Hasil untuk "cond-mat.mtrl-sci"

Kai Xu, Luis Pérez-Fidalgo, Bethan L. Charles et al.

The exceptional optoelectronic properties of metal halide perovskites (MHPs) are presumed to arise, at least in part, from the peculiar interplay between the inorganic metal-halide sublattice and the atomic or molecular cations enclosed in the cage voids. The latter can exhibit a roto-translative dynamics, which is shown here to be at the origin of the structural behavior of MHPs as a function of temperature, pressure and composition. The application of high hydrostatic pressure allows for unraveling the nature of the interaction between both sublattices, characterized by the simultaneous action of hydrogen bonding and steric hindrance. In particular, we find that under the conditions of unleashed cation dynamics, the key factor that determines the structural stability of MHPs is the repulsive steric interaction rather than hydrogen bonding. Taking as example the results from pressure and temperature-dependent photoluminescence and Raman experiments on MAPbBr$_3$ but also considering the pertinent MHP literature, we provide a general picture about the relationship between the crystal structure and the presence or absence of cationic dynamic disorder. The reason for the structural sequences observed in MHPs with increasing temperature, pressure, A-site cation size or decreasing halide ionic radius is found principally in the strengthening of the dynamic steric interaction with the increase of the dynamic disorder. In this way, we have deepened our fundamental understanding of MHPs; knowledge that could be coined to improve performance in future optoelectronic devices based on this promising class of semiconductors.

Takashi U. Ito

A recent muon spin rotation ($μ^+$SR) study on a paramagnetic defect complex formed upon implantation of $μ^+$ pseudo-proton into SrTiO$_3$ is reviewed with a specific focus on the relation with experimental signatures of coexisting delocalized and localized electrons in hydrogen-irradiated metallic SrTiO$_3$ films. The paramagnetic defect complex, composed of interstitial $μ^+$ and Ti$^{3+}$ small polaron, is characterized by a small dissociation energy of about 30 meV. Density functional theory (DFT) calculations in the generalized gradient approximation (GGA) +$U$ scheme for a corresponding hydrogen defect complex reveal that a thermodynamic donor level associated with electron transfer from an H$^+$-Ti$^{3+}$ complex to the conduction band can form just below the conduction band minimum for realistic $U$ values. These findings suggest that the coexistence of delocalized and localized electrons can be realized in hydrogen-irradiated SrTiO$_3$ in electron-rich conditions.

Yuhki Kohsaka

We present a statistical method to remove background and estimate a unit height of atomic steps of an image obtained using a scanning probe microscope. We adopt a mixture model consisting of multiple statistical distributions to describe an image. This statistical approach provides a comprehensive way to subtract a background surface even in the presence of atomic steps as well as to evaluate terrace heights in a single framework. Moreover, it also enables us to extract further quantitative information by introducing additional prior knowledge about the image. An example of this extension is estimating a unit height of atomic steps together with the terrace heights. We demonstrate the capability of our method for a topographic image of a Cu(111) surface taken using a scanning tunneling microscope. The background subtraction corrects all terraces to be parallel to a horizontal plane and the precision of the estimated unit height reaches the order of a picometer. An open-source implementation of our method is available on the web.

Mikhail S. Storozhevykh, Larisa V. Arapkina, Sergey M. Novikov et al.

The method of software analysis of high-resolution TEM images using the peak pairs algorithm in combination with Raman spectroscopy was employed to study lattice deformations in Ge/Si(001) structures with low-temperature Ge quantum dots. It was found that the stresses do not spread in a thick Si layer above quantum dots, but completely relax via the formation of a thin boundary layer of mixed composition. However, intermixing of Ge and Si is absent beneath the Ge layer in samples with a Ge coverage of 10 Å. Besides intermixing was not observed at all, both beneath and above the Ge layer, in samples with a Ge coverage of 6 Å or less. This may be due to the predominance of Ge diffusion into the Si matrix from the {105} facets of Ge huts, not from the Ge wetting layer, at low temperatures of the Ge/Si structure deposition. The critical thickness of Si coverage at which the intense stress-induced diffusion takes place is determined to lie in the range from 5 to 8 nm.

Alessandro Colombo, Davide Emilio Galli, Liberato De Caro et al.

