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Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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At least 487 records · Page 27
All sourcesNASA NTRSDOE OSTI
DOE OSTI2023

Bandwidth Control and Symmetry Breaking in a Mott‐Hubbard Correlated Metal

Abstract In Mott materials strong electron correlation yields a spectrum of complex electronic structures. Recent synthesis advancements open realistic opportunities for harnessing Mott physics to design transformative devices. However, a major bottleneck in realizing such devices remains the lack of control over the electron correlation strength. This stems from the complexity of the electronic structure, which often veils the basic mechanisms underlying the correlation strength. This study presents control of the correlation strength by tuning the degree of orbital overlap using picometer‐scale lattice engineering. This study illustrates how bandwidth control and concurrent symmetry breaking can govern the electronic structure of a correlated SrVO 3 model system. This study shows how tensile and compressive biaxial strain oppositely affect the SrVO 3 in‐plane and out‐of‐plane orbital occupancy, resulting in the partial alleviation of the orbital degeneracy. The spectral weight redistribution under strain is derived and explained, which illustrates how high tensile strain drives the system toward a Mott insulating state. Implementation of such concepts can push correlated electron phenomena closer toward new solid‐state devices and circuits. These findings therefore pave the way for understanding and controlling electron correlation in a broad range of functional materials, driving this powerful resource for novel electronics closer toward practical realization.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2020

Measurement of D 0 -meson + hadron two-dimensional angular correlations in Au + Au collisions at s N N = 200 GeV

Open heavy flavor hadrons provide unique probes of the medium produced in ultra-relativistic heavy-ion collisions. Due to their increased mass relative to light-flavor hadrons, long lifetime, and early production in hard-scattering interactions, they provide access to the full evolution of the partonic medium formed in heavy-ion collisions. This paper reports two-dimensional (2D) angular correlations between neutral D-mesons and unidentified charged particles produced in minimum-bias Au+Au collisions at s N N = 200 GeV. D 0 and D 0 ¯ mesons are reconstructed via their weak decay to K ∓ π ± using the Heavy Flavor Tracker (HFT) in the Solenoidal Tracker at RHIC (STAR) experiment. Correlations on relative pseudorapidity and azimuth (Δη,ΔΦ) are presented for peripheral, mid-central and central collisions with D 0 transverse momentum from 2 to 10 GeV/c. Attention is focused on the 2D peaked correlation structure near the triggered D 0 -meson, the {\em near-side} (NS) peak, which serves as a proxy for a charm-quark containing jet. The correlated NS yield of charged particles per D 0 -meson and the 2D widths of the NS peak increase significantly from peripheral to central collisions. These results are compared with similar correlations using unidentified charged particles, consisting primarily of light-flavor hadrons, at similar trigger particle momenta. Similar per-trigger yields and widths of the NS correlation peak are observed. Here, the present results provide additional evidence that D 0 -mesons undergo significant interactions with the medium formed in heavy-ion collision and show, for the first time, significant centrality evolution of the NS 2D peak in the correlations of particles associated with a heavy-flavor hadron produced in these collisions.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2016

Angular correlations of photons from solution diffraction at a free-electron laser encode molecular structure

During X-ray exposure of a molecular solution, photons scattered from the same molecule are correlated. If molecular motion is insignificant during exposure, then differences in momentum transfer between correlated photons are direct measurements of the molecular structure. In conventional small- and wide-angle solution scattering, photon correlations are ignored. This report presents advances in a new biomolecular structural analysis technique, correlated X-ray scattering (CXS), which uses angular intensity correlations to recover hidden structural details from molecules in solution. Due to its intense rapid pulses, an X-ray free electron laser (XFEL) is an excellent tool for CXS experiments. A protocol is outlined for analysis of a CXS data set comprising a total of half a million X-ray exposures of solutions of small gold nanoparticles recorded at the Spring-8 Ångström Compact XFEL facility (SACLA). From the scattered intensities and their correlations, two populations of nanoparticle domains within the solution are distinguished: small twinned, and large probably non-twinned domains. Finally, it is shown analytically how, in a solution measurement, twinning information is only accessible via intensity correlations, demonstrating how CXS reveals atomic-level information from a disordered solution of like molecules.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2014

