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At least 109 records · Page 6

Theoretical study of electron correlation effects in transition metal dimers

Introduction of partially localized orbitals is shown to reduce the number of terms needed to describe the bonding in transition metal clusters. Using this formalism, it is possible to compute the various intra- and inter-atomic electron correlation contributions to the bond energy. Calculations demonstrate the relative importance of several kinds of electron correlation terms involving the 3p, 3d, and 4s electrons. Improved interaction potentials are obtained for the dimers V(2) and Cr(2) when additional correlation is added to the CAS SCF results of Walch, Bauschlicher, Roos, and Nelin (1983).

Das, G. P.↗

Cascade of electronic transitions in magic-angle twisted bilayer graphene

Magic-angle twisted bilayer graphene exhibits a variety of electronic states, including correlated insulators, superconductors and topological phases. Understanding the microscopic mechanisms responsible for these phases requires determination of the interplay between electron–electron interactions and quantum degeneracy (the latter is due to spin and valley degrees of freedom). Signatures of strong electron–electron correlations have been observed at partial fillings of the flat electronic bands in recent spectroscopic measurements, and transport experiments have shown changes in the Landau level degeneracy at fillings corresponding to an integer number of electrons per moiré unit cell. However, the interplay between interaction effects and the degeneracy of the system is currently unclear. Here in this paper we report a cascade of transitions in the spectroscopic properties of magic-angle twisted bilayer graphene as a function of electron filling, determined using high-resolution scanning tunnelling microscopy. We find distinct changes in the chemical potential and a rearrangement of the low-energy excitations at each integer filling of the moiré flat bands. These spectroscopic features are a direct consequence of Coulomb interactions, which split the degenerate flat bands into Hubbard sub-bands. We find these interactions, the strength of which we can extract experimentally, to be surprisingly sensitive to the presence of a perpendicular magnetic field, which strongly modifies the spectroscopic transitions. The cascade of transitions that we report here characterizes the correlated high-temperature parent phase from which various insulating and superconducting ground-state phases emerge at low temperatures in magic-angle twisted bilayer graphene.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Perspective on Kramers symmetry breaking and restoration in relativistic electronic structure methods for open-shell systems

Without rigorous symmetry constraints, solutions to approximate electronic structure methods may artificially break symmetry. In the case of the relativistic electronic structure, if time-reversal symmetry is not enforced in calculations of molecules not subject to a magnetic field, it is possible to artificially break Kramers degeneracy in open shell systems. This leads to a description of excited states that may be qualitatively incorrect. Despite this, different electronic structure methods to incorporate correlation and excited states can partially restore Kramers degeneracy from a broken symmetry solution. For single-reference techniques, the inclusion of double and possibly triple excitations in the ground state provides much of the needed correction. Formally, however, this imbalanced treatment of the Kramers-paired spaces is a multi-reference problem, and so methods such as complete-active-space methods perform much better at recovering much of the correct symmetry by state averaging. Using multi-reference configuration interaction, any additional corrections can be obtained as the solution approaches the full configuration interaction limit. A recently proposed “Kramers contamination” value is also used to assess the magnitude of symmetry breaking.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Global Distribution and Sources of Volatile and Nonvolatile Aerosol In the Remote Troposphere

Airborne measurements of aerosol (Condensation Nuclei, CN) and selected trace gases made in the areas of the North Atlantic Ocean during SONEX (October/November 1997), and the south tropical Pacific Ocean during PEM-Tropics A (September/October 1996) and PEM-Tropics B (March/April 1999) have been analyzed. Emphasis is on the interpretations of variations in the number densities of the fine (>17 nm) and ultrafine (>8 nm) CN in the upper troposphere (8-12 km). These data suggest that large number densities of highly volatile CN (10(exp 4)-10(exp 5)/cu cm) are present in the clean upper troposphere with highest values over the tropical1subtropical region. Through marine convection and long-distance horizontal transport, volatile CN originating from the tropical/subtropical regions can frequently impact the abundance of aerosol in the middle and upper troposphere at mid to high latitudes. Nonvolatile aerosol particles behave in a manner similar to tracers of combustion (CO) and photochemical pollution (PAN), implying a source from continental pollution of industrial or biomass burning origin. In the upper troposphere, we find that volatile and nonvolatile partials number densities are inversely correlated. An aerosol microphysical model is used to suggest that coagulation of fine volatile particles with fewer larger nonvolatile particles provides one possible mechanism for this relationship. It appears that nonvolatile particles, of principally anthropogenic origin,provide a highly efficient removal process for the fine volatile aerosol.

