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At least 325 records · Page 18

Interfacial Charge Engineering in Ferroelectric-Controlled Mott Transistors

Heteroepitaxial coupling at complex oxide interfaces introduces a powerful tool for engineering the charge degree of freedom in strongly correlated materials, which can be utilized to achieve tailored functionalities that are inaccessible in the bulk form. In this work, the charge-transfer effect between two strongly correlated oxides, Sm 0.5 Nd 0.5 NiO 3 (SNNO) and La 0.67 Sr 0.33 MnO 3 (LSMO), is exploited to realize a giant enhancement of the ferroelectric field effect in a prototype Mott field-effect transistor. By switching the polarization field of a ferroelectric Pb(Zr,Ti)O 3 (PZT) gate, nonvolatile resistance modulation in the Mott transistors with single-layer SNNO and bilayer SNNO/LSMO channels is induced. For the same channel thickness, the bilayer channels exhibit up to two orders of magnitude higher resistance-switching ratio at 300 K, which is attributed to the intricate interplay between the charge screening at the PZT/SNNO interface and the charge transfer at the SNNO/LSMO interface. X-ray absorption spectroscopy and X-ray photoelectron spectroscopy studies of SNNO/LSMO heterostructures reveal about 0.1 electron per 2D unit cell transferred between the interfacial Mn and Ni layers, which is corroborated by first-principles density functional theory calculations. The study points to an effective strategy to design functional complex oxide interfaces for developing high-performance nanoelectronic and spintronic applications.

36 MATERIALS SCIENCE↗

Topological and magnetic properties of the interacting Bernevig-Hughes-Zhang model

We investigate the effects of electronic correlations on the Bernevig-Hughes-Zhang model using the real-space density matrix renormalization group (DMRG) algorithm. We introduce a method to probe topological phase transitions in systems with strong correlations using DMRG, substantiated by an unsupervised machine learning methodology that analyzes the orbital structure of the real-space edges. Including the full multi-orbital Hubbard interaction term, we construct a phase diagram as a function of a gap parameter (m) and the Hubbard interaction strength (U) via exact DMRG simulations on N×4 cylinders. Our analysis confirms that the topological phase persists in the presence of interactions, consistent with previous studies, but it also reveals an intriguing phase transition from a paramagnetic to a stripey antiferromagnetic topological insulator. The combination of the magnetic structure factor, strength of magnetic moments, and the orbitally resolved density, provides real-space information on both topology and magnetism in a strongly correlated system.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

New Suns in the Cosmos. IV. The Multifractal Nature of Stellar Magnetic Activity in Kepler Cool Stars

In the present study, we investigate the multifractal nature of a long-cadence time series observed by the Kepler mission for a sample of 34 M dwarf stars and the Sun in its active phase. Using the Multifractal Detrending Moving Average algorithm, which enables the detection of multifractality in nonstationary time series, we define a set of multifractal indices based on the multifractal spectrum profile as a measure of the level of stellar magnetic activity. This set of indices is given by the (A, Δα, C, H)-quartet, where A, Δα, and C are related to geometric features from the multifractal spectrum and the global Hurst exponent H describes the global structure and memorability of time series dynamics. As a test, we measure these indices and compare them with a magnetic index defined as S {sub ph} and verify the degree of correlation among them. First, we apply the Poincaré plot method and find a strong correlation between the 〈S{sub ph}〉 index and one of the descriptors that emerges from this method. As a result, we find that this index is strongly correlated with long-term features of the signal. From the multifractal perspective, the 〈S{sub ph}〉 index is also strongly linked to the geometric properties of the multifractal spectrum except for the H index. Furthermore, our results emphasize that the rotation period of stars is scaled by the H index, which is consistent with Skumanich’s relationship. Finally, our approach suggests that the H index may be related to the evolution of stellar angular momentum and a star’s magnetic properties.

