that the MA molecules are able to 'freely' spin around at room temperature even though they carry an intrinsic dipole moment. We have performed large supercell (2592 atoms) finite temperature ab-initio molecular dynamics calculations to study the correlation between the molecules in the framework. An underlying long range anti-ferroelectric ordering of the molecular dipoles is observed. The dynamical correlation between neighboring molecules shows a maximum around room temperature in the mid-temperature phase. In this phase, the rotations are slow enough to (partially) couple to neighbors via the Pb-I cage. This results in a collective motion of neighboring molecules in which the cage acts as the mediator. At lower and higher temperatures the motions are less correlated.

preprint2016arXiv

Stacking-sequence-independent band structure and shear exfoliation of two-dimensional electride materials

The electronic band structure of crystals is generally influenced by the periodic arrangement of their constituent atoms. Specifically, the emerging two-dimensional (2D) layered structures have shown different band structures with respect to their stacking configurations. Here, based on first-principles density-functional theory calculations, we demonstrate that the band structure of the recently synthesized 2D Ca$_2$N electride changes little for the stacking sequence as well as the lateral interlayer shift. This intriguing invariance of band structure with respect to geometrical variations can be attributed to a complete screening of [Ca$_2$N]$^{+}$ cationic layers by anionic excess electrons delocalized between the cationic layers. The resulting weak interactions between 2D dressed cationic layers give rise to not only a shallow potential barrier for bilayer sliding but also an electron-doping facilitated shear exfoliation. Our findings open a route for exploration of the peculiar geometry-insensitive electronic properties in 2D electride materials, which will be useful for future thermally stable electronic applications.

preprint2016arXiv

Elasto-buoyant heavy spheres: a unique way to test non-linear elasticity

Extra-large deformations in ultra-soft elastic materials are ubiquitous, yet systematic studies and methods to understand the mechanics of such huge strains are lacking. Here we investigate this complex problem systematically with a simple experiment: by introducing a heavy bead of radius $a$ in an incompressible ultra-soft elastic medium. We find a scaling law for the penetration depth ($δ$) of the bead inside the softest gels as $δ\sim a^{3/2}$. While this result is inconsistent with an ideal neo-Hookean model of elastic deformation, according to which the displacement fields must diverge, it is vindicated by an original asymptotic analytic model developed in this article. This model demonstrates that the observed relationship is precisely at the demarcating boundary of what would be required for the field variables to either diverge or converge. This correspondence between a unique mathematical prediction and the experimental observation ushers in new insights into the behavior of the deformations of strongly non-linear materials.

preprint2016arXiv

An Array of Layers in Silicon Sulfides: Chain-like and Ground State Structures

While much is known about isoelectronic materials related to carbon nanostructures, such as boron nitride layers and nanotubes, rather less is known about equivalent silicon based materials. Following the recent discovery of phosphorene, we herein discuss isoelectronic silicon monosulfide monolayers. We describe a set of anisotropic ground state structures that clearly have a high stability with respect to the near isotropic silicon monosulfide monolayers. The source of the layer anisotropy is related to the presence of Si-S double chains linked by some Si-Si covalent bonds, which lye at the core of the increased stability, together with a remarkable spd hybridization on Si. The involvement of d orbitals brings more variety to silicon-sulfide based nanostructures that are isoelectronic to phosphorene, which could be relevant for future applications, adding extra degrees of freedom.

preprint2016arXiv

Electronic structure tuning via surface modification in semimetallic nanowires

Electronic structure properties of nanowires (NW) with diameters of 1.5 nm and 3 nm based on semimetallic $α$-Sn are investigated by employing density functional theory and perturbative $GW$ methods. We explore the dependence of electron affinity, band structure and band gap values with crystallographic orientation, NW cross-sectional size and surface passivants of varying electronegativity. We consider four chemical terminations in our study: methyl ($\rm{CH_3}$), hydrogen ($\rm{H}$), hydroxyl ($\rm{OH}$), and fluorine ($\rm{F}$). Results suggest a high degree of elasticity of Sn-Sn bonds within the SnNWs' cores with no significant structural variations for nanowires with different surface passivants. Direct band gaps at Brillouin zone centers are found for most studied structures with quasi-particle corrected band gap magnitudes ranging from 0.25 eV to 3.54 eV in 1.5 nm diameter structures indicating an exceptional range of properties for semimetal NWs below the semimetal-to-semiconductor transition. Band gap variations induced by changes in surface passivants indicate the possibility of realizing semimetal-semiconductor interfaces in NWs with constant cross-section and cryst

preprint2016arXiv

Persisting of Polar Distortion with Electron Doping in Lone-Pair Driven Ferroelectrics