Coherent Diffractive Imaging is a lensless technique that allows imaging of matter at a spatial resolution not limited by lens aberrations. This technique exploits the measured diffraction pattern of a coherent beam scattered by periodic and non-periodic objects to retrieve spatial information. The diffracted intensity, for weak-scattering objects, is proportional to the modulus of the Fourier Transform of the object scattering function. Any phase information, needed to retrieve its scattering function, has to be retrieved by means of suitable algorithms. Here we present a new approach, based on a memetic algorithm, i.e. a hybrid genetic algorithm, to face the phase problem, which exploits the synergy of deterministic and stochastic optimization methods. The new approach has been tested on simulated data and applied to the phasing of transmission electron microscopy coherent electron diffraction data of a $\text{SrTiO}_\text{3}$ sample. We have been able to quantitatively retrieve the projected atomic potential, and also image the oxygen columns, which are not directly visible in the relevant high-resolution transmission electron microscopy images. Our approach proves to be a new powerful tool for the study of matter at atomic resolution and opens new perspectives in those applications in which effective phase retrieval is necessary.

J. Matsuno, N. Ogawa, K. Yasuda et al.

Electron transport coupled with magnetism has attracted attention over the years as exemplified in anomalous Hall effect due to a Berry phase in momentum space. Another type of unconventional Hall effect -- topological Hall effect, originating from the real-space Berry phase, has recently become of great importance in the context of magnetic skyrmions. We have observed topological Hall effect in bilayers consisting of ferromagnetic SrRuO$_3$ and paramagnetic SrIrO$_3$ over a wide region of both temperature and magnetic field. The topological term rapidly decreases with the thickness of SrRuO$_3$, ending up with the complete disappearance at 7 unit cells of SrRuO$_3$. Combined with model calculation, we concluded that the topological Hall effect is driven by interface Dzyaloshinskii-Moriya interaction, which is caused by both the broken inversion symmetry and the strong spin-orbit coupling of SrIrO$_3$. Such interaction is expected to realize the Néel-type magnetic skyrmion, of which size is estimated to be $\sim$10 nm from the magnitude of topological Hall resistivity. The results established that the high-quality oxide interface enables us to tune the chirality of the system; this can be a step towards the future topological electronics.

D. A. Zatsepin, D. W. Boukhvalov, E. Z. Kurmaev et al.

Systematic investigation of atomic structure of N-ion implanted TiO2 (thin films and bulk ceramics) was performed by XPS measurements (core levels and valence bands) and first-principles density functional theory (DFT) calculations. In bulk samples experiment and theory demonstrate anion N->O substitution. For the thin films case experiments evidence valuable contributions from N2 and NO molecule-like structures and theoretical modeling reveals a possibility of formation of these species as result of the appearance of interstitial nitrogen defects on the various surfaces of TiO2. Energetics of formation of oxygen vacancies and its key role for band gap reduction is also discussed.

Rémi Dingreville, Richard A. Karnesky, Guillaume Puel et al.

With the increasing interplay between experimental and computational approaches at multiple length scales, new research directions are emerging in materials science and computational mechanics. Such cooperative interactions find many applications in the development, characterization and design of complex material systems. This manuscript provides a broad and comprehensive overview of recent trends where predictive modeling capabilities are developed in conjunction with experiments and advanced characterization to gain a greater insight into structure-properties relationships and study various physical phenomena and mechanisms. The focus of this review is on the intersections of multiscale materials experiments and modeling relevant to the materials mechanics community. After a general discussion on the perspective from various communities, the article focuses on the latest experimental and theoretical opportunities. Emphasis is given to the role of experiments in multiscale models, including insights into how computations can be used as discovery tools for materials engineering, rather than to "simply" support experimental work. This is illustrated by examples from several application areas on structural materials. This manuscript ends with a discussion on some problems and open scientific questions that are being explored in order to advance this relatively new field of research.

H. Knuepfer, C. B. Muratov

We investigate the ground state of a uniaxial ferromagnetic plate with perpendicular easy axis and subject to an applied magnetic field normal to the plate. Our interest is the asymptotic behavior of the energy in macroscopically large samples near the saturation field. We establish the scaling of the critical value of the applied field strength below saturation at which the ground state changes from the uniform to a branched domain magnetization pattern and the leading order scaling behavior of the minimal energy. Furthermore, we derive a reduced sharp-interface energy giving the precise asymptotic behavior of the minimal energy in macroscopically large plates under a physically reasonable assumption of small deviations of the magnetization from the easy axis away from domain walls. On the basis of the reduced energy, and by a formal asymptotic analysis near the transition, we derive the precise asymptotic values of the critical field strength at which non-trivial minimizers (either local or global) emerge. The non-trivial minimal energy scaling is achieved by magnetization patterns consisting of long slender needle-like domains of magnetization opposing the applied field