79 ASTRONOMY AND ASTROPHYSICS↗

Spectrometric Estimation of Total Nitrogen Concentration in Douglas-Fir Foliage

Spectral measurements of fresh and dehydrated Douglas-fir foliage, from trees cultivated under three fertilization treatments, were acquired with a laboratory spectrophotometer. The slope (first-derivative) of the fresh- and dry-leaf absorbance spectra at locations near known protein absorption features was strongly correlated with total nitrogen (TN) concentration of the foliage samples. Particularly strong correlation was observed between the first-derivative spectra in the 2150-2170 nm region and TN, reaching a local maximum in the fresh-leaf spectra of -0.84 at 2 160 nm. Stepwise regression was used to generate calibration equations relating first derivative spectra from fresh, dry/intact, and dry/ground samples to TN concentration. Standard errors of calibration were 1.52 mg g-1 (fresh), 1.33 (dry/intact), and 1.20 (dry/ground), with goodness-of-fit 0.94 and greater. Cross-validation was performed with the fresh-leaf dataset to examine the predictive capability of the regression method; standard errors of prediction ranged from 1.47 - 2.37 mg g(exp -1) across seven different validation sets, prediction goodness of fit ranged from .85-.94, and wavelength selection was fairly insensitive to the membership of the calibration set. All regressions in this study tended to select wavelengths in the 2100-2350 nm region, with the primary selection in the 2142-2172 nm region. The study provides positive evidence concerning the feasibility of assessing TN status of fresh-leaf samples by spectrometric means. We assert that the ability to extract biochemical information from fresh-leaf spectra is a necessary but insufficient condition regarding the use of remote sensing for canopy-level biochemical estimation.

Johnson, Lee F.↗

Morphology of galaxies in compact groups

Results of a study of galaxy morphology in a homogeneous sample of 98 compact groups of galaxies are reported. Of all the galaxies, 49 percent are of late morphological type (S + Irr), somewhat less than the corresponding fraction for field galaxies. Similarly, for first-ranked galaxies only, 48 percent are late type. Several strong correlations are found between galaxy type and the galaxy environment. Morphological concordance occurs between galaxies within a group. Galaxy morphological type correlates with group optical luminosity, and galaxy morphology correlates with velocity dispersion. The latter correlation is found to be the more fundamental of the two. No strong correlation between morphological type and galaxy space density is found in these compact groups, contrary to the situation in rich clusters and loose groups. These results indicate that the morphological types of galaxies in compact groups are strongly influenced by the environment, and that this influence occurs mostly at the time of galaxy formation.

Hickson, Paul↗

Density matrix embedding in an antisymmetrized geminal power bath

Density matrix embedding theory (DMET) has emerged as a powerful tool for performing wave function-in-wave function embedding for strongly correlated systems. In traditional DMET, an accurate calculation is performed on a small impurity embedded in a mean field bath. Here, we extend the original DMET equations to account for correlation in the bath via an antisymmetrized geminal power (AGP) wave function. The resulting formalism has a number of advantages. First, it allows one to properly treat the weak correlation limit of independent pairs, which DMET is unable to do with a mean-field bath. Second, it associates a size extensive correlation energy with a given density matrix (for the models tested), which AGP by itself is incapable of providing. Third, it provides a reasonable description of charge redistribution in strongly correlated but non-periodic systems. Thus, AGP-DMET appears to be a good starting point for describing electron correlation in molecules, which are aperiodic and possess both strong and weak electron correlation.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Microscopic Distributions of Defect Luminescence From Subgrain Boundaries in Multicrystalline Silicon Wafers

We investigate the microscopic distributions of sub-band-gap luminescence emission (the so-called D-lines D1/D2/D3/D4) and the band-to-band luminescence intensity, near recombination-active sub-grain boundaries in multicrystalline silicon wafers for solar cells. We find that the sub-band-gap luminescence from decorating defects/impurities (D1/D2) and from intrinsic dislocations (D3/D4) have distinctly different spatial distributions, and are asymmetric across the sub-grain boundaries. The presence of D1/D2 is correlated with a strong reduction in the band-to-band luminescence, indicating a higher recombination activity. In contrast, D3/D4 emissions are not strongly correlated with the band-to-band intensity. Based on spatially-resolved, synchrotron-based micro-X-ray fluorescence measurements of metal impurities, we confirm that high densities of metal impurities are present at locations with strong D1/D2 emission but low D3/D4 emission. Finally, we show that the observed asymmetry of the sub-band-gap luminescence across the sub-grain boundaries is due to their inclination below the wafer surface. Based on the luminescence asymmetries, the sub-grain boundaries are shown to share a common inclination locally, rather than be orientated randomly.