Singh, Hanwant B.↗

Cross-correlation between the 170 GHz survey map and the COBE differential microwave radiometer first-year maps

This letter describes results of a cross-correlation between the 170 GHz partial-sky survey, made with a 3.8 deg beam balloon-borne instrument, and the COBE DMR 'Fit Technique' reduced galaxy all-sky map with a beam of 7 deg. The strong correlation between the data sets implies that the observed structure is consistent with thermal variations in a 2.7 K emitter. A chi-square analysis applied to the correlation function rules out the assumption that there is no structure in either of the two maps. A second test shows that if the DMR map has structure but the 170 GHz map does not, the probability of obtaining the observed correlation is small. Further analyses support the assumption that both maps have structure and that the 170 GHz-DMR cross-correlation is consistent with the analogous DMR correlation function. Maps containing various combinations of noise and Harrison-Zel'dovich power spectra are simulated and correlated to reinforce the result. The correlation provides compelling evidence that both instruments have observed fluctuations consistent with anisotropies in the cosmic microwave background.

Ganga, Ken↗

Mixing across stable density interfaces in forced stratified turbulence

Understanding how turbulence enhances irreversible scalar mixing in density-stratified fluids is a central problem in geophysical fluid dynamics. While isotropic overturning regions are commonly the focus of mixing analyses, we here investigate whether significant mixing may arise in anisotropic statically stable regions of the flow. Focusing on a single forced direct numerical simulation of stratified turbulence, we analyse spatial correlations between the vertical density gradient $\partial \rho /\partial z$ and the dissipation rates of kinetic energy $\epsilon$ and scalar variance $\chi$ , the latter quantifying scalar mixing. The domain is characterized by relatively well-mixed density layers separated by sharp stable interfaces that are correlated with high vertical shear. While static instability is most prevalent within the mixed layers, much of the scalar mixing is localized to the intervening interfaces, a phenomenon not apparent if considering local static instability or $\epsilon$ alone. While the majority of the domain is characterized by the canonical flux coefficient $\varGamma \equiv \chi /\epsilon =0.2$ , often assumed in ocean mixing parametrizations, extreme values of $\chi$ within the statically stable interfaces, associated with elevated $\varGamma$ , strongly skew the bulk statistics. Our findings suggest that current parametrizations of turbulent mixing may be biased by undersampling, such that the most common, but not necessarily the most significant, mixing events are overweighted. Having focused here on a single simulation of stratified turbulence, it is hoped that our results motivate a broader investigation into the role played by stable density interfaces in mixing, across a wider range of parameters and forcing schemes representative of ocean turbulence.

Couchman, Miles M. P. (ORCID:0000000246676829)↗

Ultrafast disruptive probing: Simultaneously keeping track of tens of reaction pathways

Ultrafast science depends on different implementations of the well-known pump–probe method. Here, we provide a formal description of ultrafast disruptive probing, a method in which the probe pulse disrupts a transient species that may be a metastable ion or a transient state of matter. Disruptive probing has the advantage of allowing for simultaneous tracking of the yield of tens of different processes. Our presentation includes a numerical model and experimental data on multiple products resulting from the strong-field ionization of two different molecules, partially deuterated methanol and norbornene. The correlated enhancement and depletion signals between all the different fragmentation channels offer comprehensive information on photochemical reaction pathways. In combination with ion imaging and/or coincidence momentum imaging or as complementary to atom-specific probing or ultrafast diffraction methods, disruptive probing is a particularly powerful tool for the study of strong-field laser–matter interactions.