Shu Nie, R. M. Feenstra

The 5x5, 6rt(3)x6rt(3)-R30deg, and graphene-covered 6rt(3)x6rt(3)-R30deg reconstructions of the SiC(0001) surface are studied by scanning tunneling microscopy and spectroscopy. For the 5x5 structure a rich spectrum of surface states is obtained, with one state in particular found to be localized on top of structural protrusions (adatoms) observed on the surface. Similar spectra are observed on the bare 6rt(3)x6rt(3)-R30deg reconstruction, and in both cases the spectra display nearly zero conductivity at the Fermi-level. When graphene covers the 6rt(3)x6rt(3)-R30deg surface the conductivity at the Fermi-level shows a marked increase, and additionally the various surface state peaks seen in the spectrum shift in energy and fall in intensity. The influence of the overlying graphene on the electronic properties of the interface is discussed, as are possible models for the interface structure.

I. G. Gurtubay, Wei Ku, J. M. Pitarke et al.

We present an all-electron study of the dynamical density-response function of hexagonal close-packed transition metals Sc and Ti. We elucidate various aspects of the interplay between the crystal structure and the electron dynamics by investigating the loss function, and the associated dielectric function, for wave-vector transfers perpendicular and parallel to the hexagonal plane. As expected, but contrary to recent work, we find that the free-electron-like aspects of the dynamical response are rather isotropic for small wave vectors. The crystal local-field effects are found to have an impact on the plasmon energy for small wave vectors, which gives rise to an interplay with the exchange-correlation effects built into the many-body kernel. The loss function lineshape shows a significant dependence on propagation direction; in particular, for propagation on the hexagonal plane the plasmon hybridizes substantially with fine structure due to d-electron transitions, and its dispersion curve becomes difficult to establish, beyond the small wave vector limit. The response is calculated in the framework of time-dependent density functional theory (TDDFT), based on a full-potential linearized augmented-plane-wave (LAPW) ground-state, in which the exchange-correlation effects are treated in the local-density approximation.

P. M. Echenique, J. Osma, M. Machado et al.

Theoretical investigations of surface-state electron dynamics in noble metals are reported. The dynamically screened interaction is computed, within many-body theory, by going beyond a free-electron description of the metal surface. Calculations of the inelastic linewidth of Shockley surface-state electrons and holes in these materials are also presented. While the linewidth of excited holes at the surface-state band edge (${\bf k}_\parallel=0$) is dominated by a two-dimensional decay channel, within the surface-state band itself, our calculations indicate that major contributions to the electron-electron interaction of surface-state electrons above the Fermi level come from the underlying bulk electrons.

Mathieu Bouville, Shenyang Hu, Long-Qing Chen et al.

Polycrystalline thin films can be unstable with respect to island formation (agglomeration) through grooving where grain boundaries intersect the free surface and/or thin film-substrate interface. We develop a phase-field model to study the evolution of the phases, composition, microstructure and morphology of such thin films. The phase-field model is quite general, describing compounds and solid solution alloys with sufficient freedom to choose solubilities, grain boundary and interface energies, and heats of segregation to all interfaces. We present analytical results which describe the interface profiles, with and without segregation, and confirm them using numerical simulations. We demonstrate that the present model accurately reproduces the theoretical grain boundary groove angles both at and far from equilibrium. As an example, we apply the phase-field model to the special case of a Ni(Pt)Si (Ni/Pt silicide) thin film on an initially flat silicon substrate.

D. E. Steinhauer, C. P. Vlahacos, F. C. Wellstood et al.

We describe the use of a near-field scanning microwave microscope to image the permittivity and tunability of bulk and thin film dielectric samples on a length scale of about 1 micron. The microscope is sensitive to the linear permittivity, as well as to nonlinear dielectric terms, which can be measured as a function of an applied electric field. We introduce a versatile finite element model for the system, which allows quantitative results to be obtained. We demonstrate use of the microscope at 7.2 GHz with a 370 nm thick barium strontium titanate thin film on a lanthanum aluminate substrate. This technique is nondestructive and has broadband (0.1-50 GHz) capability. The sensitivity of the microscope to changes in relative permittivity is 2 at permittivity = 500, while the nonlinear dielectric tunability sensitivity is 10^-3 cm/kV.

