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The significant advancements in perovskite solar cell (PSC) research and development have reignited optimism for the practicality of solar energy. A deeper comprehension of the fundamental mechanisms is essential for enhancing the current solar technology. Impedance spectroscopy (IS) characterization, in conjunction with other analytical methods, stands out as the primary approach for gaining insights into the internal workings of solar cells. The continuous analysis and refinement of electrochemical spectroscopy data for PSCs have unveiled intricate operational details. Despite the ongoing improvements, the absence of a centralized repository for this information poses challenges for tracking progress effectively. This review paper aims to consolidate the physical phenomena behind the development of PSC research, aiming to establish a comprehensive knowledge base on impedance plots, equivalent circuits, and related processes.

Coherence times of spin qubits in solid-state platforms are often limited by the presence of a spin bath. While some properties of these typically dark bath spins can be indirectly characterized via the central qubit, it is important to characterize their properties by direct measurement. Here we use pulsed electron paramagnetic resonance (pEPR) based Carr-Purcell-Meiboom-Gill (CPMG) dynamical decoupling to measure the magnetic noise power spectra for ensembles of P1 (substitutional nitrogen) centers in diamond that typically form the bath for NV (nitrogen-vacancy) centers. The experiments on the P1 centers were performed on a low [N] CVD (chemical vapor deposition) sample and a high [N] HPHT (high-temperature, high-pressure) sample at 89 mT. We characterize the NV centers of the latter sample using the same 2.5 GHz pEPR spectrometer. All power spectra show two distinct features, a broad component that is observed to scale as approximately $1/\omega^{0.7-1.0}$, and a prominent peak at the $^{13}$C Larmor frequency. The behavior of the broad component is consistent with an inhomogeneous distribution of Lorentzian spectra due to clustering of P1 centers, which has recently been shown to be prevalent in HPHT diamond. It is unknown if such clustering occurs in CVD diamond. We develop techniques utilizing harmonics of the CPMG filter function to improve characterization of high-frequency signals, which we demonstrate on the $^{13}$C nuclear Larmor frequency. At 190 mT this is 2.04 MHz, 5.7 times higher than the CPMG modulation frequency ($<357$ kHz, hardware-limited). We assess the robustness of our methods in the presence of finite pulse widths and flip angle errors. Understanding the interactions of dark spins will inform methods of diamond fabrication for quantum technology. These techniques are applicable to ac magnetometry for nanoscale nuclear magnetic resonance and chemical sensing., Comment: 55 pages, 21 figures

Dynamic nuclear polarization (DNP) is a method of enhancing NMR signals via the transfer of polarization from electron spins to nuclear spins using on-resonance microwave (MW) irradiation. In most cases, monochromatic continuous-wave (MCW) MW irradiation is used. Recently, several groups have shown that the use of frequency modulation of the MW irradiation can result in an additional increase in DNP enhancement above that obtained with MCW. The effect of frequency modulation on the solid effect (SE) and the cross effect (CE) has previously been studied using the stable organic radical 4-hydroxy TEMPO (TEMPOL) at temperatures under 20 K. Here, in addition to the SE and CE, we discuss the effect of frequency modulation on the Overhauser effect (OE) and the truncated CE (tCE) in the room-temperature $^{13}$C-DNP of diamond powders. We recently showed that diamond powders can exhibit multiple DNP mechanisms simultaneously due to the heterogeneity of P1 (substitutional nitrogen) environments within diamond crystallites. We explore the enhancement obtained via the two most important parameters for frequency modulation 1) Modulation frequency, $f_{m}$ (how fast the modulation frequency is varied) and 2) Modulation amplitude, $\Delta\omega$ (the magnitude of the change in microwave frequency) influence the enhancement obtained via each mechanism. Frequency modulation during DNP not only allows us to improve DNP enhancement, but also gives us a way to control which DNP mechanism is most active. By choosing the appropriate modulation parameters, we can selectively enhance some mechanisms while simultaneously suppressing others.

We use microwave-induced dynamic nuclear polarization (DNP) of the substitutional nitrogen defects (P1 centers) in diamond to hyperpolarize bulk $^{13}$C nuclei in both single crystal and powder samples at room temperature at 3.34 T. The large ($>100$-fold) enhancements demonstrated correspond to a greater than 10,000 fold improvement in terms of signal averaging of the 1\% abundant $^{13}$C spins. The DNP was performed using low-power solid state sources under static (non-spinning) conditions. The DNP spectrum (DNP enhancement as a function of microwave frequency) of diamond powder shows features that broadly correlate with the EPR spectrum. A well-defined negative Overhauser peak and two solid effect peaks are observed for the central ($m_I=0$) manifold of the $^{14}$N spins. Previous low temperature measurements in diamond had measured a positive Overhauser enhancement in this manifold. Frequency-chirped millimeter-wave excitation of the electron spins is seen to significantly improve the enhancements for the two outer nuclear spin manifolds ($m_I = \pm 1$) and to blur some of the sharper features associated with the central manifolds. The outer lines are best fit using a combination of the cross effect and a truncated cross effect -- which is known to mimic features of an Overhauser effect. Similar features are also observed in experiments on single crystal samples. The observation of all of these mechanisms in a single material system under the same experimental conditions is likely due to the significant heterogeneity of the high pressure, high temperature (HPHT) type Ib diamond samples used. Large room temperature DNP enhancements at fields above a few Tesla enable spectroscopic studies with better chemical shift resolution under ambient conditions.

