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At least 973 records · Page 54

Predicting the climate change impacts on water-carbon coupling cycles for a loess hilly-gully watershed

Understanding the climate change impacts on water and carbon cycles is of great importance for comprehensive watershed management. Although many studies have been conducted on the future climate change impacts on either water cycle or carbon cycle, the potential impacts on water-carbon coupling cycles are still poorly understood. Here we used an integrated hydro-biochemical model (SWAT-DayCent) to quantitatively investigate the climate change impacts on water-carbon coupling cycles with a case study of typical loess hilly-gully watershed-the Jinghe River Basin (JRB) on the Loess Plateau. We used climate scenarios data derived under the three Representative Concentration Pathways (RCPs2.6, 4.5 and 8.5) by five downscaled Global Circulation Models (GCMs) and set two future periods of 2020–2049 (near future, NF) and 2070–2099 (far future, FF). It was projected that the annual precipitation would generally decrease slightly during the NF period but increase by 4–11% during the FF period, while the maximum/minimum air temperatures would increase significantly. The average annual streamflow would decrease (with up to 20.1% under RCP8.5) and evapotranspiration (ET) would remain almost unchanged during the NF period; however, both of them would increase during the FF period. The net primary production (NPP) would be generally higher due to the CO2 fertilization, whereas the soil organic carbon would decrease across all scenarios due to the warmer climate. The NPP-ET was projected to be closely coupled across all scenarios, and this coupling was mainly controlled by the inter-annual variability (IAV) of precipitation. Moreover, the precipitation IAV combined with NPP-ET coupling could also jointly control the NPP variability in the JRB. These projections in water-carbon coupling cycles can be useful to make better-informed decisions for future water resources and ecosystem management of the loess hilly-gully regions.

climate change↗

High fidelity multiphysics tightly coupled model for a lead cooled fast reactor concept and application to statistical calculation of hot channel factors

A tightly coupled multiphysics code system is established using the MOOSE framework for hot channel factor (HCF) evaluation on a Lead Fast Reactor (LFR) concept. The coupled system is driven by the Griffin multiphysics coupling capability under which the MOOSE Heat Transfer module and NekRS computational fluid dynamics solver are coupled for conjugate heat transfer using the Cardinal application. The coupled capability is demonstrated on an LFR assembly model based on materials and geometry of a prototypical lead-cooled fast reactor design by Westinghouse Electric Company, LLC. Moreover, the work integrates the Multiphysics Object Oriented Simulation Environment (MOOSE) Stochastic Tools Module (STM) to perform calculations for statistical analysis of HCF. Furthermore, the coupling strategy and workflow demonstrated in this paper is not only useful for predicting accurate hot channel factors for different kinds of advanced reactors but also for other engineering applications such as control rod worth assessment, generation of high-fidelity database for Artificial intelligence (AI)/machine learning (ML) training, design optimization and multi-resolution modeling.

Cardinal↗

Effects of inter-pulse coupling on nanosecond pulsed high frequency discharge ignition in a flowing mixture

This work numerically investigates the effects of non-equilibrium nanosecond plasma discharge pulse rep- etition frequency, pulse number, and flow velocity on the critical ignition volume, minimum ignition energy, and chemistry in a plasma-assisted H 2 /air flow at 300 K and 1 atm using a multi-scale adaptive reduced chemistry solver for plasma assisted combustion (MARCS-PAC). The interactions between discharges/ignition kernels spanning decoupled, partially-coupled and fully-coupled regimes in a pulse train are studied. For a single pulse discharge, increased flow velocity increases the minimum ignition energy required due to the increase of convective heat loss and flame stretch. The results show that the minimum ignition kernel prop- agation speed at the critical ignition kernel volume increases with the flow velocity. The minimum critical ignition volume decreases with the increase of plasma discharge energy. For sequential two-pulse discharges, ignition fails at both decoupled and partially-coupled regimes even when the total discharge energy is above the minimum ignition energy, but succeeds only in the fully-coupled regime at a shorter inter-pulse time. Overlap of the OH radical pool between the sequential two-pulse discharges and the increase of the chemistry effect due to the increase of reduced electric field in the fully-coupled regime contribute to the ignition enhancement. In addition, for two-pulse discharges in the fully-coupled discharge regime, the mixture can be ignited at a total energy below the minimum ignition energy of a single pulse with the same flow conditions. Moreover, for a given total discharge energy with multiple pulsed discharges, the enhancement of the ignition kernel volume has a non-monotonic dependence on discharge frequency and pulse number. The effective ignition enhancement can be achieved with an optimal pulse repetition frequency and pulse number. Furthermore, this work provides a new understanding of the mechanism for repetitive plasma ignition and insights for the optimization of plasma ignition in a reactive flow.