14 SOLAR ENERGY↗

Building and testing correlations for the estimation of one‐electron reduction potentials of a diverse set of organic molecules

We describe and evaluate a method for computationally predicting reduction potentials of a diverse group of organic molecules by linearly correlating calculated lowest unoccupied molecular orbital energies with ground state reduction potentials measured in acetonitrile. The approach is shown to provide a unique combination of extreme computational simplicity and excellent accuracy across a diverse range of organic structures and a wide window of reduction potentials. A disparate set of molecules (74 compounds belonging to six distinct structural families, comprised of molecules containing C, H, N, O, F, Cl, and Br, with functional groups including esters, ketones, halides, nitriles, quinones, alkenes, arenes, heteroarenes, and pyridinium and higher benzologs, all containing conjugated pi systems, spanning a 3.5‐V range of reduction potentials) was used to build the correlations. This methodology was found to be computationally inexpensive compared with other approaches and to permit the useful prediction of reduction potentials of additional molecules of diverse structural types not included in the families used to determine the correlation parameters. The effects of varying the basis set used in the B3LYP electronic structure calculations and including solvent (compared with calculations in gas phase) were also examined. It was found that the inclusion of a continuum solvent model in the calculations was required for accurate results, particularly when including cationic species in the correlations (although when only neutral molecules were examined, reasonable results could even be obtained in vacuo ). Several of the best correlations were used to predict the reduction potentials of seven much larger and structurally diverse chromophores that were not included in the correlation data set. Strong correlations ( r 2 values > 0.99) with very good predictive abilities (root mean square deviation < 60 mV) were found. This extremely simple and computationally efficient entirely closed‐shell methodology is proven robust and useful for the design of new molecules capable of participating in redox processes, including electron transfer reactions. Copyright © 2015 John Wiley & Sons, Ltd.

Méndez‐Hernández, Dalvin D.↗

Kinetic Isolation between Turnovers on Au 18 Nanoclusters: Formic Acid Decomposition One Molecule at a Time

Formic acid (HCOOH or FA) is a clean, safe, and renewable hydrogen storage material. Although Au catalysts decompose vapor-phase FA with high activity and selectivity toward hydrogen, the active site and reaction mechanism remain unclear. Here, we show that the subnanometric Au 18 cluster (0.8 nm in diameter) is likely the active species for FA decomposition. We performed coverage self-consistent, density functional theory-based kinetic Monte Carlo simulations of FA decomposition on gas-phase Au18 clusters, predicting 100% selectivity toward hydrogen and turnover frequencies close to experimentally determined values. The active site is made up of a triangular ensemble of three atoms each possessing a coordination number of 5. Although there are two active site ensembles on the Au18 cluster, their occupations are strongly correlated because of strong, stabilizing interactions between pairs of open-shell adsorbates mediated by the superatomic nature of the cluster. Because the occupation of the active sites blocks the dissociation of additional HCOOH molecules, there is kinetic isolation between turnovers: only one HCOOH molecule can dissociate on the cluster at a time. This explains the extraordinary, experimentally observed selectivity of Au catalysts toward HD during decomposition of HCOOD and DCOOH. Our work offers nanoscale insights into the reaction mechanisms of FA decomposition over Au. This represents a rare example of heterogeneous catalysis by a cluster that catalyzes reactants one molecule at a time. Our work on Au18 thus sheds light on how the unique electronic properties of subnanometric clusters can be used to design quasi-molecular catalysts with high activity and selectivity.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Analytic gradients for compressed multistate pair-density functional theory

Photochemical reactions often involve states that are closely coupled due to near degeneracies, for example by proximity to conical intersections. Therefore, a multistate method is used to accurately describe these states; for example, ordinary perturbation theory is replaced by quasidegenerate perturbation theory. Multiconfiguration pair-density functional theory (MC-PDFT) provides an efficient way to approximate the full dynamical correlation energy of strongly correlated systems, and we recently proposed compressed multistate pair-density functional theory (CMS-PDFT) to treat closely coupled states. In the present paper, we report the implementation of analytic gradients for CMS-PDFT in both OpenMolcas and PySCF, and here we illustrate the use of these gradients by applying the method to the excited states of formaldehyde and phenol.

