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At least 1,495 records · Page 83

Primary $\gamma$-ray intensities and $\gamma$-strength functions from discrete two-step $\gamma$-ray cascades in radiative proton-capture experiments

Background: Reaction rates of radiative capture reactions can play a crucial role in the nucleosynthesis of heavy nuclei in explosive stellar environments. These reaction rates depend strongly on $\gamma$-ray decay widths in the reaction products, which are, for nonresonant capture reactions at high excitation energies, derived from the $\gamma$-ray strength function and the nuclear level density. Recently, the ratio method was applied to primary $\gamma$ rays observed from ($\textit{d, p}$) reactions and nuclear resonance fluorescence measurements to extract the dipole strength in atomic nuclei and to test the generalized Brink-Axel hypothesis. Purpose: The purpose of this work is to apply the ratio method to primary $\gamma$-ray intensities of the 63,65 Cu($\textit{p},\gamma$) reactions to extract $\gamma$-ray strength information on the nuclei 64,66 Zn. Here, the impact of spin distribution, total $\gamma$-ray decay widths, level densities, and width fluctuations on the application of the ratio method will be discussed. Additionally, by comparing the relative $\gamma$-ray strength at different excitation energies, conclusions on the validity of the generalized Brink-Axel hypothesis can be made. Method: The radiative proton capture reaction measurements have been performed at the HORUS $\gamma$-ray spectrometer of the University of Cologne at one excitation energy for each reaction. Primary $\gamma$-ray intensities have been determined by normalizing secondary $\gamma$-ray transitions in two-step cascades using their absolute branching ratio. The ratio method was applied to the measured primary $\gamma$-ray intensities as well as to previous measurements by Erlandsson et al. at different excitation energies. Results: The relative strength function curve for 64 Zn from our measurement shows no significant deviation from the previous measurement at a different excitation energy. The same is true for 66 Zn where both measurements were at almost the same excitation energy. Absolute $\gamma$-strength function values have been obtained by normalizing the relative curves to quasiparticle random phase approximation calculations because of the absence of experimental data in the respective energy region. Conclusion: The generalized Brink-Axel hypothesis, i.e., the independence of the strength function on the excitation energy, seems to hold in the studied energy region and nuclei. The method to obtain primary $\gamma$-ray intensities from two-step cascade spectra was shown to be a valuable and sensitive tool although its uncertainties are connected to the knowledge of the low-energy level scheme of the investigated nucleus. The scaling in the ratio method should be taken with care, because the relative strength is not a simple sum of $f_{E1}$ and $f_{M1}$ but a somewhat complex linear combination dependent on the excitation energy of the nucleus.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Gauge constrained algorithm of variational discrete action theory at N = 3 for the multiorbital Hubbard model

The recently developed variational discrete action theory (VDAT) provides a systematic variational approach to the ground state of the quantum many-body problem, where the quality of the solution is controlled by an integer N, and increasing N monotonically approaches the exact solution. VDAT can be exactly evaluated in the d = ∞ multiorbital Hubbard model using the self-consistent canonical discrete action theory (SCDA), which requires a self-consistency condition for the integer time Green's functions. Previous work demonstrates that N = 3 accurately captures multiorbital Mott/Hund physics at a cost similar to the Gutzwiller approximation. Here we employ a gauge constraint to automatically satisfy the self-consistency condition of the SCDA at N = 3, yielding an even more efficient algorithm with enhanced numerical stability. We derive closed form expressions of the gauge constrained algorithm for the multiorbital Hubbard model with general density-density interactions, allowing VDAT at N = 3 to be straightforwardly applied to the seven-orbital Hubbard model. We present results and a performance analysis using N = 2 and N = 3 for the SU⁡(2⁢N orb ) Hubbard model in d = ∞ with N orb = 2–8, and compare to numerically exact dynamical mean-field theory solutions where available. Finally, the developments in this work will greatly facilitate the application of VDAT at N = 3 to strongly correlated electron materials.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Machine learning the spectral function of a hole in a quantum antiferromagnet

