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At least 973 records · Page 54

Local Jahn-Teller distortions and orbital ordering in Ba 3 Cu 1+x Sb 2-x O 9 investigated by neutron scattering

In this study, a spin-orbital quantum liquid state is theoretically proposed in the honeycomb lattice of Ba 3 CuSb 2 O 9 , enabled by dynamic short-range correlations between the spin and orbital degrees of freedom. Using neutron diffraction, the local atomic structure of Ba 3 Cu 1+x Sb 2-x O 9 at x = 0 and 0.1 is obtained via the pair density function analysis. The results indicate that both compositions exhibit local Jahn-Teller (JT) distortions with the elongated CuO 3 octahedral configuration. In Ba 3 Cu 1.1 Sb 1.9 O 9 , JT ordering of the distorted CuO 3 octahedra gives rise to the orthorhombic symmetry with ferro-orbital order. On the other hand, in Ba 3 CuSb 2 O 9 , even though the CuO 3 octahedra are JT distorted, there is no long-range ordering hence the symmetry is hexagonal. Furthermore, the local singlet excitation at 5.8 meV observed in Ba 3 CuSb 2 O 9 below 50 K is absent in Ba 3 Cu 1.1 Sb 1.9 O 9 . Instead, an excitation at 2.5 meV is observed in the latter, which is likely associated with short-range spin order.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Parallelized traveling cluster approximation to study numerically spin-fermion models on large lattices

Lattice spin-fermion models are quite important to study correlated systems where quantum dynamics allows for a separation between slow and fast degrees of freedom. The fast degrees of freedom are treated quantum mechanically while the slow variables, generically referred to as the “spins,” are treated classically. At present, exact diagonalization coupled with classical Monte Carlo (ED + MC) is extensively used to solve numerically a general class of lattice spin-fermion problems. In this common setup, the classical variables (spins) are treated via the standard MC method while the fermion problem is solved by exact diagonalization. The “traveling cluster approximation” (TCA) is a real space variant of the ED + MC method that allows to solve spin-fermion problems on lattice sizes with up to 10 3 sites. In this paper, we present a novel reorganization of the TCA algorithm in a manner that can be efficiently parallelized. Finally, this allows us to solve generic spin-fermion models easily on 10 4 lattice sites and with some effort on 10 5 lattice sites, representing the record lattice sizes studied for this family of models.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Exact Potential Energy Surface for Molecules in Cavities

We find and analyze the exact time-dependent potential energy surface driving the proton motion for a model of cavity-induced suppression of proton-coupled electron transfer. We show how, in contrast to the polaritonic surfaces, its features directly correlate to the proton dynamics and we discuss cavity modifications of its structure responsible for the suppression. Furthermore, the results highlight the interplay between nonadiabatic effects from coupling to photons and coupling to electrons and suggest caution is needed when applying traditional dynamics methods based on polaritonic surfaces.

74 ATOMIC AND MOLECULAR PHYSICS↗

Honeycomb-Lattice Mott Insulator on Tantalum Disulphide

Effects of electron many-body interactions amplify in an electronic system with a narrow bandwidth opening a way to exotic physics. A narrow band in a two-dimensional (2D) honeycomb lattice is particularly intriguing as combined with Dirac bands and topological properties but the material realization of a strongly interacting honeycomb lattice described by the Kane-Mele-Hubbard model has not been identified. Here we report a novel approach to realize a 2D honeycomb-lattice narrow-band system with strongly interacting 5$\textit{d}$ electrons. Iin this work, we engineer a well-known triangular lattice 2D Mott insulator 1$\textit{T}$ – TaS 2 into a honeycomb lattice utilizing an adsorbate superstructure. Potassium (K) adatoms at an optimum coverage deplete one-third of the unpaired $\textit{d}$ electrons and the remaining electrons form a honeycomb lattice with a very small hopping. Ab initio calculations show extremely narrow $Z_2$ topological bands mimicking the Kane-Mele model. Electron spectroscopy detects an order of magnitude bigger charge gap confirming the substantial electron correlation as confirmed by dynamical mean field theory. It could be the first artificial Mott insulator with a finite spin Chern number.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Quantum Phase Diagram and Spontaneously Emergent Topological Chiral Superconductivity in Doped Triangular-Lattice Mott Insulators