Monotonically increasing functions of any quantum correlation can make all multiparty states monogamous

Monogamy of quantum correlation measures puts restrictions on the sharability of quantum correlations in multiparty quantum states. Multiparty quantum states can satisfy or violate monogamy relations with respect to given quantum correlations. We show that all multiparty quantum states can be made monogamous with respect to all measures. More precisely, given any quantum correlation measure that is non-monogamic for a multiparty quantum state, it is always possible to find a monotonically increasing function of the measure that is monogamous for the same state. The statement holds for all quantum states, whether pure or mixed, in all finite dimensions and for an arbitrary number of parties. The monotonically increasing function of the quantum correlation measure satisfies all the properties that are expected for quantum correlations to follow. We illustrate the concepts by considering a thermodynamic measure of quantum correlation, called the quantum work deficit.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2016

Enhancing non-local correlations in the bipartite partitions of two qubit-system with non-mutual interaction

Several quantum-mechanical correlations, notably, quantum entanglement, measurement-induced nonlocality and Bell nonlocality are studied for a two qubit-system having no mutual interaction. Analytical expressions for the measures of these quantum-mechanical correlations of different bipartite partitions of the system are obtained, for initially two entangled qubits and the two photons are in their vacuum states. It is found that the qubits-fields interaction leads to the loss and gain of the initial quantum correlations. The lost initial quantum correlations transfer from the qubits to the cavity fields. It is found that the maximal violation of Bell’s inequality is occurring when the quantum correlations of both the logarithmic negativity and measurement-induced nonlocality reach particular values. The maximal violation of Bell’s inequality occurs only for certain bipartite partitions of the system. The frequency detuning leads to quick oscillations of the quantum correlations and inhibits their transfer from the qubits to the cavity modes. It is also found that the dynamical behavior of the quantum correlation clearly depends on the qubit distribution angle.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2014

Triplet correlation functions in liquid water

Triplet correlations have been shown to play a crucial role in the transformation of simple liquids to anomalous tetrahedral fluids [M. Singh, D. Dhabal, A. H. Nguyen, V. Molinero, and C. Chakravarty, Phys. Rev. Lett. 112, 147801 (2014)]. Here we examine triplet correlation functions for water, arguably the most important tetrahedral liquid, under ambient conditions, using configurational ensembles derived from molecular dynamics (MD) simulations and reverse Monte Carlo (RMC) datasets fitted to experimental scattering data. Four different RMC data sets with widely varying hydrogen-bond topologies fitted to neutron and x-ray scattering data are considered [K. T. Wikfeldt, M. Leetmaa, M. P. Ljungberg, A. Nilsson, and L. G. M. Pettersson, J. Phys. Chem. B 113, 6246 (2009)]. Molecular dynamics simulations are performed for two rigid-body effective pair potentials (SPC/E and TIP4P/2005) and the monatomic water (mW) model. Triplet correlation functions are compared with other structural measures for tetrahedrality, such as the O–O–O angular distribution function and the local tetrahedral order distributions. In contrast to the pair correlation functions, which are identical for all the RMC ensembles, the O–O–O triplet correlation function can discriminate between ensembles with different degrees of tetrahedral network formation with the maximally symmetric, tetrahedral SYM dataset displaying distinct signatures of tetrahedrality similar to those obtained from atomistic simulations of the SPC/E model. Triplet correlations from the RMC datasets conform closely to the Kirkwood superposition approximation, while those from MD simulations show deviations within the first two neighbour shells. The possibilities for experimental estimation of triplet correlations of water and other tetrahedral liquids are discussed.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2014

Different X-ray spectral evolution for black hole X-ray binaries in dual tracks of radio-X-ray correlation