Understanding charge motion in a background of interacting quantum spins is a fundamental problem in quantum many-body physics. The most extensively studied model for this problem is the so-called t-t'-t''-J model, where the determination of the parameter t' in the context of cuprate superconductors is challenging. Here we present a theoretical study of the spectral functions of a mobile hole in the t-t'-t''-J model using two machine-learning techniques: K-nearest neighbor regression (KNN) and a feed-forward neural network (FFNN). We employ the self-consistent Born approximation to generate a dataset of about 1.3 x 10 5 spectral functions. Here we show that, for the forward problem, both methods allow for the accurate and efficient prediction of spectral functions, allowing, e.g., rapid searches through parameter space. Furthermore, we find that for the inverse problem (inferring Hamiltonian parameters from spectra), the FFNN can, but the KNN cannot, accurately predict the model parameters using merely the density of states. Our results suggest that it may be possible to use deep-learning methods to predict materials parameters from experimentally measured spectral functions.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Tailoring the Electronic Structures and Spectral Properties of ZnO with Irradiation Defects Generated Under Intense Electronic Excitation: A Combined Experimental and DFT Approach

Here, the relationship between the composition of the internal defect states, spectral properties, and correlated electronic structures of wurtzite zinc oxide (ZnO) crystals under 645 MeV Xe 35+ irradiation is systematically investigated, employing experimental characterizations combined with first-principle calculations. Based on the ion irradiation-induced thermal expansion and relaxation processes, the high concentration of vacancy/interstitial defects produced from the transient disordered phase in molten track states trigger photoelectric changes, as follows: i) the generation of internal defect states effectively reduces the intrinsic bandgap (3.25 eV → 2.66 eV); ii) a large number of defective active sites inhibits the recombination between electron–hole pairs, causing dark conductance and photoconductance to increase with increasing damage levels until optimal fluence is achieved. Based on the density functional theory (DFT) with the GGA + U (GGA = generalized gradient approximation) method, the defective models associated with the different electronic structures, density of states, formation energy, and the nature of the chemical bonding are established. The narrowing of the bandgap observed experimentally and the enhancement of carrier concentration originating from the internal electron defect states are qualitatively verified, therefore laying the foundation for designing future nanoscale photoelectronic devices and microelectronics applications.

36 MATERIALS SCIENCE↗

Nonequilibrium solvent effects in Born-Oppenheimer molecular dynamics for ground and excited electronic states

The effects of solvent on molecular processes such as excited state relaxation and photochemical reaction often occurs in a nonequilibrium regime. Dynamic processes such as these can be simulated using excited state molecular dynamics. In this work, we describe methods of simulating nonequilibrium solvent effects in excited state molecular dynamics using linear-response time-dependent density functional theory and apparent surface charge methods. These developments include a propagation method for solvent degrees of freedom and analytical energy gradients for the calculation of forces. Molecular dynamics of acetaldehyde in water or acetonitrile are demonstrated where the solute-solvent system is out of equilibrium due to photoexcitation and emission.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Average-atom treatment of relaxation time in x-ray Thomson scattering from warm dense matter

Here, the influence of finite relaxation times on Thomson scattering from warm dense plasmas is examined within the framework of the average-atom approximation. Presently most calculations use the collision-free Lindhard dielectric function to evaluate the free-electron contribution to the Thomson cross section. In this work, we use the Mermin dielectric function, which includes relaxation time explicitly. The relaxation time is evaluated by treating the average atom as an impurity in a uniform electron gas and depends critically on the transport cross section. The calculated relaxation rates agree well with values inferred from the Ziman formula for the static conductivity and also with rates inferred from a fit to the frequency-dependent conductivity. Transport cross sections determined by the phase-shift analysis in the average-atom potential are compared with those evaluated in the commonly used Born approximation. The Born approximation converges to the exact cross sections at high energies; however, differences that occur at low energies lead to corresponding differences in relaxation rates. The relative importance of including relaxation time when modeling x-ray Thomson scattering spectra is examined by comparing calculations of the free-electron dynamic structure function for Thomson scattering using Lindhard and Mermin dielectric functions. Applications are given to warm dense Be plasmas, with temperatures ranging from 2 to 32 eV and densities ranging from 2 to 64 g/cc.

74 ATOMIC AND MOLECULAR PHYSICS↗

Photoelectron spectra of copper oxide cluster anions from first principles methods

We present results and analyses for the photoelectron spectra of small copper oxide cluster anions (CuO – , CuO – 2 , CuO – 3 , and Cu 2 O – ). The spectra are computed using various techniques, including density functional theory (DFT) with semi-local, global hybrid, and optimally tuned range-separated hybrid functionals, as well as many-body perturbation theory within the GW approximation based on various DFT starting points. The results are compared with each other and with the available experimental data. We conclude that as in many metal-organic systems, self-interaction errors are a major issue that is mitigated by hybrid functionals. However, these need to be balanced against a strong role of non-dynamical correlation—especially in smaller, more symmetric systems—where errors are alleviated by semi-local functionals. In conclusion, the relative importance of the two phenomena, including practical ways of balancing the two constraints, is discussed in detail.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Discrete Empirical Interpolation Method Based Dynamic Load Model Reduction