Free electrons can screen out long-range Coulomb interaction and destroy the polar distortion in some ferroelectric materials, whereas the coexistence of polar distortion and metallicity were found in several non-central-symmetric metals (NCSMs). Therefore, the mechanisms and designing of NCSMs have attracted great interests. In this work, by first-principles calculation, we found the polar distortion in the lone-pair driven ferroelectric material PbTiO$_3$ can not only persist, but also increase with electron doping. We further analyzed the mechanisms of the persisting of the polar distortion. We found that the Ti site polar instability is suppressed but the Pb site polar instability is intact with the electron doping. The Pb-site instability is due to the lone-pair mechanism which can be viewed as a pseudo-Jahn-Teller effect, a mix of the ground state and the excited state by ion displacement from the central symmetric position. The lone-pair mechanism is not strongly affected by the electron doping because neither the ground state or the excited state involved is at the Fermi energy. The enhancement of the polar distortion is related to the increasing of the Ti ion size by dopin

preprint2016arXiv

Phase-field modeling of chemical control of polarization stability and switching dynamics in ferroelectric thin film

Phase-field simulation (PFS) have revolutionized the understanding of domain structure and switching behavior in ferroelectric thin films and ceramics. Generally, PFS is based on solution of a (set) of Ginzburg-Landau equations for a defined order parameter field(s) under physical boundary conditions (BCs) of fixed potential or charge. While well-matched to the interfaces in bulk materials and devices, these BCs are generally not applicable to free ferroelectric surfaces. Here, we developed a self-consistent phase-field model with boundary conditions based on electrochemical equilibria. We chose Pb(Zr0.2Ti0.8)O3 ultrathin film consisting of (001) oriented single tetragonal domain (Pz) as a model system, and systematically studied the effects of oxygen partial pressure, temperature and surface ion on the ferroelectric state, and compared it with the case of complete screening. We have further explored the polarization switching induced by the oxygen partial pressure and observed pronounced size effect induced by chemical screening. Our work thus helps to understand the emergent phenomena in ferroelectric thin films brought about by the electrochemical ionic surface compensations.

preprint2016arXiv

Resonance Damping of the THz-frequency Transverse Acoustic Phonon in the Relaxor Ferroelectric KTa1-xNbxO3

The damping ($Γ_a$) of the transverse acoustic (TA) phonon in single crystals of the relaxor $KTa_{1-x}Nb_xO_3$ with x=0.15-0.17 was studied by means of high resolution inelastic cold neutron scattering near the (200) B.Z. point where diffuse scattering is absent, although it is present near (110). In a wide range of temperatures centered on the phase transition, T=195K-108K, the TA phonon width (damping) exhibits a step increase around momentum q=0.07, goes through a shallow maximum at q=0.09-0.12 and remains high up to the highest momentum studied of q=0.16. These experimental results are explained in terms of a resonant interaction between the TA phonon and the collective or correlated reorientation through tunneling of the off-center Nb+5 ions. The observed TA damping is successfully reproduced in a simple model that includes an interaction between the TA phonon and a dispersionless localized mode (LM) with frequency $ω_L$ and damping $Γ_L$ ($Γ_L < ω_L$), itself coupled to the transverse optic (TO) mode. Maximum damping of the TA phonon occurs when its frequency $ω_a \approx{ω_L}$. $ω_L$ and $Γ_L$ are moderately dependent on temperature but the oscillator strength, $M_2$, of th

preprint2017arXiv

Generation and evolution of spin-, valley- and layer-polarized excited carriers in inversion-symmetric WSe2