Microstructures, i.e., architected materials, are designed today, typically, by maximizing an objective, such as bulk modulus, subject to a volume constraint. However, in many applications, it is often more appropriate to impose constraints on other physical quantities of interest. In this paper, we consider such generalized microstructural optimization problems where any of the microstructural quantities, namely, bulk, shear, Poisson ratio, or volume, can serve as the objective, while the remaining can serve as constraints. In particular, we propose here a neural-network (NN) framework to solve such problems. The framework relies on the classic density formulation of microstructural optimization, but the density field is represented through the NN's weights and biases. The main characteristics of the proposed NN framework are: (1) it supports automatic differentiation, eliminating the need for manual sensitivity derivations, (2) smoothing filters are not required due to implicit filtering, (3) the framework can be easily extended to multiple-materials, and (4) a high-resolution microstructural topology can be recovered through a simple post-processing step. The framework is illustrated through a variety of microstructural optimization problems.

Annealing of crystalline multilayers composed of two miscible elements usually causes interfacial mixing of the constituent atoms, possibly leading to the formation of binary alloys at the interfaces. Magnetron sputtered c-Ni/a-Zr multilayers deposited at room temperature were vacuum annealed isochronally at 200degC and 400degC to observe thermal stability of the interfaces constituting the crystalline/amorphous multilayers. Control over the interfacial behaviour can aid the formation of materials with novel properties. The resultant changes in structural and magnetic properties of the multilayers were investigated in detail through X-ray Reflectivity, Polarized Neutron Reflectivity, SIMS and SQUID-based magnetization measurement techniques. The compositional variations in the amorphous mixed layers formed at the Ni-on-Zr and Zr-on-Ni interfaces due to atomic transport, were carefully observed as a function of annealing. Interface widths proceeded to increase with annealing at the expense of the Ni and Zr layers. The Ni-on-Zr interface was seen to be unstable at both temperatures; but the overall response of the interfaces to atomic diffusion was more pronounced when the multilayers were annealed at 400degC. Under conditions of supersaturation of atoms within restricted spaces of the interfacial layers and the limited availability of components within the multilayer, unexpected demixing effects were observed at both the interfaces. A large increase in magnetic moment obtained after annealing at 400degC, was attributed to the high densification of the Ni layers as well as to the incorporation of Ni crystallites into the Zr-on-Ni interface layers.

Monophasic and homogeneous Ni10Zr7 nanocrystalline alloy films were successfully grown at room temperature by co-sputtering in an indigenously developed three-gun DC/RF magnetron sputtering unit. The films could be produced with long-range crystallographic and chemical order in the alloy, thus overcoming the widely acknowledged inherent proclivity of the glass forming Ni-Zr couple towards amorphization. Crystallinity of these alloys is a desirable feature with regard to improved efficacy in applications such as hydrogen storage, catalytic activity and nuclear reactor engineering, to name a few. Thermal stability of this crystalline phase, being vital for transition to viable applications, was investigated through systematic annealing of the alloy films at 473 K, 673 K and 923 K for various durations. While the films were stable at 473 K, the effect of annealing at 673 K was to create segregation into nanocrystalline Ni (superparamagnetic) and amorphous Ni+Zr (non-magnetic) phases. Detailed analyses of the physical and magnetic structures before and after annealing were performed through several techniques effectual in analyzing stratified configurations and the findings were all consistent with each other. Polarized neutron and X-ray reflectometry, grazing incidence x-ray diffraction, time-of-flight secondary ion mass spectroscopy and X-ray photoelectron spectroscopy were used to gauge phase separation at nanometer length scales. SQUID based magnetometry was used to investigate macroscopic magnetic properties. Simulated annealing performed on this system using molecular dynamic calculations corroborated well with the experimental results. This study provides a thorough understanding of the creation and thermal evolution of a crystalline Ni-Zr alloy.