74 ATOMIC AND MOLECULAR PHYSICS↗

Sachdev-Ye-Kitaev models and beyond: Window into non-Fermi liquids

In this work is a review of the Sachdev-Ye-Kitaev (SYK) model of compressible quantum many-body systems without quasiparticle excitations, and its connections to various theoretical studies of non-Fermi liquids in condensed matter physics. The review is placed in the context of numerous experimental observations on correlated electron materials. Strong correlations in metals are often associated with their proximity to a Mott transition to an insulator created by the local Coulomb repulsion between the electrons. The phase diagrams of a number of models of such a local electronic correlation are explored, employing a dynamical mean-field theory in the presence of random spin exchange interactions. Numerical analyses and analytical solutions, using renormalization group methods and expansions in large spin degeneracy, lead to critical regions that display SYK physics. The models studied include the single-band Hubbard model, the t–J model, and the two-band Kondo-Heisenberg model in the presence of random spin exchange interactions. Also examined are non-Fermi liquids obtained by considering each SYK model with random four-fermion interactions to be a multiorbital atom, with the SYK atoms arranged in an infinite lattice. Connections are made to theories of sharp Fermi surfaces without any low-energy quasiparticles in the absence of spatial disorder, obtained by coupling a Fermi liquid to a gapless boson; a systematic large-N theory of such a critical Fermi surface, with SYK characteristics, is obtained by averaging over an ensemble of theories with random boson-fermion couplings. Finally, an overview of the links between the SYK model and quantum gravity is presented, and the review ends with an outlook on open questions.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Interannual Variability of OLR as Observed by AIRS and CERES

The paper examines spatial anomaly time series of Outgoing Longwave Radiation (OLR) and Clear Sky OLR (OLR(sub CLR)) as determined using observations from CERES Terra and AIRS over the time period September 2002 through June 2011. We find excellent agreement of the two OLR data sets in almost every detail down to the x11deg spatial grid point level. The extremely close agreement of OLR anomaly time series derived from observations by two different instruments implies high stability of both sets of results. Anomalies of global mean, and especially tropical mean, OLR are shown to be strongly correlated with an El Nino index. These correlations explain that the recent global and tropical mean decreases in OLR over the time period studied are primarily the result of a transition from an El Nino condition at the beginning of the data record to La Nina conditions toward the end of the data period. We show that the close correlation of mean OLR anomalies with the El Nino Index can be well accounted for by temporal changes of OLR within two spatial regions, one to the east of, and one to the west of, the NOAA Nino-4 region. Anomalies of OLR in these two spatial regions are both strongly correlated with the El Nino Index as a result of the strong anti-correlation of anomalies of cloud cover and mid-tropospheric water vapor in these two regions with the El Nino Index.

Susskind, Joel↗

Exploring DFT+U parameter space with a Bayesian calibration assisted by Markov chain Monte Carlo sampling

Abstract The density-functional theory is widely used to predict the physical properties of materials. However, it usually fails for strongly correlated materials. A popular solution is to use the Hubbard correction to treat strongly correlated electronic states. Unfortunately, the values of the Hubbard U and J parameters are initially unknown, and they can vary from one material to another. In this semi-empirical study, we explore the U and J parameter space of a group of iron-based compounds to simultaneously improve the prediction of physical properties (volume, magnetic moment, and bandgap). We used a Bayesian calibration assisted by Markov chain Monte Carlo sampling for three different exchange-correlation functionals (LDA, PBE, and PBEsol). We found that LDA requires the largest U correction. PBE has the smallest standard deviation and its U and J parameters are the most transferable to other iron-based compounds. Lastly, PBE predicts lattice parameters reasonably well without the Hubbard correction.