Manipulation of spin and valley degrees of freedom is a key step towards realizing novel quantum technologies, for which atomically thin transition metal dichalcogenides (TMDCs) have been established as promising candidates. In monolayer TMDCs, the lack of inversion symmetry gives rise to a spin-valley correlation of the band structure allowing for valley-selective electronic excitation with circularly polarized light. Here we show that, even in centrosymmetric samples of 2H-WSe2, circularly polarized light can generate spin-, valley- and layer-polarized excited states in the conduction band. Employing time- and angle-resolved photoemission spectroscopy (trARPES) with spin-selective excitation, the dynamics of valley and layer pseudospins of the excited carriers are investigated. Complementary time-dependent density functional theory (TDDFT) calculations of the excited state populations reveal a strong circular dichroism of the spin-, valley- and layer-polarizations and a pronounced 2D character of the excited states in the K valleys. We observe scattering of carriers towards the global minimum of the conduction band on a sub-100 femtosecond timescale to states with three-dimension

preprint2016arXiv

Gate-independent energy gap in non-covalently intercalated bilayer graphene on SiC(0001)

Our first-principles calculations show that an energy gap around 0.12-0.25 eV can be engineered in epitaxial graphene on SiC(0001) through the non-covalent intercalation of transition- or alkali-metals, yet originated from the distinct mechanisms. The former is attributed to the combined effects of metal induced perpendicular electric field and interaction while the latter is solely attributed to the built-in electric field. A great advantage of this scheme is that the gap size is almost independent of the gate voltage up to 1 V/nm, thus reserving the electric means to tune the Fermi level of graphene when configured as field-effect transistors. Given the recent progress in experimental techniques on the intercalated graphene, our findings provide a practical way to incorporate the graphene with the current semiconductor industry.

preprint2017arXiv

Critical assessment of the equilibrium melting-based, energy distribution theory of supercooled liquids and application to jammed systems

Despite decades of intense study, the mechanisms underlying the extraordinary dynamics of supercooled liquids as they approach the glass transition remain, at best, mis-characterized, and at worst, misunderstood. A long standing endeavor is to understand the remarkable increase of the viscosity with supercooling. Recently, a new theory of supercooled liquids has been proposed that starts from first principles, using elementary statistical mechanics arguments, to derive a form for the viscosity that contains only a single fitting parameter in its simplest form. In this we demonstrate that this exact same form may be derived from a different starting point, and then critically examine its performance. In the process we find that functional form proposed fits the viscosity data of a diverse group of 45 liquids exceptionally well over a wide temperature range, and uncover a number of interesting correlations of the single parameter with various thermodynamic quantities, ultimately allowing for the prediction of low temperature viscosity from high temperature data. Additionally, we find that similar physical reasoning can be used to derive a similar, single parameter form for the viscos

preprint2016arXiv

Theory of Exciton Energy Transfer in Carbon Nanotube Composites

We compute the exciton transfer (ET) rate between semiconducting single-wall carbon nanotubes (SWNTs). We show that the main reasons for the wide range of measured ET rates reported in the literature are 1) exciton confinement in local quantum wells stemming from disorder in the environment and 2) exciton thermalization between dark and bright states due to intratube scattering. The SWNT excitonic states are calculated by solving the Bethe-Salpeter equation using tight-binding basis functions. The ET rates due to intertube Coulomb interaction are computed via Fermi's golden rule. In pristine samples, the ET rate between parallel (bundled) SWNTs of similar chirality is very high ($\sim 10^{14}\;\text{s}^{-1}$) while the ET rate for dissimilar or nonparallel tubes is considerably lower ($\sim 10^{12}\;\text{s}^{-1}$). Exciton confinement reduces the ET rate between same-chirality parallel SWNTs by two orders of magnitude, but has little effect otherwise. Consequently, the ET rate in most measurements will be on the order of $ 10^{12}\;\text{s}^{-1}$, regardless of the tube relative orientation or chirality. Exciton thermalization between bright and dark states further reduces the

preprint2016arXiv

Comparison of device structures for the dielectric breakdown measurement of hexagonal boron nitride

