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Luminescent and magnetic [TbEu] 2D metal–organic frameworks

Here, we present the synthesis, through a simple, microwave-assisted method, of lanthanoid-based 2D metal–organic frameworks (MOFs) of general formula [Ln x Ln' 1–x (MeCOO)(PhCOO) 2 ], including homonuclear compounds (x = 1), Ln$=$Eu, Tb, and heterometallic compounds, [TbEu]. The crystalline material is formed by neutral nanosheets held together by van der Waals interactions, which can be easily exfoliated by sonication. Photoluminescent emission in the visible range was observed for all of the synthesized 2D MOF compounds via excitation of the ligand, showing benzoates are efficient antenna ligands. Efficient energy transfer from Tb → Eu was observed in the heterometallic [TbEu] compounds, which could potentially perform as luminescent thermometers. Inks containing nanosheets of 2D MOFs exfoliated in solution were prepared, and luminescent prints of Tb and Eu 2D MOFs on paper were made to show the possible application for anticounterfeiting. Frequency-dependent ac susceptibility results show the occurrence of slow magnetic relaxation in [TbEu] compounds through direct relaxation mechanisms, affected by bottleneck effect. A slowing down of the relaxation time is observed as the Eu/Tb ratio increases.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Electrochemical hydrogen isotope exchange of amines controlled by alternating current frequency

Here, we report an electrochemical protocol for hydrogen isotope exchange (HIE) at α-C(sp 3 )–H amine sites. Tetrahydroisoquinoline and pyrrolidine are selected as two model substrates because of their different proton transfer (PT) and hydrogen atom transfer (HAT) kinetics at the α-C(sp 3 )–H amine sites, which are utilized to control the HIE reaction outcome at different applied alternating current (AC) frequencies. We found the highest deuterium incorporation for tetrahydroisoquinolines at 0 Hz (i.e., under direct current (DC) electrolysis conditions) and pyrrolidines at 0.5 Hz. Analysis of the product distribution and D isotope incorporation at different frequencies reveals that the HIE of tetrahydroisoquinolines is limited by its slow HAT, whereas the HIE of pyrrolidines is limited by the overoxidation of its α-amino radical intermediates. Here, the AC-frequency-dependent HIE of amines can be potentially used to achieve selective labeling of α-amine sites in one drug molecule, which will significantly impact the pharmaceutical industry.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Interface diagnostics platform for thin-film solid-state batteries

Understanding the impedances of battery materials and their interfaces remains a major challenge, usually addressed by electrochemical impedance spectroscopy (EIS) where frequency-dependent complex impedance of full battery cells is measured and then modeled by a network of connected electrical elements. As conventionally applied, this approach produces ambiguity in that (1) multiple different network configurations may fit the data convincingly and (2) the method offers no direct association of the electrical elements with physical features of the battery. Here we present a new methodology that resolves both sources of ambiguity, enabled by expanding the experimental scope to directly inform the configuration of elements and their parameters in the network model. We demonstrate this methodology using thin film fabrication of solid state battery devices patterned by shadow masked sputter deposition, so that diagnostic devices corresponding to individual interface and material components can be fabricated simultaneously with full cell batteries. EIS models for the diagnostic devices can then be connected to form full cell networks whose topology matches the well-known physical configuration of the battery. When connected in this way, the full network model – made from connecting the diagnostic device EIS models – fits the full cell EIS data. For the case of a thin film solid state battery composed of amorphous silicon anode, lithium phosphorus oxynitride (LiPON) solid electrolyte, and lithium vanadium oxide (Li x V 2 O 5 ) cathode, we show that the approach allows us to identify ionic impedance/conductivity of the cathode/electrolyte as a limiting impedance and the anode/electrolyte interface cycling instability as a primary degradation factor.