42 ENGINEERING↗

Low-Temperature Non-Oxidative Coupling of Methane on Atomically Dispersed Titanium–Aluminum–Boron Nanopowder

Nonoxidative coupling of methane represents a long-standing challenge in heterogeneous catalysis, as it requires activation of the carbon–hydrogen (C–H) bond, controlled carbon–carbon (C–C) bond formation, and effective hydrogen management without relying on oxidants. Here, we report a low-temperature C–H activation and nonoxidative C–C coupling of methane over atomically dispersed titanium–aluminum–boron nanopowder (Ti–Al–B NP) utilizing a catalytic microreactor coupled to synchrotron single-photon photoionization reflectron time-of-flight mass spectrometry. The soft-ionization, in situ probing method detects the nascent reaction products and radical intermediates under operando conditions, including methyl radical, C2 hydrocarbons, and molecular hydrogen. Methane activation is initiated at 800 K, approximately 700 K below the gas-phase decomposition threshold, leading predominantly to ethylene formation with selectivity reaching up to 78% among the C–C coupled products. Electronic structure calculations on model Ti–Al–B clusters elucidate a cooperative catalytic mechanism in which titanium enables methane adsorption and C–H activation, boron acts as a reversible hydrogen reservoir, and aluminum stabilizes methylene intermediates, thereby facilitating selective C–C coupling and dehydrogenation. These findings establish a distinct catalyst architecture for nonoxidative methane coupling based on earth abundant elements alternative to expensive platinum and other noble metal-containing conventional catalysts and provide molecular-level design principles for controlling dehydrogenation and subsequent C–C bond formation in challenging light alkane conversions.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Heterogeneity in Warm‐Season Land‐Atmosphere Coupling Over the U.S. Southern Great Plains

Abstract Heterogeneity in warm‐season (May–August) land‐atmosphere (LA) coupling is quantified with the long‐time, multiple‐station measurements from the U.S. Department of Energy Atmospheric Radiation Measurement (ARM) program and the Moderate Resolution Imaging Spectroradiometer satellite remote sensing at the Southern Great Plains (SGP). We examine the coupling strength at seven additional locations with the same surface type (i.e., pasture/grassland) as the ARM SGP central facility (CF). To simultaneously consider multiple factors and consistently quantify their relative contributions, we apply a multiple linear regression method to correlate the surface evaporative fraction (EF) with near‐surface soil moisture (SM) and leaf area index (LAI). The observations show moderate to weak terrestrial segment LA coupling with large heterogeneity across the ARM SGP domain in warm season. Large spatial variabilities in the contributions from SM and LAI to the EF changes are also found. The coupling heterogeneities appear to be associated with differences in land use, anthropogenic activities, rooting depth, and soil type at different stations. Therefore, the complex LA interactions at the SGP cannot be well represented by those at the CF/E13 based on the metrics applied here. Overall, the LAI exerts more influence on the EF than does the SM due to its overwhelming impacts on the latent heat flux. This study complements previous studies based on measurements only from the CF and has important implications for modeling LA coupling in weather and climate models. The multiple linear regression provides a more comprehensive measure of the integrated impacts on LA coupling from several different factors.