36 MATERIALS SCIENCE↗

Electronic structure and two-band superconductivity in unconventional high- T c cuprates Ba 2 CuO 3+δ

We report that the recently discovered cuprate superconductor Ba 2 CuO 3+δ exhibits a high T c ≃73 K at δ ≃ 0.2. The polycrystal grown under high pressure has a structure similar to La 2 CuO 4 but with dramatically different lattice parameters due to the CuO 6 octahedron compression. The crystal field in the compressed Ba 2 CuO 4 leads to an inverted Cu 3d e g complex with the d x 2 -y 2 orbital sitting below the d 3z 2 - r 2 and an electronic structure highly unusual compared to the conventional cuprates. We construct a two-orbital Hubbard model for the Cu d 9 state at hole doping x = 2δ and study the orbital-dependent strong correlation and superconductivity. For the undoped case at x = 0 , we found that strong correlation drives an orbital-polarized Mott-insulating state with the spin-1/2 moment of the localized d 3z 2 - r 2 orbital. In contrast to the single-band cuprates where superconductivity is suppressed in the overdoped regime, hole doping the two-orbital Mott insulator leads to orbital-dependent correlations and the robust spin and orbital exchange interactions produce a high-T c antiphase d-wave superconductor even in the heavily doped regime at x = 0.4 . We conjecture that Ba 2 CuO 3+δ realizes mixtures of such heavily hole-doped superconducting Ba 2 CuO 4 and disordered Ba 2 CuO 3 chains in a single-layer or predominately separated bilayer structure. Our findings suggest that unconventional cuprates with liberated orbitals as doped two-band Mott insulators can be a direction for realizing high-T c superconductivity with enhanced transition temperature T c .

36 MATERIALS SCIENCE↗

CHANGO: A Software Tool for Boost Stage Guidance of the Space Launch System Exploration Mission 1

The Day of Launch Initiation Load Update (DOLILU) System is the means by which the Space Launch System (SLS) Vehicle trajectory is designed, verified, and uploaded on the Day of Launch (DOL) in order to ensure a safe flight. Launch vehicles are designed to fly down a narrow angle of attack and sideslip angle corridor in order to keep them within structural load limits. The angle of attack and sideslip angle response to the launch vehicle experiences can vary significantly based upon the winds experienced on the DOL. SLS Boost Stage flight employs an open-loop guidance scheme through Solid Rocket Booster (SRB) separation. In the SLS open-loop scheme, the vehicle will fly a prescribed set of attitudes as a function of the change in altitude since launch. This set of reference attitude values and corresponding altitude reference independent values are designed with ground software using winds measured on the DOL with the goal of minimizing angle of attack and sideslip angle, thereby minimizing related ascent integrated vehicle structural loads. The table of Boost Stage attitude commands as a function of altitude gained since launch is called the chi table. A software tool called CHANGO (Chi Angle Optimizer) designs the Boost Stage chi table which is uploaded to the vehicle’s flight computer and used during ascent by the flight software (FSW). The wind and atmospheric conditions are measured prior to launch and pre-processed to become input to the CHANGO software along with a set of parameters developed in advance of the DOL. CHANGO’s target set consists of the heading and altitude rate at SRB separation determined well before launch by the Program to Optimize Simulated Trajectories (POST). CHANGO consists of a simplified three degree-of-freedom (3-DOF) simulation representing the SLS launch configuration. In general, the launch azimuth is strongly correlated with the heading at SRB separation, and the initial pitchover rate is strongly correlated with the altitude rate at SRB separation. CHANGO uses an adaptation of Powell’s method to vary the initial pitchover rate and launch azimuth to solve a 2-dimentional minimization problem. CHANGO’s trajectory simulation is phase-based, with flight events separating the phases. Each flight phase has different attitude alignment logic. CHANGO’s 3-DOF simulation starts when the vehicle’s thrust-to-weight ratio equals one, and ends at a pre-calculated SRB separation time.