Improving the film quality in the synthesis of large-area hexagonal boron nitride films (h-BN) for two-dimensional material devices remains a great challenge. The measurement of electrical breakdown dielectric strength (EBD) is one of the most important methods to elucidate the insulating quality of h-BN. In this work, the EBD of high quality exfoliated single-crystal h-BN was investigated using three different electrode structures under different environmental conditions to determine the ideal electrode structure and environment for EBD measurement. A systematic investigation revealed that EBD is not sensitive to contact force or electrode area but strongly depends on the relative humidity during measurement. Once the measurement environment is properly managed, it was found that the EBD values are consistent within experimental error regardless of the electrode structure, which enables the evaluation of the crystallinity of synthesized h-BN at the microscopic and macroscopic level by utilizing the three different electrode structures properly for different purposes.

preprint2017arXiv

Electronic structure and oxygen reduction on tunable [Ti(IV)Pc]2+and Ti(II)Pc titanyl-phthalocyanines: A quantum chemical prediction

The high cost of platinum-based catalysts has hampered the commercialization of polymer electrolyte membrane fuel cells (PEMFCs). Hence, the electronic structure and oxygen reduction ability of [Ti(IV)Pc]2+, Ti(II)Pc titanyl-phthalocyanines, and their tailored peripheral and axial ligand complexes were theoretically investigated to determine non-precious cathode catalysts. Our results revealed that the peripherally substituted and unsubstituted Ti(II)Pc triplet complexes can spontaneously reduce peroxide. The singlet [Ti(IV)Pc]2+ parent complex has a 6.45 eV barrier. However, fluorine substitution at peripheral positions reduced the energy barrier up to 0.45 eV. In addition, chlorine substitution has shown spontaneous peroxide reduction as in the case of triplets. The high catalytic activity of Ti(II)Pc complexes and singlet chlorine substituted complex is attributed to the optimal charge transfer between dioxygen molecule and the novel catalyst complexes. As a result, Ti(II)Pcs and chlorine substituted singlet complexes are considered as potential substitutions for the noble Pt-based catalyst for the PEMFCs.

preprint2016arXiv

Sequential pulsed laser deposition of homoepitaxial SrTiO$_3$ thin films

Control of thin film stoichiometry is of primary relevance to achieve desired functionality. Pulsed laser deposition ablating from binary-oxide targets (sequential deposition) can be applied to precisely control the film composition, offsetting the importance of growth conditions on the film stoichiometry. In this work, we demonstrate that the cation stoichiometry of SrTiO$_3$ thin films can be finely tuned by sequential deposition from SrO and TiO$_2$ targets. Homoepitaxial SrTiO$_3$ films were deposited at different substrate temperatures and Ti/Sr pulse ratios, allowing the establishment of a growth window for stoichiometric SrTiO$_3$. The growth kinetics and nucleation processes were studied by reflection high-energy electron diffraction and atomic force microscopy, providing information about the growth mode and the degree of off-stoichiometry. At the optimal (stoichiometric) growth conditions, films exhibit atomically flat surfaces, whereas off-stoichiometry is accommodated by crystal defects, 3D islands and/or surface precipitates depending on the substrate temperature and the excess cation. This technique opens the way to precisely control stoichiometry and doping of oxide

preprint2016arXiv

Time-reversal-breaking topological phases in antiferromagnetic Sr$_2$FeOsO$_6$ films

In this work, we studied time-reversal-breaking topological phases as a result of the interplay between antiferromagnetism and inverted band structures in thin films of antiferromagnetic double perovskite transition-metal Sr$_2$FeOsO$_6$. By combining the first-principles calculations and analytical models, we demonstrate that the quantum anomalous Hall phase and chiral topological superconducting phase can be realized in this system. We find that to achieve time-reversal-breaking topological phases in antiferromagnetic materials, it is essential to break the combined symmetry of time reversal and inversion, which generally exists in antiferromagnetic structures. As a result, we can utilize an external electric gate voltage to induce the phase transition between topological phases and trivial phases, thus providing an electrically controllable topological platform for the future transport experiments.

preprint2016arXiv

Theoretical and numerical investigation of diffusive instabilities in multi-component alloys