The investigation of devitrification in thermally annealed nanodimensional glassy alloy thin films provides a comprehensive understanding of their thermal stability, which can be used to explore potential applications. The amorphous to crystalline polymorphous transformation of cosputtered NiZr alloy (Ni78Zr22 at%) films, with a thickness lower than the reported critical limit of devitrification, was studied through detailed structural characterization and molecular dynamics (MD) simulations. Devitrification to a nanocrystalline state (Ni7Zr2 structure) was observed at 800 degC, with an increase in density (approx 3.6%) much higher than that achieved in bulk alloys. Variation in the magnetic property of the films and the overall physical structure including morphology and composition were examined before and after annealing. MD simulations were employed to effectively elucidate not only the high densification but also the increased magnetic moment after annealing, which was correlated with the simulated change in the coordination number around Ni atoms. The structural relaxation process accompanying devitrification was described as a disorder-to-order transformation while highlighting the crucial role played by chemical short range order prevalent in glassy materials.

Heavy metal-ferromagnet bilayer structures have attracted great research interest for charge-to-spin interconversion. In this work, we have investigated the effect of the permalloy seed layer on the Ta polycrystalline phase and its spin Hall angle. Interestingly, for the same deposition rates the crystalline phase of Ta deposited on Py seed layer strongly depends on the thickness of the seed layer. We have observed a phase transition from $\alpha$-Ta to ($\alpha$+$\beta$)-Ta while increasing the Py seed layer thickness. The observed phase transition is attributed to the strain at interface between Py and Ta layers. Ferromagnetic resonance-based spin pumping studies reveal that the spin-mixing conductance in the to ($\alpha$+$\beta$)-Ta is relatively higher as compared to the to $\alpha$-Ta. Spin Hall angles of to $\alpha$-Ta and to ($\alpha$+$\beta$)-Ta are extracted from inverse spin Hall effect (ISHE) measurements. Spin Hall angle of the to ($\alpha$+$\beta$)-Ta is estimated to be $\theta$_SH=-0.15 which is relatively higher than that of to $\alpha$-Ta. Our systematic results connecting the phase of the Ta with seed layer and its effect on the efficiency of spin to charge conversion might resolve ambiguities across various literature and open up new functionalities based on the growth process for the emerging spintronic devices., Comment: 24 Pages, 5 figures

The magnetic glassy state is a fascinating phenomenon, which results from the kinetic arrest of the first order magnetic phase transition. Interesting properties, such as metastable magnetization and nonequilibrium magnetic phases, are naturally developed in the magnetic glassy state. Here, we report magnetic glass property in the low spin state of Co3+ in EuBaCo2O5+{\delta} ({\delta} = 0.47) cobaltite at low temperature (T < 60 K). The measurements of magnetization under the cooling and heating in unequal fields, magnetization relaxation and thermal cycling of magnetization show the kinetic arrest of low magnetization state below 60 K. The kinetically arrested low temperature magnetic phase is further supported through the study of isothermal magnetic entropy, which shows the significant entropy change. The present results will open a new window to search the microscopic relation between the spin state transitions and the kinetic arrest induced magnetic glassy phenomena in complex materials.

Skyrmion racetrack memory has a lots of potential in future non-volatile solid state devices. In general such devices require current to nucleate skyrmions via spin transfer torque (STT) effect. Further the current is also required to drive the skyrmions in the nanowire device. However the current applied during nucleation of successive skyrmions may have unwanted perturbation \emph{viz.} Joule heating and skyrmion Hall effect, on the propagation of previously generated skyrmions. Therefore new methodology is required to decouple the generation and propagation of skyrmions. Here we present a novel route via micromagnetic simulation for generation of skyrmions from triangular antidot structure in a ferromagnetic nanotrack using local oersted field. Antidots are holes in a magnetic nanoelement. Controlled skyrmion injection can be achieved by tuning the dimensions of the antidots that are placed at either end of the nanotrack. Multiple skyrmions can be simultaneously generated by incorporating more number of antidots. Here we propose a novel design to realise skyrmionic racetrcak memory where one can individually generate and manipulate the skyrmions within the nanotrack.

Dynamic nuclear polarization (DNP) enhanced nuclear magnetic resonance (NMR) offers a promising route to studying local atomic environments at the surface of both crystalline and amorphous materials. We take advantage of unpaired electrons due to defects close to the surface of the silicon microparticles to hyperpolarize adjacent $^{1}$H nuclei. At 3.3 T and 4.2 K, we observe the presence of two proton peaks, each with a linewidth on the order of 5 kHz. Echo experiments indicate a homogeneous linewidth of $\sim 150-300$ Hz for both peaks, indicative of a sparse distribution of protons in both environments. The downfield peak at 10 ppm lies within the typical chemical shift range for proton NMR, and was found to be relatively stable over repeated measurements. The upfield peak was found to vary in position between -19 and -37 ppm, well outside the range of typical proton NMR shifts, and indicative of a high-degree of chemical shielding. The upfield peak was also found to vary significantly in intensity across different experimental runs, suggesting a weakly-bound species. These results suggest that the hydrogen is located in two distinct microscopic environments on the surface of these Si particles.