Recently, an 'outlier' track of radio-X-ray correlation was found, which is much steeper than the former universal correlation, where dual tracks were speculated to be triggered by different accretion processes. In this work, we test this issue by exploring hard X-ray spectral evolution in four black-hole X-ray binaries with multiple, quasi-simultaneous radio and X-ray observations. First, we find that hard X-ray photon indices, Γ, are negatively and positively correlated with X-ray fluxes when the X-ray flux, F{sub 3-9} {sub keV}, is below and above a critical flux, F{sub X,} {sub crit}, which are consistent with predictions of the advection-dominated accretion flow and the disk-corona model, respectively. Second, and most importantly, we find that the radio-X-ray correlations are also clearly different when the X-ray fluxes are higher and lower than the critical flux as defined by X-ray spectral evolution. The data points with F{sub 3-9} {sub keV} ≳ F{sub X,} {sub crit} have a steeper radio-X-ray correlation (F{sub X}∝F{sub R}{sup b} and b ∼ 1.1-1.4), which roughly forms the ''outlier'' track. However, the data points with anti-correlation of Γ – F{sub 3-9} {sub keV} either stay in the universal track with b ∼ 0.61 or stay in the transition track (from the universal to 'outlier' tracks or vice versa). Therefore, our results support that the universal and ''outlier'' tracks of radio-X-ray correlations are regulated by radiatively inefficient and radiatively efficient accretion model, respectively.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2015

CORRELATIONS OF DISK AND JET EMISSION DEVIATING FROM THE FUNDAMENTAL PLANE

The variability of the accretion rate, which is believed to induce the aperiodic variability of X-ray emission from disks, may affect the energy injection into a jet. In this spirit, a correlation between disk emission and jet emission can be formed even if the mean luminosity of disk emission remains constant. In this work, these correlations are found in the situation in which the luminosity of disk emission is variable and kept at a constant mean value. The obtained correlations may be shallower than that of the fundamental plane of black hole activity. In addition, the slope of correlation may increase with increasing observed frequency of jet emission. For the luminosities spaced over three days, the slope of correlation decreases with increasing black hole mass. The deviation of our found correlations from that of the fundamental plane is related to the suppression of variability in the jet emission in comparison with that in the disk emission. This mechanism may work in some sources in which shallower correlations have been reported. Moreover, it implies that luminosities used to estimate the relation of the fundamental plane should cover an appropriate timescale, in which the variability of jet emission is not significantly suppressed.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2014

Detection of thermal SZ-CMB lensing cross-correlation in Planck nominal mission data

The nominal mission maps from the Planck satellite contain a wealth of information about secondary anisotropies in the cosmic microwave background (CMB), including those induced by the thermal Sunyaev-Zel'dovich (tSZ) effect and gravitational lensing. As both the tSZ and CMB lensing signals trace the large-scale matter density field, the anisotropies sourced by these processes are expected to be correlated. We report the first detection of this cross-correlation signal, which we measure at 6.2σ significance using the Planck data. We take advantage of Planck's multifrequency coverage to construct a tSZ map using internal linear combination techniques, which we subsequently cross-correlate with the publicly-released Planck CMB lensing potential map. The cross-correlation is subject to contamination from the cosmic infrared background (CIB), which is known to correlate strongly with CMB lensing. We correct for this contamination via cross-correlating our tSZ map with the Planck 857 GHz map and confirm the robustness of our measurement using several null tests. We interpret the signal using halo model calculations, which indicate that the tSZ-CMB lensing cross-correlation is a unique probe of the physics of intracluster gas in high-redshift, low-mass groups and clusters. Our results are consistent with extrapolations of existing gas physics models to this previously unexplored regime and show clear evidence for contributions from both the one- and two-halo terms, but no statistically significant evidence for contributions from diffuse, unbound gas outside of collapsed halos. We also show that the amplitude of the signal depends rather sensitively on the amplitude of fluctuations (σ{sub 8}) and the matter density (Ω{sub m}), scaling as σ{sub 8}{sup 6.1}Ω{sub m}{sup 1.5} at ℓ = 1000. We constrain the degenerate combination σ{sub 8}(Ω{sub m}/0.282){sup 0.26} = 0.824±0.029, a result that is in less tension with primordial CMB constraints than some recent tSZ analyses. We also combine our measurement with the Planck measurement of the tSZ auto-power spectrum to demonstrate a technique that can in principle constrain both cosmology and the physics of intracluster gas simultaneously. Our detection is a direct confirmation that hot, ionized gas traces the dark matter distribution over a wide range of scales in the universe ( ∼ 0.1–50 Mpc/h)