25 ENERGY STORAGE↗

Planck 2013 results. XXIII. Isotropy and statistics of the CMB

The two fundamental assumptions of the standard cosmological model-that the initial fluctuations are statistically isotropic and Gaussian-are rigorously tested using maps of the cosmic microwave background (CMB) anisotropy from the Planck satellite. The detailed results are based on studies of four independent estimates of the CMB that are compared to simulations using a fiducial ΛCDM model and incorporating essential aspects of the Planck measurement process. Deviations from isotropy have been found and demonstrated to be robust against component separation algorithm, mask choice, and frequency dependence. Many of these anomalies were previously observed in the WMAP data, and are now confirmed at similar levels of significance (about 3σ). However, we find little evidence of non-Gaussianity, with the exception of a few statistical signatures that seem to be associated with specific anomalies. In particular, we find that the quadrupole-octopole alignment is also connected to a low observed variance in the CMB signal. A power asymmetry is now found to persist on scales corresponding to about ℓ = 600 and can be described in the low-ℓ regime by a phenomenological dipole modulation model. However, any primordial power asymmetry is strongly scale-dependent and does not extend to arbitrarily small angular scales. Finally, it is plausible that some of these features may be reflected in the angular power spectrum of the data, which shows a deficit of power on similar scales. Indeed, when the power spectra of two hemispheres defined by a preferred direction are considered separately, one shows evidence of a deficit in power, while its opposite contains oscillations between odd and even modes that may be related to the parity violation and phase correlations also detected in the data. Although these analyses represent a step forward in building an understanding of the anomalies, a satisfactory explanation based on physically motivated models is still lacking.

79 ASTRONOMY AND ASTROPHYSICS↗

Planck 2013 results. XVIII. The gravitational lensing-infrared background correlation

The multi-frequency capability of the Planck satellite provides information both on the integrated history of star formation (via the cosmic infrared background, or CIB) and on the distribution of dark matter (via the lensing effect on the cosmic microwave background, or CMB). The conjunction of these two unique probes allows us to measure directly the connection between dark and luminous matter in the high redshift (1 ≤ z ≤ 3) Universe. We use a three-point statistic optimized to detect the correlation between these two tracers. Following a thorough discussion of possible contaminants and a suite of consistency tests, using lens reconstructions at 100, 143 and 217 GHz and CIB measurements at 100–857 GHz, we report the first detection of the correlation between the CIB and CMB lensing. The well matched redshift distribution of these two signals leads to a detection significance with a peak value of 42/19σ at 545 GHz and a correlation as high as 80% across these two tracers. Our full set of multi-frequency measurements (both CIB auto- and CIB-lensing cross-spectra) are consistent with a simple halo-based model, with a characteristic mass scale for the halos hosting CIB sources of log 10 ( M/M ⊙ ) = 10.5 ± 0.6. Leveraging the frequency dependence of our signal, we isolate the high redshift contribution to the CIB, and constrain the star formation rate (SFR) density at z ≥ 1. Here, we measure directly the SFR density with around 2σ significance for three redshift bins between z = 1 and 7, thus opening a new window into the study of the formation of stars at early times.

79 ASTRONOMY AND ASTROPHYSICS↗

Planck intermediate results. LVI. Detection of the CMB dipole through modulation of the thermal Sunyaev-Zeldovich effect: Eppur si muove II

The largest temperature anisotropy in the cosmic microwave background (CMB) is the dipole, which has been measured with increasing accuracy for more than three decades, particularly with the Planck satellite. The simplest interpretation of the dipole is that it is due to our motion with respect to the rest frame of the CMB. Since current CMB experiments infer temperature anisotropies from angular intensity variations, the dipole modulates the temperature anisotropies with the same frequency dependence as the thermal Sunyaev-Zeldovich (tSZ) effect. Here, we present the first, and significant, detection of this signal in the tSZ maps and find that it is consistent with direct measurements of the CMB dipole, as expected. The signal contributes power in the tSZ maps, which is modulated in a quadrupolar pattern, and we estimate its contribution to the tSZ bispectrum, noting that it contributes negligible noise to the bispectrum at relevant scales.