Karsten Reuter, Matthias Scheffler

We present density-functional theory calculations of Ru 3d and O 1s surface core-level shifts (SCLSs) at an oxygen-rich Ru(0001) surface, namely for the O(1x1)/Ru(0001) chemisorption phase and for two surface terminations of fully oxidized RuO_2(110). Including final-state effects, the computed SCLSs can be employed for the analysis of experimental X-ray photoelectron spectroscopy (XPS) data enabling a detailed study of the oxidation behaviour of the Ru(0001) surface. We show that certain peaks can be used as a fingerprint for the existence of the various phases and propose that the long disputed satellite peak in RuO_2(110) XPS data originates from a hitherto unaccounted surface termination.

V. A. Kulbachinskii, V. G. Kytin, A. V. Golikov et al.

The photoconductivity of GaAs structures delta-doped by Sn has been investigated for wavelengths lambda= 650-1200 nm in the temperature interval T= 4.2-300 K. The electron densities and mobilities, before and after illumination, have been determined by magnetoresistance, Shubnikov-de Haas effect and Hall effect measurements, in high magnetic fields. For the heavily doped structures (n_H> 2x10^13 cm^-2) we observe under illumination by light with wavelengths larger than the band-gap wavelength of the host material (lambda= 815 nm at T= 4.2 K) first positive (PPPC) and then negative (NPPC) persistent photoconductivity. The NPPC is attributed to the ionisation of DX centres and PPPC is explained by the excitation of electrons from Cr impurity states in the substrate. For lambda< 815 nm in addition the excitation of electron over the band gap of GaAs contributes to the PPPC. For the lightly doped structures (n_H<= 2x10^13 cm^-2) the photoconductivity effect is always positive.

P. L. de Andres, K. Reuter, F. J. Garcia-Vidal et al.

We analyze BEEM experiments. At low temperatures and low voltages, near the threshold value of the Schottky barrier, the BEEM current is dominated by the elastic component. Elastic scattering by the lattice results in the formation of focused beams and narrow lines in real space. To obtain the current injected in the semiconductor, we compute the current distribution in reciprocal space and, assuming energy and $k_{\parallel}$ conservation. Our results show an important focalization of the injected electron beam and explain the similarity between BEEM currents for Au/Si(111) and Au/Si(100).

Rene Messina, Michele Soucail, Ladislas Kubin

Abnormal grain growth in the presence of second phase particles is investigated with the help of a two-dimensional Monte Carlo simulation. An aggregate of equiaxed grains is considered with constant grain boundary energy and mobility. The only driving force accounted for stems from the grain boundary curvature. The process of abnormal grain growth is investigated as a function of two governing parameters, the initial degree of pinning of the matrix grains by the particles and the initial size advantage of the anomalous grain. In such conditions, moderate growth is obtained whose specific features are discussed with respect to the available models. It is shown that it is possible to obtain drastic grain growth by introducing the thermally activated unpinning of grain boundaries from particles. For this purpose, a simplified but effective procedure is proposed and discussed that includes the influence of the capillary force on the height of the local energy barrier for grain unpinning.

M. E. Gruner, P. Entel

We perform constant pressure Monte Carlo simulations of a spin-analogous model which describes coupled spatial and magnetic degrees of freedom on an fcc lattice. Our calculations qualitatively reproduce magnetovolume effects observed in some rare earth manganese compounds, especially in the anti-Invar material YMn2. These are a sudden collapse of the magnetic moment which is connected with a huge volume change, and a largely enhanced thermal expansion coefficient.

T. Makino, Y. Segawa, M. Kawasaki et al.

Recently the developments in the field of II-VI-oxides have been spectacular. Various epitaxial methods has been used to grow epitaxial ZnO layers. Not only epilayers but also sufficiently good-quality multiple quantum wells (MQWs) have also been grown by laser molecular-beam epitaxy (laser-MBE). We discuss mainly the experimental aspect of the optical properties of excitons in ZnO-based MQW heterostructures. Systematic temperature-dependent studies of optical absorption and photoluminescence in these MQWs were used to evaluate the well-width dependence and the composition dependence of the major excitonic properties. Based on these data, the localization of excitons, the influence of exciton-phonon interaction, and quantum-confined Stark effects are discussed. The optical spectra of dense excitonic systems are shown to be determined mainly by the interaction process between excitons and biexcitons. The high-density excitonic effects play a role for the observation of room-temperature stimulated emission in the ZnO MQWs. The binding energies of exciton and biexciton are enhanced from the bulk values, as a result of quantum-confinement effects.