47 OTHER INSTRUMENTATION↗

Electron-stimulated desorption study of hydrogen-exposed aluminum films

H2 adsorption of evaporated clean and H2-exposed aluminum films is investigated by using the electron-stimulated desorption (ESD) method. A strong H(+)ESD signal is observed on a freshly evaporated aluminum surface which is clean according to previously proposed cleanlines criteria. An increased H(+) yield on H2 exposure is also observed. However, the increasing rate of H(+) emission could be directly correlated with small increases in H2O partial pressure during H2 exposure. It is proposed that the oxidation of aluminum by water vapor and subsequent adsorption of H2 or water is the primary process of the enhanced high H(+) yield during H2 exposure.

Park, CH.↗

A chemical study of individual green glasses and brown glasses from 15426 - Implications for their petrogenesis

Systematic chemical analyses of individual Apollo 15 green glasses were performed in order to: (1) study chemical variations among them; (2) understand their petrogenesis and source region; and (3) study their possible relationships with mare basalts in general. Brown glasses were also analyzed in order to study their chemical variations and their petrogenetic relationships to green glasses and mare basalts. The chemical composition of green and brown glasses is shown and variation diagrams of Sc, Cr2O3, FeO, and Co abundances in green glasses are presented. Igneous fractionation, two component magma mixing, and partial melting of heterogeneous source materials are alternate scenarios to explain strong observed correlations. The composition of green glasses indicates that they were derived by partial melting of the fractionated cumulate source materials formed from a magma ocean which had experienced certain degrees of olivine and plagioclase fractional crystallization.

Ma, M.-S.↗

Element-Element Correlations Among Martian Meteorite Bulk Compositions: Peculiarities Explained(?) by Mixing, with Implications for the Composition of Mars

Most estimates of the chemical corn position of Mars' mantle and core derive from elementelement correlations bulk analyses of Martian meteorites [I-31. To use the correlations in this manner assumes implicitly that they reflect mineraVmelt fractionations (e.g., partial melting, fractional crystallization, accumulation) among a cogenetic suite of igneous rocks. However, similar correlations can zppear from mixing of chemical components, and need not imply that the components were cogenetic nor that they had an igneous origin. Several aspects of the elemental and isotopic chem istries of the Martian meteorites can be explained by mixing of geochemical components (mantle or crustal), e.g. [5,6]. Thus, it is worth asking whether mixing rektions might be seen in bulk chemical data, and (if so) whether the mixing components can be used to infer average planet or mantle compositions.

Treiman, A. H.↗

Distribution of Fe3+ and H in Minerals During Partial Melting and Metasomatism of Spinel Peridotite

Oxygen fugacity and water content are crucial parameters for many chemical and physical properties of the Earth's mantle, for example bearing on fluid type, melting initiation, and deformation. However, the exact behaviour of Fe3+ and H during melting and metasomatism is still under debate. Here, the Fe3+/ΣFe ratio (Mössbauer and EMP) and water content (FTIR) of peridotite minerals are examined in mantle xenoliths from Kilbourne Hole (KH), NM, and Dish Hill (DH), CA (USA). These spinel peridotites have compositions consistent with partial melting with variable degrees of metasomatism (undetectable to cryptic to modal). Pyroxenites also allow to examine melt-rock reactions. Bulk-rock Fe2O3 content of the KH peridotites correlates with indices of melting (positive with bulk-rock Al2O3 and Cpx Yb contents, and negative with spinel Cr#) confirming that Fe3+ behaves as an incompatible element during melting. Correlations of the Fe3+/ΣFe ratio of minerals with these indices, however, indicates that Fe3+ is incompatible in Cpx but compatible in Opx and spinel during melting. Water contents in olivine, Cpx and Opx from most KH peridotites can be explained by partial melting and correlate negatively with the Fe3+/ΣFe ratio of spinel and Opx but positively with that of Cpx. This indicates partial control of Fe3+ on the incorporation of H in pyroxene, but not related to a redox equilibrium in Cpx. The higher Fe3+/ΣFe ratio of spinel in the metasomatized KH and DH peridotites, and in the pyroxenites confirms that oxidation characterizes modal metasomatism. Metasomatism, however, is not necessarily accompanied by water addition.