79 ASTRONOMY AND ASTROPHYSICS↗

Polarization and variability of compact sources measured in Planck time-ordered data

This paper introduces a new Planck Catalog of Polarized and Variable Compact Sources (PCCS-PV) comprising 153 sources, the majority of which are extragalactic. The data include both the total flux density and linear polarization measured by Planck with frequency coverage from 30 to 353 GHz, and temporal spacing ranging from days to years. We classify most sources as beamed, extragalactic radio sources; the catalog also includes several radio galaxies, Seyfert galaxies, and Galactic and Magellanic Cloud sources, including H II regions and planetary nebulae. An advanced extraction method applied directly to the multifrequency Planck time-ordered data, rather than the mission sky maps, was developed to allow an assessment of the variability of polarized sources. Our analysis of the time-ordered data from the Planck mission, tod2flux, allowed us to catalog the time-varying emission and polarization properties for these sources at the full range of polarized frequencies employed by Planck, 30-353 GHz. PCCS-PV provides the time-and frequency-dependent, polarized flux densities for all 153 sources. To illustrate some potential applications of the PCCS-PV, we conducted preliminary comparisons of our measurements of selected sources with published data from other astronomical instruments. In summary, we find general agreement between the Planck and the Institut de Radioastronomie Millimétrique (IRAM) polarization measurements as well as with the Metsähovi 37 GHz values at closely similar epochs. Here, these combined measurements also show the value of PCCS-PV results and the PCCS2 catalog for filling in missing spectral (or temporal) coverage and helping to define the spectral energy distributions of extragalactic sources. In turn, these results provide useful clues as to the physical properties of the sources.

79 ASTRONOMY AND ASTROPHYSICS↗

Range, resolution and power of THz systems for remote detection of concealed radioactive materials

This paper analyzes parameters required for realizing remote detection of a concealed source of ionizing radiation by observing the occurrence of breakdown in air by a focused wave beam. Production of free electrons and the free electron density in the absence/presence of additional sources of ionization are analyzed. The maximum electron density in the discharge and the time required for this density to return after the discharge back to its stationary level, are estimated. The optimal excess of the power density and the corresponding power level as the function of frequency are determined. It is shown that the optimal frequency of such systems ranges from 0.3 up to 0.8 THz. The paper also determines the range of such systems as the function of the source frequency and power and contains a brief analysis of available sources of microwave, millimeter-wave and THz radiation.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Fluid and kinetic models of negative ion sheaths

Due to the presence of a large transverse magnetic field (B{sub x} and B{sub y} where z is the extraction axis), the extraction of electrons from a negative ion source is likely to happen with a large angle with respect to z axis. The negative ion and electron sheaths are here studied both with kinetic and with fluid models. First, Vlasov-Poisson models are reduced to one dimensional integrodifferential equations, discussing also trapped orbits. The integrodifferential equations for electron transport are analytically solved for a variety of extraction potentials (in 1D). Collision frequency dependency from electron flow speed and temperature is discussed. Then both ion and electron space charge and fluid motion are solved, using electron densities expression consistent with kinetic model. Results for the sheath charge profile and extraction field as a function of B{sub x} are shown.

43 PARTICLE ACCELERATORS↗

Electrochemical strain microscopy with blocking electrodes: The role of electromigration and diffusion

Electrochemical strains are a ubiquitous feature of solid state ionic devices ranging from ion batteries and fuel cells to electroresistive and memristive memories. We proposed a scanning probe microscopy (SPM) based approach, referred as electrochemical strain microscopy (ESM), for probing local ionic flows and electrochemical reactions in solids based on bias-strain coupling. In ESM, the sharp SPM tip concentrates the electric field in a small (10-50 nm) region of material, inducing interfacial electrochemical processes and ionic flows. Furthermore, we use the resultant electrochemical strains to determine it from dynamic surface displacement and provide information on local electrochemical functionality. We also analyze image formation mechanism in ESM for a special case of mixed electronic-ionic conductor with blocking tip electrode, and determine frequency dependence of response, role of diffusion and electromigration effects, and resolution and detection limits.