54 ENVIRONMENTAL SCIENCES↗

Perspectives on Geospace Plasma Coupling

There are a large variety of fascinating and instructive aspects to examining the coupling of mass and energy from the solar wind into the Earth's magnetosphere. Past research has suggested that magnetic reconnection (in a fluid sense) on the day-side magnetopause plays the key role in controlling the energy coupling. However, both linear and nonlinear coupling processes involving kinetic effects have been suggested through various types of innovative data analysis. Analysis and modeling results have also indicated a prominent role for multi-scale processes of plasma coupling. Examples include evidence of control by solar wind turbulence in the coupling sequence and localized (finite gyroradius) effects in dayside plasma transport. In this paper we describe several solar wind-magnetosphere coupling scenarios. We particularly emphasize the study of solar wind driving of magnetospheric substorm, and related geomagnetic disturbances.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Electron/phonon coupling in group-IV transition-metal and rare-earth nitrides

Transport electron/phonon coupling parameters and Eliashberg spectral functions α{sub tr}{sup 2}F(ℏω) are determined for group-IV transition-metal (TM) nitrides TiN, ZrN, and HfN, and the rare-earth (RE) nitride CeN using an inversion procedure based upon temperature-dependent (4 < T < 300 K) resistivity measurements of high-crystalline-quality stoichiometric epitaxial films grown on MgO(001) by magnetically-unbalanced reactive magnetron sputtering. Transport electron/phonon coupling parameters λ{sub tr} vary from 1.11 for ZrN to 0.82 for HfN, 0.73 for TiN, and 0.44 for CeN. The small variation in λ{sub tr} among the TM nitrides and the weak coupling in CeN are consistent with measured superconducting transition temperatures 10.4 (ZrN), 9.18 (HfN), 5.35 (TiN), and <4 K for CeN. The Eliashberg spectral function describes the strength and energy spectrum of electron/phonon coupling in conventional superconductors. Spectral peaks in α{sup 2}F(ℏω), corresponding to regions in energy-space for which electrons couple to acoustic ℏω{sub ac} and optical ℏω{sub op} phonon modes, are centered at ℏω{sub ac} = 33 and ℏω{sub op} = 57 meV for TiN, 25 and 60 meV for ZrN, 18 and 64 meV for HfN, and 21 and 39 meV for CeN. The acoustic modes soften with increasing cation mass; optical mode energies remain approximately constant for the TM nitrides, but are significantly lower for the RE nitride due to a lower interatomic force constant. Optical/acoustic peak-intensity ratios are 1.15 ± 0.1 for all four nitrides, indicating similar electron/phonon coupling strengths α{sub tr}(ℏω) for both modes.

36 MATERIALS SCIENCE↗

Antenna-coupled microcavities for terahertz emission

We have investigated the capacitive coupling between dipolar antennas and metal-dielectric-metal wire microcavities with strong sub-wavelength confinement in the terahertz region. The coupling appears in reflectivity measurements performed on arrays of antenna-coupled elements, which display asymmetric Fano lineshapes. The experimental data are compared to a temporal coupled-mode theory and finite elements electromagnetic simulations. We show that the Fano interferences correspond to coupling between a subradiant mode (microcavity) and a superradiant mode (antennas). This phenomenon allows one to enhance and control the radiative coupling of the strongly confined mode with the vacuum. These concepts are very useful for terahertz optoelectronic devices based on deep-sub-wavelength active regions.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Calculation of nuclear spin-spin coupling constants using frozen density embedding

We present a method for a subsystem-based calculation of indirect nuclear spin-spin coupling tensors within the framework of current-spin-density-functional theory. Our approach is based on the frozen-density embedding scheme within density-functional theory and extends a previously reported subsystem-based approach for the calculation of nuclear magnetic resonance shielding tensors to magnetic fields which couple not only to orbital but also spin degrees of freedom. This leads to a formulation in which the electron density, the induced paramagnetic current, and the induced spin-magnetization density are calculated separately for the individual subsystems. This is particularly useful for the inclusion of environmental effects in the calculation of nuclear spin-spin coupling constants. Neglecting the induced paramagnetic current and spin-magnetization density in the environment due to the magnetic moments of the coupled nuclei leads to a very efficient method in which the computationally expensive response calculation has to be performed only for the subsystem of interest. We show that this approach leads to very good results for the calculation of solvent-induced shifts of nuclear spin-spin coupling constants in hydrogen-bonded systems. Also for systems with stronger interactions, frozen-density embedding performs remarkably well, given the approximate nature of currently available functionals for the non-additive kinetic energy. As an example we show results for methylmercury halides which exhibit an exceptionally large shift of the one-bond coupling constants between {sup 199}Hg and {sup 13}C upon coordination of dimethylsulfoxide solvent molecules.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Experimental characterization and modeling of non-linear coupling of the LHCD power on Tore Supra