A fast and accurate predictive tool for polymer properties is demanding and will pave the way to iterative inverse design. In this work, we apply graph convolutional neural networks (GCNN) to predict the dielectric constant and energy bandgap of polymers. Using density functional theory (DFT) calculated properties as the ground truth, GCNN can achieve remarkable agreement with DFT results. Moreover, we show that GCNN outperforms other machine learning algorithms. Our work proves that GCNN relies only on morphological data of polymers and removes the requirement for complicated hand-crafted descriptors, while still offering accuracy in fast predictions., Comment: Accepted for NIPS 2018 Workshop on Machine Learning for Molecules and Materials

We introduce the use of Crystal Graph Convolutional Neural Networks (CGCNN), Fully Connected Neural Networks (FCNN) and XGBoost to predict thermoelectric properties. The dataset for the CGCNN is independent of Density Functional Theory (DFT) and only relies on the crystal and atomic information, while that for the FCNN is based on a rich attribute list mined from Materialsproject.org. The results show that the optimized FCNN is three layer deep and is able to predict the scattering-time independent thermoelectric powerfactor much better than the CGCNN (or XGBoost), suggesting that bonding and density of states descriptors informed from materials science knowledge obtained partially from DFT are vital to predict functional properties.

Successful materials innovations can transform society. However, materials research often involves long timelines and low success probabilities, dissuading investors who have expectations of shorter times from bench to business. A combination of emergent technologies could accelerate the pace of novel materials development by 10x or more, aligning the timelines of stakeholders (investors and researchers), markets, and the environment, while increasing return-on-investment. First, tool automation enables rapid experimental testing of candidate materials. Second, high-throughput computing (HPC) concentrates experimental bandwidth on promising compounds by predicting and inferring bulk, interface, and defect-related properties. Third, machine learning connects the former two, where experimental outputs automatically refine theory and help define next experiments. We describe state-of-the-art attempts to realize this vision and identify resource gaps. We posit that over the coming decade, this combination of tools will transform the way we perform materials research. There are considerable first-mover advantages at stake, especially for grand challenges in energy and related fields, including computing, healthcare, urbanization, water, food, and the environment., Comment: 22 pages, 3 figures

We use dynamic nuclear polarization (DNP) enhanced nuclear magnetic resonance (NMR) at liquid helium temperatures to directly detect hydrogen attached to the surface of silicon microparticles. The proton NMR spectrum from a dry sample of polycrystalline silicon powder (1-5 $\mu$m) shows a distinctively narrow Lorentzian-shaped resonance with a width of 6.2 kHz, indicative of a very sparse distribution of protons attached to the silicon surface. These protons are within a few atomic monolayers of the silicon surface. The high sensitivity NMR detection of surface protons from low surface area ($0.26 - 1.3 \: m^2/g$) particles is enabled by an overall signal enhancement of 4150 over the room temperature NMR signal at the same field. When the particles were suspended in a solvent with 80% H2O and 20% D2O, the narrow peak was observed to grow in intensity over time, indicating growth of the sparse surface proton layer. However, when the particles were suspended in a solvent with 20% H2O and 80% D2O, the narrow bound-proton peak was observed to shrink due to exchange between the surface protons and the deuterium in solution. This decrease was accompanied by a concomitant growth in the intensity of the frozen solvent peak, as the relative proton concentration of the solvent increased. When the particles were suspended in the organic solvent hexane, the proton NMR spectra remained unchanged over time. These results are consistent with the known chemisorption of water on the silicon surface resulting in the formation of hydride and hydroxyl species. Low-temperature DNP NMR can thus be used as a non-destructive probe of surface corrosion for silicon in aqueous environments. This is important in the context of using silicon MEMS and bioMEMS devices in such environments, for silicon micro- and nano-particle MRI imaging agents, and the use of nanosilicon for splitting water in fuel cells.

Structural, impedance, ferroelectric and magnetic properties were examined in multiferroic Bi_{2}Fe_{4(1-x)}Co_{4x}O_{9} (0$\leq$x$\leq$0.02) ceramics synthesized via solid-state reaction method. X-ray diffraction analysis and Rietveld refinement showed secondary phase formation (for x$\geq$0.01) which was subsequently confirmed from room temperature Raman spectroscopy study. The frequency dependence of impedance and electric modulus of the material showed the presence of non-Debye type relaxation in all the samples. The values of the activation energies calculated from imaginary impedance and modulus lie in the range of 0.92-0.99 eV which confirmed that the oxygen vacancies play an important role in the conduction mechanism. Moreover, suitable amount of Co substitution significantly enhanced the remnant polarisation (2P_{r}) from 0.1193 $\mu$C/cm^{2} (x=0) to 0.2776 $\mu$C/cm^{2} (x=0.02). Besides, room temperature M-H measurement showed improved ferromagnetic hysteresis loop for all the modified samples. The remnant magnetization (M_{r}) and coercive field (H_{c}) increased from 0.0007 emu/gm and 42 Oe for x=0 to 0.1401 emu/gm and 296 Oe for x=0.02. The improved ferroelectricity was due to Co 3d-O 2p hybridization and enhanced magnetization originated from the partial substitution of Co^{3+} ions leading to breakdown of balance between the anti-parallel sub lattice magnetization of Fe^{3+} ions.