Mechanical properties of engineering alloys are strongly correlated to their microstructural length scale. Diffusive insta- bilities of the Mullins-Sekerka type is one of the principal mechanisms through which the scale of the microstructural features are determined during solidification. In contrast to binary systems, in multicomponent alloys with arbitrary interdiffusivities, the growth rate as well as the maximally growing wavelengths characterizing these instabilities depend on the the dynamically selected equilibrium tie-lines and the steady state growth velocity. In this study, we derive analytical expressions to characterize the dispersion behavior in isothermally solidified multicomponent (quaternary) alloys for different choices of the inter-diffusivity matrices and confirm our calculations using phase-field simulations. Thereafter, we perform controlled studies to capture and isolate the dependence of instability length scales on solute diffusivities and steady state planar front velocities, which leads to an understanding of the process of length scale selection during the onset of instability for any alloy composition with arbitrary diffusivities, comprising of both ind

preprint2016arXiv

Frequency estimate for multicomponent crystalline compounds

Among crystal structures of N-component metal alloys, far fewer examples are known with N>=4 than with N=2 or 3, in apparent contradiction to the exponentially growing number of possible combinations of elements. Two effects contribute to this shortfall. Since the N-component composition space resides within a d-dimensional simplex with d=N-1, the vanishing volume in high dimensions reduces the distinct N-component compositions. Additionally, the increasing surface area makes it more probable that stable structures reside on the surface of the simplex (containing fewer than N components) as opposed to its interior. Despite their rarity, we propose that the actual number of N=4- and 5-component alloys greatly exceeds the number that are currently known. Specific estimates are developed through application of the empirical Miedema enthalpy model.

preprint2017arXiv

Anomalous resistivity upturn in epitaxial L21-Co2MnAl films

We report the controllable growth and the intriguing transport behavior of high-spin-polarization epitaxial L21-Co2MnAl films, which exhibit a low-temperature (T) resistivity upturn with pronounced T1/2 dependence, close relevance to structural disorder, and robust independence of magnetic fields. The resistivity upturn turns out to be qualitatively contradictory to weak localization, particle-particle channel electron-electron interaction (EEI), and orbital two-channel Kondo effect, leaving a three-dimensional particle-hole channel EEI the most likely physical source. Our result highlights a considerable tunability of the structural and electronic disorder of magnetic films by varying growth temperature, affording unprecedented insights into the spin polarization and the resistivity upturn.

preprint2016arXiv

Ab initio study of the strain dependence of thermopower in electron-doped SrTiO$_3$

In this paper we explore the different mechanisms that affect the thermopower of a band insulating perovskite (in this case, SrTiO$_3$) when subject to strain (both compressive or tensile). We analyze the high temperature, entropy dominated limit and the lower temperature, energy-transport regime. We observe that the effect of strain in the high-temperature Seebeck coefficient is small at the concentration levels of interest for thermoelectric applications. However, the effective mass changes substantially with strain, which produces an opposite effect to that of the degeneracy-breakups produced by strain. In particular, we find that the thermopower can be enhanced by applying tensile strain in the adequate regime. We conclude that the detrimental effect of strain in thermopower due to band splitting is a minor effect that will not hamper the optimization of the thermoelectric properties of oxides with t$_{2g}$-active bands by applying strain.

preprint2016arXiv

Wide-Field Strain Imaging with Preferentially-Aligned Nitrogen-Vacancy Centers in Polycrystalline Diamond

We report on wide-field optically detected magnetic resonance imaging of nitrogen-vacancy centers (NVs) in type IIa polycrystalline diamond. These studies reveal a heterogeneous crystalline environment that produces a varied density of NV centers, including preferential orientation within some individual crystal grains, but preserves long spin coherence times. Using the native NVs as nanoscale sensors, we introduce a 3-dimensional strain imaging technique with high sensitivity ( $< 10^{-5}$ Hz$^{-1/2}$) and diffraction-limited resolution across a wide field of view.

preprint2015arXiv

Poisson's Ratio of Layered Two-dimensional Crystals

We present first-principles calculations of elastic properties of multilayered two-dimensional crystals such as graphene, h-BN and 2H-MoS2 which shows that their Poisson's ratios along out-of-plane direction are negative, near zero and positive, respectively, spanning all possibilities for sign of the ratios. While the in-plane Poisson's ratios are all positive regardless of their disparate electronic and structural properties, the characteristic interlayer interactions as well as layer stacking structures are shown to determine the sign of their out-of-plane ratios. Thorough investigation of elastic properties as a function of the number of layers for each system is also provided, highlighting their intertwined nature between elastic and electronic properties.

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