To achieve steady state operation on future tokamaks, in particular on ITER, the unique capability of a LHCD system to efficiently drive off-axis non-inductive current is needed. In this context, it is of prime importance to study and master the coupling of LH wave to the core plasma at high power density (tens of MW/m{sup 2}). In some specific conditions, deleterious effects on the LHCD coupling are sometimes observed on Tore Supra. At high power the waves may modify the edge parameters that change the wave coupling properties in a non-linear manner. In this way, dedicated LHCD experiments have been performed using the LHCD system of Tore Supra, composed of two different conceptual designs of launcher: the Fully Active Multijunction (FAM) and the new Passive Active Multijunction (PAM) antennas. A nonlinear interaction between the electron density and the electric field has been characterized in a thin plasma layer in front of the two LHCD antennas. The resulting dependence of the power reflection coefficient with the LHCD power, leading occasionally to trips in the output power, is not predicted by the standard linear theory of the LH wave coupling. Therefore, it is important to investigate and understand the possible origin of such non-linear effects in order to avoid their possible deleterious consequences. The PICCOLO-2D code, which self-consistently treats the wave propagation in the antenna vicinity and its interaction with the local edge plasma density, is used to simulate Tore Supra discharges. The simulation reproduces very well the occurrence of a non-linear behavior in the coupling observed in the LHCD experiments. The important differences and trends between the FAM and the PAM antennas, especially a larger increase in RC for the FAM, are also reproduced by the PICCOLO-2D simulation. The working hypothesis of the contribution of the ponderomotive effect in the non-linear observations of LHCD coupling is therefore validated through this comprehensive modeling for the first time on the FAM and PAM antennas on Tore Supra.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Tailoring interlayer coupling and coercivity in Co/Mn/Co trilayers by controlling the interface roughness

Epitaxial Co/Mn/Co trilayers with a wedged Mn layer were grown on Cu(001) and studied by magneto-optical Kerr effect measurements. The bottom Co film as well as the Mn film exhibits a layer-by-layer growth mode, which allows to modify both interface roughnesses on the atomic scale by tuning the thicknesses of the films to achieve a certain filling of their topmost atomic layers. The onset of antiferromagnetic order in the Mn layer at room temperature was found at thicknesses of 4.1 (4.8) and 3.4 (4.0) atomic monolayers (ML) for a filled (half-filled) topmost atomic layer of the bottom Co film in Mn/Co bilayers and Co/Mn/Co trilayers, respectively. Magnetization loops with only one step were found for a trilayer with half-filled topmost atomic layer of the bottom Co film, while loops with two separate steps have been observed in trilayers with an integer number of atomic layers in the bottom Co film. The coercivity of the top Co film shows an oscillation with 1 ML period as a function of the Mn thickness above 10 ML, which is interpreted as the influence of the atomic-scale control of the interface roughness on the interface exchange coupling between the antiferromagnetic Mn and the top ferromagnetic (FM) Co layer. The strength of the magnetic interlayer coupling between the top and bottom Co layers through the Mn layer for an integer number of atomic layers in the bottom Co layer, deduced from minor-loop measurements, exhibits an oscillation with a period of 2 ML Mn thickness, indicative of direct exchange coupling through the antiferromagnetic Mn layer. In addition, a long-period interlayer coupling of the two FM layers with antiparallel coupling maxima at Mn thicknesses of 2.5, 8.2, and 13.7 ML is observed and attributed to indirect exchange coupling of the Rudermann-Kittel-Kasuya-Yosida type.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Interface effect in coupled quantum wells