Dynamic load models add significant complexity to bulk power system time-domain simulations. The complexity is due to the large number of ordinary differential equations (ODEs) introduced by the dynamic load components such as induction motors. It is challenging to derive reduced-order models (ROMs) for dynamic loads due to the nonlinear functions in their governing equations. This paper applies the discrete empirical interpolation method enhanced proper orthogonal decomposition (DEIM-POD) to approximate the full dynamic load model with the ROM that minimizes the projection error of the nonlinear functions in dynamic load ODEs onto their dominant modes. This approach only requires evaluation of nonlinear functions at selected observation points. The observation points selected by DEIM also provide information for screening critical load buses where dynamic load model parameters contribute the most to the accuracy of ROM across multiple contingencies. The proposed approach is validated on IEEE 9-bus, WECC 179-bus and 2384-bus Polish systems.

bulk power system↗

Evolution of in-medium baryon-baryon scattering cross sections and stiffness of dense nuclear matter from Bayesian analyses of FOPI proton-flow excitation functions

Within a Bayesian statistical framework using a Gaussian process (GP) emulator for an isospin-dependent Boltzmann-Uehling-Uhlenbeck (IBUU) transport model simulator of heavy-ion reactions with momentum-independent Skyrme interactions, we infer from the proton directed and elliptical flow in mid-central Au + Au reactions, measured at beam energies from 150 to 1200 MeV/nucleon by the FOPI Collaboration, the posterior probability distribution functions (PDFs) of the in-medium baryon-baryon scattering cross section (BBSCS) modification factor 𝑋 (with respect to their free-space values) and the stiffness parameter 𝐾 of dense nuclear matter. Here, we find that the most probable value of 𝑋 evolves from around 0.7 to 1.0 as the beam energy 𝐸 beam /𝐴 increases. On the other hand, the posterior PDF⁡(𝐾) may have dual peaks having roughly the same height or extended shoulders at high 𝐾 values. More quantitatively, the posterior PDF⁡(𝐾) changes from having a major peak around 220 MeV, characterizing a soft EOS in the reaction at 𝐸 beam /𝐴 = 150 MeV, to one that peaks around 320 MeV, indicating a stiff EOS in the reactions at 𝐸 beam /𝐴 higher than about 600 MeV. The transition from soft to stiff happens in mid-central Au + Au reactions at beam energies around 250 MeV/nucleon in which 𝐾 = 220 MeV and 𝐾 = 320 MeV are approximately equally probable. Altogether, the FOPI proton-flow excitation function data indicate a gradual hardening of hot and dense nuclear matter as its density and temperature increase in reactions with higher beam energies.

nuclear matter↗

Computational modeling of mixed-ligand cobalt complexes with o-quinone derivative of corannulene

The structure and energy characteristics of isomers of electrically neutral adducts of tetracoordinate cobalt complexes with o-quinone derivative of corannulene were studied quantum chemically within the density functional theory (DFT) in the UB3LYP*/6-311++G(d,p) approximation. It was shown that the framework rigidity of the redox-active ligand favors convergence of the energy levels of the high-spin and low-spin isomers of the complexes under study as compared to the o-benzoquinone-containing analogues. At the same time, steric strain in the corannulene moiety causes the stability of the adducts to reduce. A compound characterized by high stabilization energy and the ability to switch its spin states via valence tautomeric rearrangements was found by systematic variation of structural parameters of cobalt bis(chelate).

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Does DFT+U mimic hybrid density functionals?

Here, this work examines the question of how a Hubbard U correction to a local exchange–correlation functional compares with adding Hartree–Fock exchange to a local functional for both solid-state and molecular properties. We compute a solid-state property, namely the band gap, and thermochemical molecular properties, in particular main-group bond energies, transition-metal–ligand bond energies, and barrier heights, to elucidate whether the DFT+U method mimics hybrid DFT. We find that a calculation with a Hubbard U correction may or may not mimic a hybrid functional – depending on the atom, the subshell, and the property to which it is applied. For band gaps, we find that adding a Hubbard U correction to the valence d orbitals of transition metals increases the band gap, which thereby gets closer to the experimental value, while adding a Hubbard U correction to valence s or p orbitals of main group elements need not always increase the band gap. For molecular thermochemistry, we find that adding a Hubbard U correction to a local density functional need not have the same effect as adding Hartree–Fock exchange to a local density functional. For example when compared to a local DFT, hybrid DFT increases the barrier height in all cases, but DFT+U does not always increase the barrier height. For the band gaps of transition metal monoxides, the Hubbard-corrected results lowered the mean errors significantly and were comparable to what could be achieved with a much more expensive hybrid functional, but for reaction barrier heights and bond energies the Hubbard correction can lower the mean error by approximately a kcal/mol. As part of the analysis, we also compare VASP and Gaussian 09 calculations for the same density functional.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Approximation of the characteristics of ion drift in parent gas