Ahmad, Naeem↗

Data from Assessing Precipitation, Evapotranspiration, and NDVI as Controls of U.S. Great Plains Plant Production

Productivity throughout the North American Great Plains grasslands is generally considered to be water limited, with the strength of this limitation increasing as precipitation decreases. We hypothesize that cumulative actual evapotranspiration water loss (AET) from April to July is the precipitation‐related variable most correlated to aboveground net primary production (ANPP) in the U.S. Great Plains (GP). We tested this by evaluating the relationship of ANPP to AET, precipitation, and plant transpiration (Tr). We used multi‐year ANPP data from five sites ranging from semiarid grasslands in Colorado and Wyoming to mesic grasslands in Nebraska and Kansas, mean annual NRCS ANPP, and satellite‐derived normalized difference vegetation index (NDVI) data. Results from the five sites showed that cumulative April‐to‐July AET, precipitation, and Tr were well correlated (R2: 0.54–0.70) to annual changes in ANPP for all but the wettest site. AET and Tr were better correlated to annual changes in ANPP compared to precipitation for the drier sites, and precipitation in August and September had little impact on productivity in drier sites. April‐to‐July cumulative precipitation was best correlated (R2 = 0.63) with interannual variability in ANPP in the most mesic site, while AET and Tr were poorly correlated with ANPP at this site. Cumulative growing season (May‐to‐September) NDVI (iNDVI) was strongly correlated with annual ANPP at the five sites (R2 = 0.90). Using iNDVI as a surrogate for ANPP, we found that county‐level cumulative April–July AET was more strongly correlated to ANPP than precipitation for more than 80% of the GP counties, with precipitation tending to perform better in the eastern more mesic portion of the GP. Including the ratio of AET to potential evapotranspiration (PET) improved the correlation of AET to both iNDVI and mean county‐level NRCS ANPP. Accounting for how different precipitation‐related variables control ANPP (AET in drier portion, precipitation in wetter portion) provides opportunity to develop spatially explicit forecasting of ANPP across the GP for enhancing decision‐making by land managers and use of grassland ANPP for biofuels.

Field Data↗

Multiple Slater Determinants and Strong Spin-Fluctuations as Key Ingredients of the Electronic Structure of Electron- and Hole-Doped Pb 10− x Cu x (PO 4 ) 6 O

LK-99, with chemical formula Pb 10−x Cu x (PO 4 ) 6 O, was recently reported to be a room-temperature superconductor. While this claim has met with little support in a flurry of ensuing work, a variety of calculations (mostly based on density-functional theory) have demonstrated that the system possesses some unusual characteristics in the electronic structure, in particular flat bands. We have established previously that within DFT, the system is insulating with many characteristics resembling the classic cuprates, provided the structure is not constrained to the P3(143) symmetry nominally assigned to it. Here we describe the basic electronic structure of LK-99 within self-consistent many-body perturbative approach, quasiparticle self-consistent GW (QSGW) approximation and their diagrammatic extensions. QSGW predicts that pristine LK-99 is indeed a Mott/charge transfer insulator, with a bandgap gap in excess of 3 eV, whether or not constrained to the P3(143) symmetry. When Pb 9 Cu(PO 4 ) 6 O is hole-doped, the valence bands modify only slightly, and a hole pocket appears. However, two solutions emerge: a high-moment solution with the Cu local moment aligned parallel to neighbors, and a low-moment solution with Cu aligned antiparallel to its environment. In the electron-doped case the conduction band structure changes significantly: states of mostly Pb character merge with the formerly dispersionless Cu d state, and high-spin and low spin solutions once again appear. Thus we conclude that with suitable doping, the ground state of the system is not adequately described by a band picture, and that strong correlations are likely. Irrespective of whether this system class hosts superconductivity or not, the transition of Pb 10 (PO 4 ) 6 O from being a band insulator to Pb 9 Cu(PO 4 ) 6 O, a Mott insulator, and multi-determinantal nature of doped Mott physics make this an extremely interesting case-study for strongly correlated many-body physics.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Nonresonant pump/probe electronic Raman scattering within nonequilibrium dynamical mean-field theory

We develop the theory for nonresonant Raman scattering of strongly correlated electrons in time-resolved pump-probe experiments. The electrons are initially pumped with an intense pulse of light and then a probe pulse measures the Raman response function after an adjustable time delay. Here, we describe how the width of the probe pulse and the strength of the electron correlations affect the Raman cross section. The theory is developed for the case of B 1g symmetry, where incident and scattered light are polarized perpendicular to each other. We illustrate the exact solution with the Falicov-Kimball model, which is solved via nonequilibrium dynamical mean-field theory.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