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2023

Variation of carrier density in semimetals via short-range correlation: A case study with nickelate NdNiO 2

Carrier density is one of the key controlling factors of material properties, particularly in controlling the essential correlations in strongly correlated materials. Typically, carrier density is externally tuned by doping or gating and remains fixed below room temperature. Strangely, the carrier density in correlated semimetals is often found to vary sensitively against weak external controls such as temperature, magnetic field, and pressure. Here, we develop a realistic simulation scheme that incorporates interatomic noncollinear magnetic correlation without a long-range order. Using the recently discovered nickelate superconductor as an example, we demonstrate a rather generic low-energy mechanism that in semimetals short-range correlation can reversely modulate the carrier density as well. Such a mutual influence between correlation and carrier density provides an extra ingredient for sensitive bifurcating behavior. This special feature of correlated semimetals explains their versatile carrier density at low energy and opens up new possibilities of functionalizing these materials.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2021

Differential two-particle number and momentum correlations with the AMPT, UrQMD, and EPOS models in Pb-Pb collisions at s N N = 2.76 TeV

We report studies of charge-independent and charge-dependent two-particle differential number correlation functions, R 2 (Δη,Δφ), and transverse momentum correlation functions, P 2 (Δη,Δφ), of charged particles produced in Pb–Pb collisions at the LHC center-of-mass energy √sNN= 2.76 TeV with the UrQMD, AMPT, and EPOS models. Model calculations for R2 and P2 correlation functions are presented for inclusive charged hadrons (h ± ) in selected transverse momentum ranges and with full azimuthal coverage in the pseudorapidity range |η|<1.0. We compare these calculations for the strength, shape, and particularly the width of the correlation functions with recent measurements of these observables by the ALICE collaboration. Our analysis indicates that comparative studies of R 2 and P 2 correlation functions provide valuable insight towards the understanding of particle production in Pb–Pb collisions. We find, in particular, that these models produce quantitatively different magnitudes and shapes for these correlation functions and none reproduce the results reported by the ALICE collaboration. Accounting for quantum number conservation in models, particularly charge conservation, is mandatory to reproduce the detailed measurements of number and transverse momentum correlation functions.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2023

Measurement of the Sensitivity of Two-Particle Correlations in $\mathcal{pp}$ Collisions to the Presence of Hard Scatterings

A key open question in the study of multiparticle production in high-energy pp collisions is the relationship between the “ridge”—i.e., the observed azimuthal correlations between particles in the underlying event that extend over all rapidities—and hard or semihard scattering processes. In particular, it is not known whether jets or their soft fragments are correlated with particles in the underlying event. To address this question, two-particle correlations are measured in pp collisions at $\sqrt{s}$=13 TeV using data collected by the ATLAS experiment at the LHC, with an integrated luminosity of 15.8 pb -1 , in two different configurations. In the first case, charged particles associated with jets are excluded from the correlation analysis, while in the second case, correlations are measured between particles within jets and charged particles from the underlying event. Second-order flow coefficients, v2, are presented as a function of event multiplicity and transverse momentum. These measurements show that excluding particles associated with jets does not affect the measured correlations. Moreover, particles associated with jets do not exhibit any significant azimuthal correlations with the underlying event, ruling out hard processes contributing to the ridge.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2022

Inference for Nonparanormal Partial Correlation via Regularized Rank-Based Nodewise Regression

Abstract Partial correlation is a common tool in studying conditional dependence for Gaussian distributed data. However, partial correlation being zero may not be equivalent to conditional independence under non-Gaussian distributions. In this paper, we propose a statistical inference procedure for partial correlations under the high-dimensional nonparanormal (NPN) model where the observed data are normally distributed after certain monotone transformations. The NPN partial correlation is the partial correlation of the normal transformed data under the NPN model, which is a more general measure of conditional dependence. We estimate the NPN partial correlations by regularized nodewise regression based on the empirical ranks of the original data. A multiple testing procedure is proposed to identify the nonzero NPN partial correlations. The proposed method can be carried out by a simple coordinate descent algorithm for lasso optimization. It is easy-to-implement and computationally more efficient compared to the existing methods for estimating NPN graphical models. Theoretical results are developed to show the asymptotic normality of the proposed estimator and to justify the proposed multiple testing procedure. Numerical simulations and a case study on brain imaging data demonstrate the utility of the proposed procedure and evaluate its performance compared to the existing methods. Data used in preparation of this article were obtained from the Alzheimer's Disease Neuroimaging Initiative (ADNI) database.