The topological superconducting state is a highly sought-after quantum state hosting topological order and Majorana excitations. Here, in this Letter, we explore the mechanism to realize the topological superconductivity (TSC) in the doped Mott insulators with time-reversal symmetry (TRS). Through large-scale density matrix renormalization group study of an extended triangular-lattice t–J model on the six- and eight-leg cylinders, we identify a d + id-wave chiral TSC with spontaneous TRS breaking, which is characterized by a Chern number C=2 and quasi-long-range superconducting order. We map out the quantum phase diagram with by tuning the next-nearest-neighbor (NNN) electron hopping and spin interaction. In the weaker NNN-coupling regime, we identify a pseudogaplike phase with a charge stripe order coexisting with fluctuating superconductivity, which can be tuned into d -wave superconductivity by increasing the doping level and system width. The TSC emerges in the intermediate-coupling regime, which has a transition to a d-wave superconducting phase with larger NNN couplings. The emergence of the TSC is driven by geometrical frustrations and hole dynamics which suppress spin correlation and charge order, leading to a topological quantum phase transition.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

CrI 3 revisited with a many-body ab initio theoretical approach

CrI 3 has recently been shown to exhibit low-dimensional, long-range magnetic ordering from few layers to single layers of CrI 3 . The properties of CrI 3 bulk and few layered systems are uniquely defined by a combination of short-range intralayer and long-range interlayer interactions; including strong correlations, exchange and spin orbit coupling. Unfortunately, both the long-range van der Waals interactions, which are driven by dynamic, many-body electronic correlations and the competing strong intralayer correlations, present a formidable challenging for the local or semi local mean-field approximations employed in workhorse electronic structure approaches like density functional theory. In this work, we employ a sophisticated many-body approach that can simultaneously describe long- and short-range correlations. Herein, we establish that the fixed-node diffusion Monte Carlo (FNDMC) method reproduces the experimental interlayer separation distance of bulk CrI 3 for the high-temperature, monoclinic phase, with a reliable prediction of the interlayer binding energy. We subsequently employed, the FNDMC results to benchmark the accuracy of several density functional theory exchange-correlation approximations.

36 MATERIALS SCIENCE↗

Structure and Dynamics of the Liver Receptor Homolog 1–PGC1 α Complex

Peroxisome proliferator-activated gamma coactivator 1-α (PGC1α) regulates energy metabolism by directly interacting with transcription factors to modulate gene expression. Among the PGC1α binding partners is liver receptor homolog 1 (LRH-1; NR5A2), an orphan nuclear hormone receptor that controls lipid and glucose homeostasis. Although PGC1α is known to bind and activate LRH-1, mechanisms through which PGC1α changes LRH-1 conformation to drive transcription are unknown. Here, we used biochemical and structural methods to interrogate the LRH-1–PGC1α complex. Purified, full-length LRH-1, as well as isolated ligand binding domain, bound to PGC1α with higher affinity than to the coactivator, nuclear receptor coactivator-2 (Tif2), in coregulator peptide recruitment assays. We present the first crystal structure of the LRH-1–PGC1α complex, which depicts several hydrophobic contacts and a strong charge clamp at the interface between these partners. In molecular dynamics simulations, PGC1α induced correlated atomic motion throughout the entire LRH-1 activation function surface, which was dependent on charge-clamp formation. In contrast, Tif2 induced weaker signaling at the activation function surface than PGC1α but promoted allosteric signaling from the helix 6/β-sheet region of LRH-1 to the activation function surface. These studies are the first to probe mechanisms underlying the LRH-1–PGC1α interaction and may illuminate strategies for selective therapeutic targeting of PGC1α-dependent LRH-1 signaling pathways.

60 APPLIED LIFE SCIENCES↗

Necklace-structured high-harmonic generation for low-divergence, soft x-ray harmonic combs with tunable line spacing

The extreme nonlinear optical process of high-harmonic generation (HHG) makes it possible to map the properties of a laser beam onto a radiating electron wave function and, in turn, onto the emitted x-ray light. Bright HHG beams typically emerge from a longitudinal phased distribution of atomic-scale quantum antennae. Here, we form a transverse necklace-shaped phased array of linearly polarized HHG emitters, where orbital angular momentum conservation allows us to tune the line spacing and divergence properties of extreme ultraviolet and soft x-ray high-harmonic combs. The on-axis HHG emission has extremely low divergence, well below that obtained when using Gaussian driving beams, which further decreases with harmonic order. This work provides a new degree of freedom for the design of harmonic combs—particularly in the soft x-ray regime, where very limited options are available. Such harmonic beams can enable more sensitive probes of the fastest correlated charge and spin dynamics in molecules, nanoparticles, and materials.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Coherent charge hopping suppresses photoexcited small polarons in ErFeO 3 by antiadiabatic formation mechanism