36 MATERIALS SCIENCE↗

Modeling and theoretical efficiency of a silicon nanowire based thermoelectric junction with area enhancement

Recent experimental work suggests that individual silicon nanowires with rough surfaces possess a thermoelectric figure of merit as high as 0.6 near room temperature. This paper addresses the possibility of using an array of such nanowires in a thermoelectric junction for generation. Employing a model of frequency dependent phonon boundary scattering, we estimate the effective thermal conductivity of the array and investigate heat flow through the junction. We show that charge transport is largely unaffected by the roughness scales considered. Enhancing the area for heat exchange at an individual 200 mu m x 200 mu m p-n junction yields significant temperature differences across the junction leading to power >0.6 mW and efficiency >1.5% for a junction with effective thermal conductivity <5 W/mK, when the source and sink are at 450 K and 300 K, respectively. We show that relatively short nanowires of similar to 50 mu m length are sufficient for obtaining peak power and reasonable efficiency. This substantially reduces the challenge of engineering low resistivity electrical contacts that critically affect power and efficiency. This paper provides insight into how fundamental transport in relation to bulk heat transfer and charge transport, affects the performance of thermoelectric junctions based on nanostructured materials. (C) 2012 American Institute of Physics. [http://dx.doi.org/10.1063/1.4728189]

Seong, M↗

Effects of domain, grain, and magnetic anisotropy distributions on magnetic permeability: Monte-Carlo approach

Existing approaches for prediction of the tensor permeability of polycrystalline ferrites may not provide reasonable estimates of demagnetized permeability below the spin resonance (i.e., low-field loss region) or in cases of partial magnetization. We propose an approach which solves the coupled Landau-Lifshitz-Gilbert equation for the dynamic magnetic fields including the minimization of free energy to determine the equilibrium magnetization direction. Unlike previous models, we employ a Monte-Carlo approach to easily calculate the (ensemble) averages of permeability over various domain/grain structures and magnetic anisotropy conditions. Material differences, such as those resulting from different preparation methods, are expressed by using probability density functions (p.d.f.) for anisotropy angle (easy axis angle), grain demagnetization factor (ng), and domain demagnetization factor (nd). Effects on the permeability tensor of grain and domain demagnetization factors and anisotropy field relative to saturation magnetization are discussed for the partially magnetized states for polycrystalline ferrites. It is found that the grain structure (i.e., grain demagnetization distribution) has a smaller effect on the frequency dependent permeability than does the same distribution of domains (i.e., domain demagnetization distribution).

36 MATERIALS SCIENCE↗

Target duality in N= 8 superconformal mechanics and the coupling of dual pairs

We couple dual pairs of N= 8 superconformal mechanics with conical targets of dimension d and 8−d. The superconformal coupling generates an oscillator-type potential on each of the two target factors, with a frequency depending on the respective dual coordinates. In the case of the inhomogeneous (3,8,5) model, which entails a monopole background, it is necessary to add an extra supermultiplet of constants for half of the supersymmetry. The N= 4 analog, joining an inhomogeneous (1,4,3) with a (3,4,1) multiplet, is also analyzed in detail.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

Trap states in AlGaN channel high-electron-mobility transistors

Frequency dependent capacitance and conductance measurements were performed to analyze the trap states in the AlGaN channel high-electron-mobility transistors (HEMTs). The trap state density in the AlGaN channel HEMTs decreases from 1.26 × 10{sup 13} cm{sup −2}eV{sup −1} at the energy of 0.33 eV to 4.35 × 10{sup 11} cm{sup −2}eV{sup −1} at 0.40 eV. Compared with GaN channel HEMTs, the trap states in the AlGaN channel HEMTs have deeper energy levels. The trap with deeper energy levels in the AlGaN channel HEMTs is another reason for the reduction of the reverse gate leakage current besides the higher Schottky barrier height.