97 MATHEMATICS AND COMPUTING↗
DOE OSTI2016

An efficient computational approach to model statistical correlations in photon counting x-ray detectors

Purpose: To introduce and evaluate an increment matrix approach (IMA) describing the signal statistics of energy-selective photon counting detectors including spatial–spectral correlations between energy bins of neighboring detector pixels. The importance of the occurring correlations for image-based material decomposition is studied. Methods: An IMA describing the counter increase patterns in a photon counting detector is proposed. This IMA has the potential to decrease the number of required random numbers compared to Monte Carlo simulations by pursuing an approach based on convolutions. To validate and demonstrate the IMA, an approximate semirealistic detector model is provided, simulating a photon counting detector in a simplified manner, e.g., by neglecting count rate-dependent effects. In this way, the spatial–spectral correlations on the detector level are obtained and fed into the IMA. The importance of these correlations in reconstructed energy bin images and the corresponding detector performance in image-based material decomposition is evaluated using a statistically optimal decomposition algorithm. Results: The results of IMA together with the semirealistic detector model were compared to other models and measurements using the spectral response and the energy bin sensitivity, finding a good agreement. Correlations between the different reconstructed energy bin images could be observed, and turned out to be of weak nature. These correlations were found to be not relevant in image-based material decomposition. An even simpler simulation procedure based on the energy bin sensitivity was tested instead and yielded similar results for the image-based material decomposition task, as long as the fact that one incident photon can increase multiple counters across neighboring detector pixels is taken into account. Conclusions: The IMA is computationally efficient as it required about 10{sup 2} random numbers per ray incident on a detector pixel instead of an estimated 10{sup 8} random numbers per ray as Monte Carlo approaches would need. The spatial–spectral correlations as described by IMA are not important for the studied image-based material decomposition task. Respecting the absolute photon counts and thus the multiple counter increases by a single x-ray photon, the same material decomposition performance could be obtained with a simpler detector description using the energy bin sensitivity.

60 APPLIED LIFE SCIENCES↗
DOE OSTI2016

On the optical-X-ray correlation from outburst to quiescence in low-mass X-ray binaries: the representative cases of V404 Cyg and Cen X-4

Low-mass X-ray binaries (LMXBs) show evidence of a global correlation of debated origin between X-ray and optical luminosity. We study for the first time this correlation in two transient LMXBs, the black hole (BH) V404 Cyg and the neutron star Cen X-4, over six orders of magnitude in X-ray luminosity, from outburst to quiescence. After subtracting the contribution from the companion star, the Cen X-4 data can be described by a single power-law correlation of the form L{sub opt}∝ L{sub X}{sup 0.44}, consistent with disk reprocessing. We find a similar correlation slope for V404 Cyg in quiescence (0.46) and a steeper one (0.56) in the outburst hard state of 1989. However, V404 Cyg is about 160–280 times optically brighter, at a given 3–9 keV X-ray luminosity, compared to Cen X-4. This ratio is a factor of 10 smaller in quiescence, where the normalization of the V404 Cyg correlation also changes. Once the bolometric X-ray emission is considered and the known main differences between V404 Cyg and Cen X-4 are taken into account (a larger compact object mass, accretion disk size, and the presence of a strong jet contribution in the hard state for the BH system), the two systems lie on the same correlation. In V404 Cyg, the jet dominates spectrally at optical–infrared frequencies during the hard state but makes a negligible contribution in quiescence, which may account for the change in its correlation slope and normalization. These results provide a benchmark to compare with data from the 2015 outburst of V404 Cyg and, potentially, other transient LMXBs as well.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2017