This paper intends to theoretically investigate the effect of the interfaces on the Rashba spin splitting of two coupled quantum wells. The results show that the interface related Rashba spin splitting of the two coupled quantum wells is both smaller than that of a step quantum well which has the same structure with the step quantum well in the coupled quantum wells. And the influence of the cubic Dresselhaus spin-orbit interaction of the coupled quantum wells is larger than that of a step quantum well. It demonstrates that the spin relaxation time of the two coupled quantum wells will be shorter than that of a step quantum well. As for the application in the spintronic devices, a step quantum well may be better than the coupled quantum wells, which is mentioned in this paper.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Communication: Localized molecular orbital analysis of the effect of electron correlation on the anomalous isotope effect in the NMR spin-spin coupling constant in methane

We discuss the effect of electron correlation on the unexpected differential sensitivity (UDS) in the {sup 1}J(C–H) coupling constant of CH{sub 4} using a decomposition into contributions from localized molecular orbitals and compare with the {sup 1}J(N–H) coupling constant in NH{sub 3}. In particular, we discuss the well known fact that uncorrelated coupled Hartree-Fock (CHF) calculations are not able to reproduce the UDS in methane. For this purpose we have implemented for the first time a localized molecular orbital analysis for the second order polarization propagator approximation with coupled cluster singles and doubles amplitudes—SOPPA(CCSD) in the DALTON program. Comparing the changes in the localized orbital contributions at the correlated SOPPA and SOPPA(CCSD) levels and at the uncorrelated CHF level, we find that the latter overestimates the effect of stretching the bond between the coupled atoms on the contribution to the coupling from the localized bonding orbital between these atoms. This disturbs the subtle balance between the molecular orbital contributions, which lead to the UDS in methane.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

The temperature dependence of vibronic lineshapes: Linear electron-phonon coupling

We calculate the effect of a linear electron-phonon coupling on vibronic transitions of dye molecules of arbitrary complexity. With the assumption of known vibronic frequencies (for instance from quantum-chemical calculations), we give expressions for the absorption or emission lineshapes in a second-order cumulant expansion. We show that the results coincide with those obtained from generalized Redfield theory if one uses the time-local version of the theory and applies the secular approximation. Furthermore, the theory allows to go beyond the Huang-Rhys approximation and can be used to incorporate Dushinsky effects in the treatment of the temperature dependence of optical spectra. We consider both, a pure electron-phonon coupling independent of the molecular vibrations and a coupling bilinear in the molecular vibrational modes and the phonon coordinates. We discuss the behavior of the vibronic density of states for various models for the spectral density representing the coupling of the vibronic system to the harmonic bath. We recover some of the results that have been derived earlier for the spin-boson model and we show that the behavior of the spectral density at low frequencies determines the dominant features of the spectra. In case of the bilinear coupling between the molecular vibrations and the phonons we give analytical expressions for different spectral densities. The spectra are reminiscent of those obtained from the well known Brownian oscillator model and one finds a zero-phonon line and phonon-side bands located at vibrational frequencies of the dye. The intensity of the phonon-side bands diminishes with increasing vibrational frequencies and with decreasing coupling strength (Huang-Rhys factor). It vanishes completely in the Markovian limit where only a Lorentzian zero-phonon line is observed.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Coupling strength in Coulomb and Yukawa one-component plasmas