74 ATOMIC AND MOLECULAR PHYSICS↗

Predictions of the poloidal asymmetries and transport frequencies in KSTAR

The extended neoclassical rotation theory formulated in Miller flux surface geometry enables unprecedented neoclassical calculations of the poloidal asymmetries in density, rotation velocities, electrostatic potential along the flux surfaces, and of the inertial (Reynolds stress) and gyroviscous transport frequencies, which are strong functions of these asymmetries. This paper presents such calculations of the poloidal asymmetries and non-negligible inertial and gyroviscous transport frequencies in two KSTAR (Korea Superconducting Tokamak Advanced Research) [Kwon et al., Nucl. Fusion 51, 094006 (2011)] Neutral Beam Injection H-mode discharges. The in-out asymmetries in the velocities are an order of magnitude larger than their up-down asymmetries. The magnitudes of the predicted inertial and gyroviscous transport frequencies depend on the magnitudes of the density and velocity asymmetries. The neoclassically predicted density asymmetries are shown to correspond with the reported measurements in tokamaks and the predicted carbon toroidal velocities agree very well with the measurements in KSTAR.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Compositional dependence of magnetic and high frequency properties of nanogranular FeCo-TiO{sub 2} films

A series of soft magnetic nanogranular FeCo-TiO{sub 2} films with different compositions of FeCo were fabricated on Si substrates by co-sputtering FeCo and TiO{sub 2}, and the magnetic and high frequency properties were studied in details. X-ray diffraction analysis confirmed that the films were nanocrystalline/amorphous composites. A high saturation magnetization of 14 kGs, a low coercivity of 5.3 Oe, a FMR frequency of 3.2 GHz, and a high resistivity of 1068 μΩ cm were obtained when the volume fraction of FeCo was 0.68. The excellence electromagnetic properties make the films an excellent candidate for microwave applications.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Nonlinear simulations to optimize magnetic nanoparticle hyperthermia

Magnetic nanoparticle hyperthermia is an attractive emerging cancer treatment, but the acting microscopic energy deposition mechanisms are not well understood and optimization suffers. We describe several approximate forms for the characteristic time of Néel rotations with varying properties and external influences. We then present stochastic simulations that show agreement between the approximate expressions and the micromagnetic model. The simulations show nonlinear imaginary responses and associated relaxational hysteresis due to the field and frequency dependencies of the magnetization. This suggests that efficient heating is possible by matching fields to particles instead of resorting to maximizing the power of the applied magnetic fields.

62 RADIOLOGY AND NUCLEAR MEDICINE↗

Measurement of the intrinsic damping constant in individual nanodisks of Y{sub 3}Fe{sub 5}O{sub 12} and Y{sub 3}Fe{sub 5}O{sub 12}|Pt

We report on an experimental study on the spin-waves relaxation rate in two series of nanodisks of diameter ϕ=300, 500, and 700 nm, patterned out of two systems: a 20 nm thick yttrium iron garnet (YIG) film grown by pulsed laser deposition either bare or covered by 13 nm of Pt. Using a magnetic resonance force microscope, we measure precisely the ferromagnetic resonance linewidth of each individual YIG and YIG|Pt nanodisks. We find that the linewidth in the nanostructure is sensibly smaller than the one measured in the extended film. Analysis of the frequency dependence of the spectral linewidth indicates that the improvement is principally due to the suppression of the inhomogeneous part of the broadening due to geometrical confinement, suggesting that only the homogeneous broadening contributes to the linewidth of the nanostructure. For the bare YIG nano-disks, the broadening is associated to a damping constant α=4 × 10{sup −4}. A threefold increase of the linewidth is observed for the series with Pt cap layer, attributed to the spin pumping effect. The measured enhancement allows to extract the spin mixing conductance found to be G{sub ↑↓}=1.55 × 10{sup 14} Ω{sup −1} m{sup −2} for our YIG(20nm)|Pt interface, thus opening large opportunities for the design of YIG based nanostructures with optimized magnetic losses.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