Peslier, A. H.↗

A Generalized, Compactly-Supported Correlation Function for Data Assimilation Applications

Correlation functions play an essential role in modern data assimilation, where they are used to model covariances given a set of tunable parameters or applied as tapering functions to localize covariances in ensemble-based schemes. One of the most widely-used correlation functions in data assimilation is the Gaspari and Cohn (1999) piecewise-rational, compactly-supported parametric correlation function (hereafter referred to as GC99). The GC99 correlation function is useful due to its tunable cut-off parameter c and Gaussian-like shape achieved when the parameter a is set to one-half. These properties are attractive for tapering functions in data assimilation applications. However, the GC99 correlation function is homogeneous over Euclidean 3-space and isotropic when restricted to the sphere, properties that may be less than ideal for some geophysical applications. GC99 is also compactly-supported on a sphere of fixed radius, which requires tuning of the cut-off parameter c that can depend on the specific application. This work presents a generalization of the GC99 correlation function that allows the cut-off parameter c and shape parameter a to vary over space to gain more flexibility in shape while maintaining its compact support property. The function, which we call the Generalized Gaspari Cohn (GenGC) correlation function, introduces inhomogeneity in Euclidean 3-space and anisotropy when restricted to the sphere by allowing both parameters c and a to vary, as functions, over the spatial domain. The GC99 correlation function is a special case of GenGC where the functions c and a are held constant, as fixed parameters rather than functions. The GenGC correlation function also generalizes the follow-on to the work of Gaspari and Cohn (1999) presented in Gaspari et al. (2006), which allowed a to vary while keeping c fixed. We illustrate through simple one- and two-dimensional examples the variety of inhomogeneous and anisotropic correlation functions GenGC can produce by varying c and a over space, and suggest applications where they may be useful in data assimilation, such as covariance modeling or localization. In particular, we describe how the GenGC correlation function can be used to construct covariances using correlation length and variance fields derived from dynamics. For example, the correlation length field for advective dynamics is governed by a partial differential equation (PDE) in N spatial dimensions, where N is the number of space dimensions of the state. Correlation length fields can be determined from this PDE and used with GenGC to construct the corresponding correlations. We can then approximate the full covariance by rescaling by the variance, which also satisfies a PDE in N spatial dimensions for advective dynamics. Thus we can approximate the full covariance without solving the covariance PDE, which is in 2N spatial dimensions, by solving just two PDEs each in only N spatial dimensions. This approach to evolving the correlation length and variance fields, then reconstructing the correlations using GenGC, is suggested as an alternative to current methods of covariance modeling in data assimilation algorithms.

GC99↗

Low-overhead transversal fault tolerance for universal quantum computation

Fast, reliable logical operations are essential for realizing useful quantum computers. By redundantly encoding logical qubits into many physical qubits and using syndrome measurements to detect and correct errors, we can achieve low logical error rates. However, for many practical quantum error correction codes such as the surface code, owing to syndrome measurement errors, standard constructions require multiple extraction rounds—of the order of the code distance d—for fault-tolerant computation, particularly considering fault-tolerant state preparation. Here we show that logical operations can be performed fault-tolerantly with only a constant number of extraction rounds for a broad class of quantum error correction codes, including the surface code with magic state inputs and feedforward, to achieve ‘transversal algorithmic fault tolerance’. Through the combination of transversal operations7 and new strategies for correlated decoding, despite only having access to partial syndrome information, we prove that the deviation from the ideal logical measurement distribution can be made exponentially small in the distance, even if the instantaneous quantum state cannot be made close to a logical codeword because of measurement errors. We supplement this proof with circuit-level simulations in a range of relevant settings, demonstrating the fault tolerance and competitive performance of our approach. Furthermore, our work sheds new light on the theory of quantum fault tolerance and has the potential to reduce the space–time cost of practical fault-tolerant quantum computation by over an order of magnitude.