The conducting gas that forms at the interface between LaAlO$_3$ and SrTiO$_3$ has proven to be a fertile playground for a wide variety of physical phenomena. The bulk of previous research has focused on the (001) and (110) crystal orientations. Here we report detailed measurements of the low-temperature electrical properties of (111) LAO/STO interface samples. We find that the low-temperature electrical transport properties are highly anisotropic, in that they differ significantly along two mutually orthogonal crystal orientations at the interface. While anisotropy in the resistivity has been reported in some (001) samples and in (110) samples, the anisotropy in the (111) samples reported here is much stronger, and also manifests itself in the Hall coefficient as well as the capacitance. In addition, the anisotropy is not present at room temperature and at liquid nitrogen temperatures, but only at liquid helium temperatures and below. The anisotropy is accentuated by exposure to ultraviolet light, which disproportionately affects transport along one surface crystal direction. Furthermore, analysis of the low-temperature Hall coefficient and the capacitance as a function of back gate voltage indicates that in addition to electrons, holes contribute to the electrical transport., Comment: 11 pages, 9 figures

Magnetic-field and microwave-frequency modulated DNP experiments have been shown to yield improved enhancements over conventional DNP techniques, and even to shorten polarization build-up times. The resulting increase in signal-to-noise ratios can lead to significantly shorter acquisition times in signal-limited multi-dimensional NMR experiments and pave the way to the study of even smaller sample volumes. In this paper we describe the design and performance of a broadband system for microwave frequency- and amplitude-modulated DNP that has been engineered to minimize both microwave and thermal losses during operation at liquid helium temperatures. The system incorporates a flexible source that can generate arbitrary waveforms at 94 GHz with a bandwidth greater than 1 GHz, as well as a probe that efficiently transmits the millimeter waves from room temperature outside the magnet to a cryogenic environment inside the magnet. Using a thin-walled brass tube as an overmoded waveguide to transmit a hybrid HE11 mode, it is possible to limit the losses to 1 dB across a 2 GHz bandwidth. The loss is dominated by the presence of a quartz window used to isolate the waveguide pipe. This performance is comparable to systems with corrugated waveguide or quasi-optical components. The overall excitation bandwidth of the probe is seen to be primarily determined by the final antenna or resonator used to excite the sample and its coupling to the NMR RF coil. Understanding the instrumental limitations imposed on any modulation scheme is key to understanding the observed DNP results and potentially identifying the underlying mechanisms. We demonstrate the utility of our design with a set of triangular frequency-modulated DNP experiments.

We have investigated magnetocaloric effect in double perovskite Gd2NiMnO6 (GNMO) and Gd2CoMnO6 (GCMO) samples by magnetic and heat capacity measurements. Ferromagnetic ordering is observed at ~130 K (~112 K) in GNMO (GCMO), while the Gd exchange interactions seem to dominate for T < 20 K. In GCMO, below 50 K, an antiferromagnetic behaviour due to 3d-4f exchnage interaction is observed. A maximum entropy (-{\Delta}SM) and adiabatic temperature change of ~35.5 J Kg-1 K-1 (~24 J Kg-1 K-1) and 10.5 K (6.5 K) is observed in GNMO (GCMO) for a magnetic field change of 7 T at low temperatures. Absence of magnetic and thermal hysteresis and their insulating nature make them promising for low temperature magnetic refrigeration.

Doping at the rare-earth site by divalent alkaline-earth ions in perovskite lattice has witnessed a variety of magnetic and electronic orders with spatially correlated charge, spin and orbital degrees of freedom. Here, we report an antisite disorder driven spontaneous exchange bias effect as a result of hole carrier (Sr2+) doping in La2-xSrxCoMnO6 (0 < x < 1) double perovskites. X-ray diffraction and Raman spectroscopy have evidenced an increase in disorder with the increase of Sr content up to x = 0.5 and thereby decreases from x = 0.5 to 1. X-ray absorption spectroscopy has revealed that only Co is present in mixed valent Co2+ and Co3+ states with Sr doping to compensate the charge neutrality. Magnetotransport is strongly correlated with the increase of antisite disorder. The antisite disorder at the B-site interrupts the long-range ferromagnetic order by introducing various magnetic interactions and instigates reentrant glassy dynamics, phase separation and canted type antiferromagnetic behavior with the decrease of temperature. This leads to novel magnetic microstructure with unidirectional anisotropy that causes spontaneous exchange bias effect that can be tuned with the amount of antisite disorder., Comment: 22 pages, 9 figs