Polarons are prevalent in condensed matter systems with strong electron-phonon coupling. The adiabaticity of the polaron relates to its transport properties and spatial extent. To date, only adiabatic small polaron formation has been measured following photoexcitation. The lattice reorganization energy is large enough that the first electron–optical phonon scattering event creates a small polaron without requiring substantial carrier thermalization. We measure that frustrating the iron-centered octahedra in the rare-earth orthoferrite ErFeO 3 leads to antiadiabatic polaron formation. Coherent charge hopping between neighboring Fe 3+ –Fe 2+ sites is measured with transient extreme ultraviolet spectroscopy and lasts several picoseconds before the polaron forms. The resulting small polaron formation time is an order of magnitude longer than previous measurements and indicates a shallow potential well, even in the excited state. The results emphasize the importance of considering dynamic electron-electron correlations, not just electron-phonon–induced lattice changes, for small polarons for transport, catalysis, and photoexcited applications.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Event-by-event mean p T fluctuations in pp and Pb–Pb collisions at the LHC

Event-by-event fluctuations of the mean transverse momentum of charged particles produced in pp collisions at √s = 0.9, 2.76 and 7 TeV, and Pb–Pb collisions at √ s NN = 2.76 TeV are studied as a function of the charged-particle multiplicity using the ALICE detector at the LHC. Dynamical fluctuations indicative of correlated particle emission are observed in all systems. The results in pp collisions show little dependence on collision energy. The Monte Carlo event generators PYTHIA and PHOJET are in qualitative agreement with the data. Peripheral Pb–Pb data exhibit a similar multiplicity dependence as that observed in pp. In central Pb–Pb, the results deviate from this trend, featuring a significant reduction of the fluctuation strength. The results in Pb–Pb are in qualitative agreement with previous measurements in Au–Au at lower collision energies and with expectations from models that incorporate collective phenomena.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

Mingus Discontinuous Multiphysics

Mingus provides hybrid coupled local/non-local mechanics analysis capabilities that extend several traditional methods to applications with inherent discontinuities. Its primary features include adaptations of solid mechanics, fluid dynamics and digital image correlation that naturally accommodate dijointed data or irregular solution fields by assimilating a variety of discretizations (such as control volume finite elements, peridynamics and meshless control point clouds). The goal of this software is to provide an analysis framework form multiphysics engineering problems with an integrated image correlation capability that can be used for experimental validation and model

Turner, Dan↗

NEAMS Update. Quarterly Report for January - March 2014

This quarterly report covers the following points: A fully three-dimensional smeared cracking model has been implemented and tested in BISON; DAKOTA-BISON was used to study the parameters that govern heat transfer across the fuel-cladding; Calculations of grain boundary mobility in UO 2 have been extended to high temperatures; Mesh adaptivity is being employed in MARMOT simulations to increase computational efficiency; Molecular dynamics simulations have shown correlation between atomic displacements and the anisotropic thermal conductivity in UO 2 ; The SHARP team continues to address the application of the toolkit to assembly deformations driven by reactivity feedback; The Nek5000 team has extended the low-Machnumber capability to mixtures with multiple species; The generalized cross section library has been tested for various fuel assemblies and reactor types; and The subgroup cross-section interface was successfully implemented in PROTEUS-SN (page 6).

99 GENERAL AND MISCELLANEOUS↗

Report on activities and findings under DOE grant “Collaborative research. An Interactive Multi-Model for Consensus on Climate Change”