Evolutions and Calibrations of Long Gamma-Ray-burst Luminosity Correlations Revisited

Luminosity correlations of long gamma-ray bursts (GRBs) are extensively proposed as an effective complementarity to trace the Hubble diagram of the universe at high redshifts, which is of great importance to explore properties of dark energy. Recently, several empirical luminosity correlations have been statistically proposed from GRB observations. However, to treat a GRB as the distance indicator, there are two key issues: the redshift evolution of luminosity correlations and their calibrations. In this paper, we choose the Amati relation, the correlation between the peak spectra energy and the equivalent isotropic energy of GRBs (E{sub p}--E{sub iso}) as an example and find that the current GRB data set implies that there could be a evolution of the luminosity correlation with respect to the redshift. Therefore, we propose an extended Amati relation with two extra redshift-dependent terms to correct the redshift evolution of the GRB relation. Second, we carefully check the reliability of the calibration method using the low-redshift GRB data. Importantly, we find that the low-redshift calibration method does not take whole correlations between Ω{sub m} and coefficients into account. Neglecting this correlation information can break the degeneracies and obtain the biased constraint on Ω{sub m}, which is very sensitive to values of parameters for the calibration. A small shift in the parameters of the “calibrated” relation could significantly change the final constraint on Ω{sub m} in the low-redshift calibration method. Finally, we simulate several GRB samples with different statistical errors and find that, in order to correctly recover the fiducial value of Ω{sub m}, using the low-redshift calibration method, we need a large number of GRB samples with high precisions.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2017

Monte Carlo sampling and correlation coefficients of critical experiments

We study the influence of calculation parameters on Monte-Carlo generated correlation coefficients of k{sub eff} values for a data set of critical experiments. The correlation coefficients can be used e.g. to reduce conservatism in bias estimations, but generally must be treated correctly if a data set includes correlations. We find that the actual value of the correlation coefficient for a given data set depends on the number of samples and the ratio of the sampling uncertainty to the Monte-Carlo uncertainty of the individual k{sub eff} calculation. We also discuss that the number of input parameters of the model to calculate the k{sub eff} values do not necessarily impact the convergence of the correlation coefficient with increasing sample number. However, we explain how varying the aforementioned parameters lead to different converged results for the correlation coefficients. The conclusion is that a correlation coefficient should not be discussed isolated but with the underlying uncertainties of both, the k{sub eff} estimation and the Monte Carlo sampling approach. The underlying modelling approach of the experimental data has to be described in detail. This should include a sensitivity analysis of the impact of input parameters on the k{sub eff} uncertainty with respect to the modelling approach.

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗
DOE OSTI2022

Dynamical electron correlation and the chemical bond. I. Covalent bonds in AH and AF (A = B–F)

Dynamical electron correlation has a major impact on the computed values of molecular properties and the energetics of molecular processes. This study focused on the effect of dynamical electron correlation on the spectroscopic constants ($R$ e , $ω$ e , $D$ e ), and potential energy curves, Δ$E$($R$), of the covalently bound AH and AF molecules, A = B–F. The changes in the spectroscopic constants (Δ$R$ e , Δ$ω$ e , Δ$D$ e ) caused by dynamical correlation are erratic and, at times, even surprising. These changes can be understood based on the dependence of the dynamical electron correlation energies of the AH and AF molecules as a function of the bond distance, i.e., Δ$E$ DEC ($R$). At large $R$, the magnitude of Δ$E$ DEC ($R$) increases nearly exponentially with decreasing $R$, but this increase slows as $R$ continues to decrease and, in many cases, even reverses at very short $R$. The changes in Δ$E$ DEC ($R$) in the region around $R$ e were as unexpected as they were surprising, e.g., distinct minima and maxima were found in the curves of Δ$E$ DEC ($R$) for the most polar molecules. The variations in Δ$E$ DEC ($R$) for $R$ ≲ $R$ e are directly correlated with major changes in the electronic structure of the molecules as revealed by a detailed analysis of the spin-coupled generalized valence bond wave function. In conclusion, the results reported here indicate that we have much to learn about the nature of dynamical electron correlation and its effect on chemical bonds and molecular properties and processes.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