We present a large magnetodielectric (MD) effect of 65 % at 100 kHz with 5 T field in B-site ordered La2CoMnO6 (LCMO) polycrystalline sample. Frequency and temperature dependent impedance and dielectric studies under magnetic field divulge both intrinsic and extrinsic origins for the observed MD effect. The temperature dependent Raman spectroscopy measurement has shown spin-lattice coupling that supports the intrinsic origin of the observed large MD response in LCMO. Extrinsic contributions to MD response mainly originate from disorder and interface effects; here, we signify this by hole carrier (Sr) doping at the A-site of the ordered LCMO sample. The comparison study has disclosed that with the disorder, the intrinsic polarization due to asymmetric hopping decreases significantly, and the disorder induced transport dominates in both MD and magnetoresistance behaviour with close resemblance., Comment: 11 pages, 7 figs

We present sharp magnetization jumps and field induced irreversibility in magnetization in multiferroic Y2CoMnO6. Appearance of magnetic relaxation and field sweep rate dependence of magnetization jumps resemble the martensite like scenario and suggests the coexistence of E*-type antiferromagnetic and ferromagnetic phases at low temperatures. In Y2CoMnO6, the critical field required for the sharp jump can be increased or decreased depening on the magnitude and direction of the cooling field; this is remarkably different from manganites or other metamagnetic materials where the critical field increases irrespective of the direction of the field cooling. The cooling field dependence on the sharp magnetization jumps has been described by considering exchange pinning mechanism at the interface, like in exchange bias model.

Evidence of coexistence of Co3+ with Co2+ in ceramic Co3TeO6 through XANES, DC magnetization and first principal studies is provided. XANES along with linear combination fit provide relative concentrations of Co2+ and Co3+.Temperature dependent DC magnetization exhibits the same antiferromagnetic behavior as observed in single crystal. The presence of both Co2+ and Co3+ suggests that if the later is in high spin state, the effective magnetic moment is similar to that observed in single crystal studies. In contrast, if Co3+ is in low spin state effective magnetic moment is similar to that observed in Co3O4. It is further shown that both Co2+ and Co3+ in high spin states constitute a favorable ground state through first principle calculations where Rietveld refined Synchrotron X-ray diffraction data are inputs., Comment: 21 pages including 4 figures and a table

We present studies of the photoluminescence (PL), absorption and Raman scattering from poly[2,7-(9,9'-bis(2-ethylhexyl))fluorene] under hydrostatic pressures of 0-100 kbar at room temperature. The well-defined PL and associated vibronics that are observed at atmospheric pressure change dramatically around 20 kbar in the bulk sample and at around 35 kbar for the thin film sample. Beyond these pressures the PL emission from the backbone is swamped by strong peaks due to aggregates and keto defects in the 2.1-2.6 eV region. The Raman peaks shift to higher energies and exhibit unexpected antiresonance lineshapes at higher pressures, indicating a strong electron-phonon interaction., Comment: 9 pages, 9 figures

We present photoluminescence studies as a function of temperature from a series of conjugated polymers and a conjugated molecule with distinctly different backbone conformations. The organic materials investigated here are: planar methylated ladder type poly para-phenylene, semi-planar polyfluorene, and non-planar para hexaphenyl. In the longer-chain polymers the photoluminescence transition energies blue shift with increasing temperatures. The conjugated molecules, on the other hand, red shift their transition energies with increasing temperatures. Empirical models that explain the temperature dependence of the band gap energies in inorganic semiconductors can be extended to explain the temperature dependence of the transition energies in conjugated molecules., Comment: 8 pages, 9 figures

The concept of duality has proved extremely powerful in extending our understanding in many areas of physics (1, 2). Charge-vortex duality has been proposed (3, 4) as a model to understand the superconductor to insulator transition (SIT) in disordered thin films (5, 6) and Josephson junction arrays (7, 8, 9). In this model, on the superconducting side, one has delocalized Cooper pairs but localized vortices; while on the insulating side, one has localized Cooper pairs but mobile vortices. Here we show a new experimental manifestation of this duality in the electron gas that forms at the interface between LaAlO$_3$ (LAO) and SrTiO$_3$ (STO) (10, 11, 12, 13, 14). The effect is due to the motion of vortices generated by the magnetization dynamics of the ferromagnet that also forms at the same interface (14, 15, 16), which results in an increase in resistance on the superconducting side of the transition, but an increase in conductance on the insulating side., Comment: 25 pages, 4 figures, 6 supplementary figures

We have studied the magnetic field effect on low frequency dielectric properties of Pr0.6Ca0.4MnO3/polyvinylidene fluoride nanocomposite with 22.5% volume fraction of Pr0.6Ca0.4MnO3 nanoparticles. A strong magnetodielectric response was observed below 120 K where Pr0.6Ca0.4MnO3 nanoparticles show the magnetic phase transition indicating a direct correlation between magnetism and dielectric properties. A large change of the dielectric permittivity ~ 30% has been observed in a magnetic field of 4.6 T with loss as low as 0.17 at 70 K. The observed magnetodielectric response has been attributed to the decrement of polaron activation barrier of Pr0.6Ca0.4MnO3 nanoparticles with the increase of magnetic field., Comment: APL (2010)