The project takes a hierarchical approach. The supermodeling scheme was first studied exhaustively with simple systems of ordinary differential equations. Results were described in detail in the previous report. The principal findings were that 1) for highly non-linear systems, such as Lorenz-63, including systems which describe phenomena on very different (atmosphere/ocean) times scales, supermodeling is far superior to any form of output-averaging; 2) negative coefficients can be used to advantage in situations where all models err in the same way, but to different degrees; 3) an interesting variant of supermodeling, “weighted supermodeling”, is the limiting case where inter-model nudging coefficients in the originally conceived “connected supermodel” become infinite, but with fixed ratios, corresponding to a direct combination of the tendencies that appear in corresponding equations for the alternative models; 4) noise is useful for avoiding local optima in training the inter-model coefficients in the supermodel. The supermodeling scheme was then investigated with simple quasigeostrophic (QG) models. As described in the previous report, it was found that QG models on a sphere can be coupled most efficaciously by working in a basis which captures the most variance, rather than the most instability, a somewhat unexpected result that still deserves scrutiny in a broader context. Further studies (since the last report) with QG channel models addressed the central question of when supermodeling is superior to output averaging in situations where nonlinearites are less extreme than with the ODEs initially studied. It was found that for realistic variations in a parameter in the QG model, output averaging is sufficient to capture all but the most subtle quantitative and qualitative behavior. Supermodeling helps when qualitative differences between the models result from unrealistically large parameter differences, or when very detailed spatial structure of the modes of variability are of interest. Therefore, the scheme may still be useful in the case of full climate models with qualitatively different parametrization schemes. A supermodel was constructed from the intermediate-complexity SPEEDO model, a primitive equation model with ocean and land. Versions defined by different parameter choices, in a realistic range, were connected and the coefficients trained. Some improvement was found as compared to output averaging. The learning algorithm used thus far gives sub-optimal, but still useful results when the CO 2 level and other parameters are varied. Spatial structure remains to be studied. The first use of supermodeling with full climate models has been with variants of the ECHAM model that use different convection schemes. As yet the models are only connected at the ocean-atmosphere interface, where weighted combinations of fluxes from the two atmospheres are passed to a common ocean, and the weights adapted during a training period. The supermodel was surprisingly successful at avoiding unrealistic features such as the double-ITCZ (Intertropical Convergence Zone), a problem that arises in both of the two models run separately. The supermodels constructed thus far have not identified dynamical regime shifts in future climate. Thus the planned connection with the work of Tsonis on the relationship between regime shifts and synchronization/de-synchronization among the major climate modes (see U. Wisconsin report) has not yet been made. However the network analysis of the climate system, in observations and models, that was done in conjunction with that study, shows that models differ strongly from one another and from observations in regard to the dynamical structure described by correlation networks [Steinhaeuser and Tsonis 2013], providing a further justification for supermodeling. Toward a general software framework for supermodeling, three versions of CAM (the Community Atmosphere Model) at NCAR were configured for inter-model nudging using the DART (Data Assimilation Research Testbed) capability to stop and re-start models in synchrony. It was clearly established that the inter-model nudging adds almost no computational burden to the runs, but there appears to be a problem with the re-initialization software that is still being debugged. Publications: Several papers were published on the basic idea of the interactive multi-model (supermodel) including demonstrations with low-order ODEs. The last of these, a semi-philosophical review paper on the relevance of synchronization generally, encountered considerable resistance but was finally published in Entropy [Duane 2015]. A paper on the ECHAM/COSMOS supermodel, containing the most promising results so far [Shen et al. 2015] is presently under review.

58 GEOSCIENCES↗

Towards the Development of Molten Salt Reactor Multiphysics Modeling Capabilities: Depletion, Thermochemistry, Reactor Dynamics, and Species Tracking

This report documents the simulation and modeling work performed under the Nuclear Energy Advanced Modeling and Simulation (NEAMS) program, utilizing the tools and codes developed under the program. The focus in this Fiscal Year (FY) is on the depletion, thermochemistry, reactor dynamics, and species transport in MSRs. The fission products travelling in the entire primary loop is unique in MSRs. There are many physical/chemical mechanisms that can significantly affect the fission products concentration in the fuel salt, e.g., diffusion into gas bubbles, diffusion in the core moderators, deposition on the surface of structures/pipes, etc. The fission product concentration in the fuel salt can potentially affect the neutronics, system dynamics, chemical potentials, etc., so accurately predicting the fission products distribution in the primary loop is important. Under the main objective, different activities are pursued to assess the NEAMS tools applicability for a variety of areas on species transport, including the depletion analyses using Griffin (fission product source), the redox potential assessment at different depletion points, the assessment of xenon transport effect on the neutronics and reactor dynamics, a survey of correlations for calculating the mass transfer coefficient of different fission products, etc.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

The terminator "toy" chemistry test: A simple tool to assess errors in transport schemes

This test extends the evaluation of transport schemes from prescribed advection of inert scalars to reactive species. The test consists of transporting two interacting chemical species in the Nair and Lauritzen 2-D idealized flow field. The sources and sinks for these two species are given by a simple, but non-linear, "toy" chemistry that represents combination (X+X → X 2 ) and dissociation (X 2 → X+X). This chemistry mimics photolysis-driven conditions near the solar terminator, where strong gradients in the spatial distribution of the species develop near its edge. Despite the large spatial variations in each species, the weighted sum X T = X+2X 2 should always be preserved at spatial scales at which molecular diffusion is excluded. The terminator test demonstrates how well the advection–transport scheme preserves linear correlations. Chemistry–transport (physics–dynamics) coupling can also be studied with this test. Examples of the consequences of this test are shown for illustration.

58 GEOSCIENCES↗