Zhou, Hengyun [QuEra Computing, Boston, MA (United↗

BPZ equations for higher degenerate fields and nonperturbative Dyson-Schwinger equations

In the two-dimensional Liouville conformal field theory, correlation functions involving a degenerate field satisfy partial differential equations due to the decoupling of the null descendant field. On the other hand, the instanton partition function of a four-dimensional N = 2 supersymmetric theory in the Ω -background at a special point of the parameter space also satisfies a partial differential equation resulting from the constraints of the gauge field configurations. This partial differential equation can be proved using the nonperturbative Dyson-Schwinger equations. We show for the next-to-simplest case that the partial differential equations obtained from two different perspectives can be identified, thereby confirming an assertion of the Bogomol’nyi-Prasad-Sommerfield/conformal field theory correspondence. Published by the American Physical Society 2024

Astronomy & Astrophysics↗

Odor intensity and characterization studies of exhaust from a turbojet engine combustor

Sensory odor tests of the exhaust from a turbojet combustor operating at simulated idle conditions were made by a human panel sniffing diluted exhaust gas. Simultaneously, samples of undiluted exhaust gas were collected on adsorbent substrates, subsequently removed by solvent flushing, and analyzed chemically by liquid chromatographic methods. The concentrations of the principal malodorous species, the aromatic (unburned fuel-related) and the oxygenated (partially burned fuel) fractions, as determined chromatographically, correlated well with the intensity of the odor as determined by sniffing. Odor intensity increased as combustion efficiency decreased. Combustor modifications which increased combustion efficiency decreased odor intensity.

Butze, H. F.↗

Odor intensity and characterization studies of exhaust from a turbojet engine combustor

Sensory odor tests of the exhaust from a turbojet combustor operating at simulated idle conditions were made by a human panel sniffing diluted exhaust gas. Simultaneously, samples of undiluted exhaust gas were collected on adsorbent substrates, subsequently removed by solvent flushing, and analyzed chemically by liquid chromatographic methods. The concentrations of the principal malodorous species, the aromatic (unburned fuel-related) and the oxygenated (partially burned fuel) fractions, as determined chromatographically, correlated well with the intensity of the odor as determined by sniffing. Odor intensity increased as combustion efficiency decreased. Combustor modifications which increased combustion efficiency decreased odor intensity.

Butze, H. F.↗

An investigation of combustion and entropy noise

The relative importance of entropy and direct combustion noise in turbopropulsion systems and the parameters upon which these noise sources depend were studied. Theory and experiment were employed to determine that at least with the apparatus used here, entropy noise can dominate combustion noise if there is a sufficient pressure gradient terminating the combustor. Measurements included combustor interior fluctuating pressure, near and far field fluctuating pressure, and combustor exit plane fluctuating temperatures, as well as mean pressures and temperatures. Analysis techniques included spectral, cross-correlation, cross power spectra, and ordinary and partial coherence analysis. Also conducted were combustor liner modification experiments to investigate the origin of the frequency content of combustion noise. Techniques were developed to extract nonpropagational pseudo-sound and the heat release fluctuation spectra from the data.

Strahle, W. C.↗

Specification-based software sizing: An empirical investigation of function metrics

For some time the software industry has espoused the need for improved specification-based software size metrics. This paper reports on a study of nineteen recently developed systems in a variety of application domains. The systems were developed by a single software services corporation using a variety of languages. The study investigated several metric characteristics. It shows that: earlier research into inter-item correlation within the overall function count is partially supported; a priori function counts, in themself, do not explain the majority of the effort variation in software development in the organization studied; documentation quality is critical to accurate function identification; and rater error is substantial in manual function counting. The implication of these findings for organizations using function based metrics are explored.

Jeffery, Ross↗