Ferromagnetism is usually considered to be incompatible with conventional superconductivity, as it destroys the singlet correlations responsible for the pairing interaction. Superconductivity and ferromagnetism are known to coexist in only a few bulk rare-earth materials. Here we report evidence for their coexistence in a two-dimensional system: the interface between two bulk insulators, LaAlO$_3$ (LAO) and SrTiO$_3$ (STO), a system that has been studied intensively recently. Magnetoresistance, Hall and electric-field dependence measurements suggest that there are two distinct bands of charge carriers that contribute to the interface conductivity. The sensitivity of properties of the interface to an electric field make this a fascinating system for the study of the interplay between superconductivity and magnetism., Comment: 4 pages, 4 figures

Thick, high quality 4H-SiC epilayers have been grown in a vertical hot-wall chemical vapor deposition system at a high growth rate on (0001) 80 off-axis substrates. We discuss the use of dichlorosilane as the Si-precursor for 4H-SiC epitaxial growth as it provides the most direct decomposition route into SiCl2, which is the predominant growth species in chlorinated chemistries. A specular surface morphology was attained by limiting the hydrogen etch rate until the system was equilibrated at the desired growth temperature. The RMS roughness of the grown films ranged from 0.5-2.0 nm with very few morphological defects (carrots, triangular defects, etc.) being introduced, while enabling growth rates of 30-100 \mum/hr, 5-15 times higher than most conventional growths. Site-competition epitaxy was observed over a wide range of C/Si ratios, with doping concentrations < 1x1014 cm-3 being recorded. X-ray rocking curves indicated that the epilayers were of high crystallinity, with linewidths as narrow as 7.8 arcsec being observed, while microwave photoconductive decay (\muPCD) measurements indicated that these films had high injection (ambipolar) carrier lifetimes in the range of 2 \mus.

We report a process to fabricate carbon nanotubes (CNT) by chemical vapor deposition at predetermined location. This process was enabled by patterning catalyst nanoparticles directly on silicon substrates with nanometer-scale precision using Dip Pen Nanolithography(R) (DPN(R)). A multi-pen writing method was employed to increase the patterning rate. The development of new molecular inks for the deposition of the precursor catalyst resulted in a high yield of isolated carbon nanotubes, ideal for subsequent device fabrication. Here, we demonstrate the advantages of the new method for producing high quality isolated CNT in scalable array geometries., Comment: 17 pages and 4 figures, 6 page supporting information and 4 supporting figures. (Cover article)

We demonstrate a novel method allowing the study of the magnetic state dynamics of a single nanoparticle by means of electron transport measurements. Elliptical 550 nm x 240 nm permalloy nanoparticles are wired with non-magnetic leads for magnetotransport measurements in the presence of a radio-frequency (RF) field. Their resistance exhibits sharp jumps due to the anisotropic magnetoresistance even at room temperature. An RF field induces DC voltage across the nanoparticle which can be partially depleted at a certain RF frequency when a magnetic vortex core resonance is present. An application of an additional DC magnetic field eliminates the vortex and reinstates the unperturbed DC voltage level. The vortex core resonance frequencies are found and the smallest resonance widths are estimated to be less than 6 MHz.

We investigated the rare-earth transition metal oxide series, Ln2CuTiO6 (Ln=Y, Dy, Ho, Er and Yb), crystallizing in the hexagonal structure with non-centrosymmetric P63cm space group for possible occurrences of multiferroic properties. Our results show that while these compounds, except Ln=Y, exhibit a low temperature antiferromagnetic transition due to the ordering of the rare-earth moments, the expected ferroelectric transition is frustrated by the large size difference between Cu and Ti at the B-site. Interestingly, this leads these compounds to attain a rare and unique combination of desirable paraelectric properties with high dielectric constants, low losses and weak temperature and frequency dependencies. First-principles calculations establish these exceptional properties result from a combination of two effects. A significant difference in the MO5 polyhedral sizes for M = Cu and M = Ti suppress the expected co-operative tilt pattern of these polyhedra, required for the ferroelectric transition, leading to relatively large values of the dielectric constant for every compound investigated in this series. Additionally, it is shown that the majority contribution to the dielectric constant arises from intermediate-frequency polar vibrational modes, making it relatively stable against any temperature variation. Changes in the temperature stability of the dielectric constant amongst different members of this series are shown to arise from changes in relative contributions from soft polar modes., Comment: Accepted for publication in Phys. Rev. B (21 pages, 2 Table, 8 Figures)

Based on the assumption that the contact barrier height determines the current flow in organic semiconductor-based electronic devices, charge injection at metal-organic (MO) interfaces has been extensively investigated, while space-charge conduction in organic bulk is generally overlooked. Recent theoretical modeling and simulation have pointed out that such a simplification is questionable due to the hopping nature of charge injection and hopping-related space-charge conduction. Here we show experimentally that charge transport in metal-organic diodes is complex interplay between injection-limited current (ILC) and space-charge-limited current (SCLC). We report the experimental observation of ILC-to-SCLC transition in Ag/pentacene/Ag diodes as a function of temperature.