In a non-ideal classical Coulomb one-component plasma (OCP), all thermodynamic properties are known to depend only on a single parameter—the coupling parameter Γ. In contrast, if the pair interaction is screened by background charges (Yukawa OCP) the thermodynamic state depends, in addition, on the range of the interaction via the screening parameter κ. How to determine in this case an effective coupling parameter has been a matter of intensive debate. Here we propose a consistent approach for defining and measuring the coupling strength in Coulomb and Yukawa OCPs based on a fundamental structural quantity, the radial pair distribution function (RPDF). The RPDF is often accessible in experiments by direct observation or indirectly through the static structure factor. Alternatively, it is directly computed in theoretical models or simulations. Our approach is based on the observation that the build-up of correlation from a weakly coupled system proceeds in two steps: First, a monotonically increasing volume around each particle becomes devoid of other particles (correlation hole), and second (upon further increase of the coupling), a shell structure emerges around each particle giving rise to growing peaks of the RPDF. Using molecular dynamics simulation, we present a systematic study for the dependence of these features of the RPDF on Γ and κ and derive a simple expression for the effective coupling parameter.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Spin-phonon coupling in BaFe{sub 12}O{sub 19} M-type hexaferrite

The spin-phonon coupling in magnetic materials is due to the modulation of the exchange integral by lattice vibrations. BaFe{sub 12}O{sub 19} M-type hexaferrite, which is the most used magnetic material as permanent magnet, transforms into ferrimagnet at high temperatures, but no spin-phonon coupling was previously observed at this transition. In this letter, we investigated the temperature-dependent Raman spectra of polycrystalline BaFe{sub 12}O{sub 19} M-type hexaferrite from room temperature up to 780 K to probe spin-phonon coupling at the ferrimagnetic transition. An anomaly was observed in the position of the phonon attributed to the Fe{sup (4)}O{sub 6}, Fe{sup (5)}O{sub 6}, and Fe{sup (1)}O{sub 6} octahedra, evidencing the presence of a spin-phonon coupling in BaM in the ferrimagnetic transition at 720 K. The results also confirmed the spin-phonon coupling is different for each phonon even when they couple with the same spin configuration.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Temperature-induced sign change of the magnetic interlayer coupling in Ni/Ni{sub 25}Mn{sub 75}/Ni trilayers on Cu{sub 3}Au(001)

We investigated the magnetic interlayer coupling between two ferromagnetic (FM) Ni layers through an antiferromagnetic (AFM) Ni{sub 25}Mn{sub 75} layer and the influence of this coupling on the exchange bias phenomenon. The interlayer coupling energy of an epitaxial trilayer of 14 atomic monolayers (ML) Ni/45 ML Ni{sub 25}Mn{sub 75}/16 ML Ni on Cu{sub 3}Au(001) was extracted from minor-loop magnetization measurements using in-situ magneto-optical Kerr effect. The interlayer coupling changes from ferromagnetic to antiferromagnetic when the temperature is increased above 300 K. This sign change is interpreted as the result of the competition between an antiparallel Ruderman-Kittel-Kasuya-Yosida (RKKY)-type interlayer coupling, which dominates at high temperature, and a stronger direct exchange coupling across the AFM layer, which is present only below the Néel temperature of the AFM layer.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Resonance hybridization and near field properties of strongly coupled plasmonic ring dimer-rod nanosystem

Combined effects of polarization, split gap, and rod width on the resonance hybridization and near field properties of strongly coupled gold dimer-rod nanosystem are comparatively investigated in the light of the constituent nanostructures. By aligning polarization of the incident light parallel to the long axis of the nanorod, introducing small split gaps to the dimer walls, and varying width of the nanorod, we have simultaneously achieved resonance mode coupling, huge near field enhancement, and prolonged plasmon lifetime. As a result of strong coupling between the nanostructures and due to an intense confinement of near fields at the split and dimer-rod gaps, the extinction spectrum of the coupled nanosystem shows an increase in intensity and blueshift in wavelength. Consequently, the near field lifespan of the split-nanosystem is prolonged in contrast to the constituent nanostructures and unsplit-nanosystem. On the other hand, for polarization of the light perpendicular to the long axis of the nanorod, the effect of split gap on the optical responses of the coupled nanosystem is found to be insignificant compared to the parallel polarization. These findings and such geometries suggest that coupling an array of metallic split-ring dimer with long nanorod can resolve the huge radiative loss problem of plasmonic waveguide. In addition, the Fano-like resonances and immense near field enhancements at the split and dimer-rod gaps imply the potentials of the nanosystem for practical applications in localized surface plasmon resonance spectroscopy and sensing.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