Polyfluorenes (PFs) represent a unique class of poly para-phenylene based blue-emitting polymers with intriguing structure-property relationships. Slight variations in the choice of functionalizing side chains result in dramatic differences in the inter- and intra-chain structures in PFs. We present photoluminescence (PL) and Raman scattering studies of bulk samples and thin films of dioctyl-substituted PF (PF8) under hydrostatic pressure. The bulk sample was further thermally annealed at 1.9 GPa. The PL vibronics of the as-is sample red-shift at an average rate of 26 meV/GPa. The thermally annealed sample is characterized by at least two phase transitions at 1.1 GPa and 4.2 GPa, each of which has a different pressure coefficient for PL vibronics. The Huang-Rhys factor, a measure of the electron-phonon interaction, is found to increase with increasing pressures signaling a higher geometric relaxation of the electronic states. The Raman peaks harden with increasing pressures; the intra-ring C-C stretch frequency at 1600 cm$^{-1}$ has a pressure coefficient of 7.2 cm$^{-1}$/GPa and exhibits asymmetric line shapes at higher pressures, characteristic of a strong electron-phonon interaction. The optical properties of PF8 under high pressure are further contrasted with those of a branched side chain substituted PF., Comment: 22 pages, 10 figures

Single crystal silicon is an excellent system in which to explore dynamic nuclear polarization (DNP), as it exhibits a continuum of properties from metallic to insulating as a function of doping concentration and temperature. At low doping concentrations DNP has been observed to occur via the solid effect, while at very high doping concentrations an Overhauser mechanism is responsible. Here we report the hyperpolarization of 29Si in n-doped silicon crystals, with doping concentrations in the range of 1-3 x 10^17 /cc. In this regime exchange interactions between donors become extremely important. The sign of the enhancement in our experiments and its frequency dependence suggest that the 29Si spins are directly polarized by donor electrons via an Overhauser mechanism within exchange-coupled donor clusters. The exchange interaction between donors only needs to be larger than the silicon hyperfine interaction (typically much smaller than the donor hyperfine coupling) to enable this Overhauser mechanism. Nuclear polarization enhancement is observed for a range of donor clusters in which the exchange energy is comparable to the donor hyperfine interaction. The DNP dynamics are characterized by a single exponential time constant that depends on the microwave power, indicating that the Overhauser mechanism is the rate-limiting step. Since only about 2 % of the silicon nuclei are located within one Bohr radius of the donor electron, nuclear spin diffusion is important in transferring the polarization to all the spins. However, the spin-diffusion time is much shorter than the Overhauser time due to the relatively weak silicon hyperfine coupling strength. In a 2.35 T magnetic field at 1.1 K, we observed a DNP enhancement of $244 +/- 84 resulting in a silicon polarization of $10.4 +/- 3.4 % following two hours of microwave irradiation., Comment: expanded and extensively modified, 20 pages, 7 figures

Ferromagnetic ordering is reported in the post-annealed samples of Co doped n-GaN formed by Co+ implantation. A maximum Curie temperature ~ 250K is recorded for the sample with 8 atomic percent Co. Particle induced x-ray emission-channeling study confirmed the substitutional Co in Ga lattice site. Local atomic arrangement around magnetic impurities is also analyzed using Raman study. A disordered model with carrier mediated coupling of localized magnetic moments is made responsible for the observed ferromagnetic ordering., Comment: 11 pages, 3 figures, Journal

Magnetization reversal (switching) using either r.f. fields or brute-force precessional switching is currently thought to ultimately be limited by the non-linear excitation of non-uniform spin waves, the so-called Suhl instability. Here we show (numerically, for the case of a sphere) that this instability can be suppressed by choosing the applied field and/or sphere diameter in such a way that the frequencies of the modes that can be excited through non-linear processes are off-resonance. While the results cannot be explained by a traditional model based on plane waves, they can be understood by projecting the actual state onto the small amplitude spin resonant eigenfunctions.

Precise arrays of sub-100 nm diameter nanodots are fabricated from magnetic oxide perovskites with the total coverage area up to 5 mm2. Epitaxial single crystal structure of the nanodots is demonstrated by cross-sectional TEM. Low temperature MFM study confirmed the ferromagnetism of the produced particles.

The silver-p-phenylene (Ag-PPP) interface is investigated using ballistic electron emission microscopy (BEEM). Multiple injection barriers and spatial nonuniformity of carrier injection over nanometer length scales are observed. No unique injection barrier is found. Physical reasons for these features are discussed. BEEM current images and the surface topography of the silver film are uncorrelated., Comment: To appear in Applied Physics Letters