The drift velocities of noble-gas and mercury ions in a constant homogeneous electric field are calculated using Monte Carlo simulations. The ion mobility is analyzed as a function of the field strength and gas temperature. The fitting parameters for calculating the drift velocity by the Frost formula at gas temperatures of 4.2, 77, 300, 1000, and 2000 K are obtained. A general approximate formula for the drift velocity as a function of the reduced field and gas temperature is derived.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Classical symmetries and the Quantum Approximate Optimization Algorithm

Here, we study the relationship between the Quantum Approximate Optimization Algorithm (QAOA) and the underlying symmetries of the objective function to be optimized. Our approach formalizes the connection between quantum symmetry properties of the QAOA dynamics and the group of classical symmetries of the objective function. The connection is general and includes but is not limited to problems defined on graphs. We show a series of results exploring the connection and highlight examples of hard problem classes where a nontrivial symmetry subgroup can be obtained efficiently. In particular, we show how classical objective function symmetries lead to invariant measurement outcome probabilities across states connected by such symmetries, independent of the choice of algorithm parameters or number of layers. To illustrate the power of the developed connection, we apply machine learning techniques toward predicting QAOA performance based on symmetry considerations. We provide numerical evidence that a small set of graph symmetry properties suffices to predict the minimum QAOA depth required to achieve a target approximation ratio on the MaxCut problem, in a practically important setting where QAOA parameter schedules are constrained to be linear and hence easier to optimize.

97 MATHEMATICS AND COMPUTING↗

First-Principle Study on the Origin of Ferromagnetism in Non-magnetic Halide Perovskite CsCdM{sub 3} (M = Cl and Br) Doped with B, C, and N

Based on the density functional theory (DFT), we elucidate the origin of magnetization in non-magnetic cubic halide perovskite CsCdM{sub 3} (M = Cl and Br) induced by substitution of non-magnetic 2p-impurities (B, C, and N) substitution. The calculations were done within the generalized gradient approximation (GGA) and GGA plus-modified Becke and Johnson (mBJ-GGA) as the exchange correlation. The results reveal that half-metallic ferromagnetism can be obtained for C- and N-dopings with the integer magnetic moment of 3.00 and 2.00 µ{sub B} per cell. However, B substitution does not induce magnetism in both CsCdCl{sub 3} and CsCdBr{sub 3} systems. The localized magnetic moments substantially come from impurity atoms. The origin of ferromagnetism can be attributed to the p - p hybridization between 2p-impurities and its surrounding halide atoms. Our results show that doped perovskites could provide a new promising class of materials for future spintronics applications.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Grid-based diffusion Monte Carlo for fermions without the fixed-node approximation

A diffusion Monte Carlo algorithm is introduced that can determine the correct nodal structure of the wave function of a few-fermion system and its ground-state energy without an uncontrolled bias. This is achieved by confining signed random walkers to the points of a uniform infinite spatial grid, allowing them to meet and annihilate one another to establish the nodal structure without the fixed-node approximation. An imaginary-time propagator is derived rigorously from a discretized Hamiltonian, governing a non-Gaussian, sign-flipping, branching, and mutually annihilating random walk of particles. The accuracy of the resulting stochastic representations of a fermion wave function is limited only by the grid and imaginary-time resolutions and can be improved in a controlled manner. Here, the method is tested for a series of model problems including fermions in a harmonic trap as well as the He atom in its singlet or triplet ground state. For the latter case, the energies approach from above with increasing grid resolution and converge within 0.015 E h of the exact basis-set-limit value for the grid spacing of 0.08 a.u. with a statistical uncertainty of 10 –5 E h without an importance sampling or Jastrow factor.

74 ATOMIC AND MOLECULAR PHYSICS↗

One-particle many-body Green’s function theory: Algebraic recursive definitions, linked-diagram theorem, irreducible-diagram theorem, and general-order algorithms

A thorough analytical and numerical characterization of the whole perturbation series of one-particle many-body Green’s function (MBGF) theory is presented in a pedagogical manner. Three distinct but equivalent algebraic (first-quantized) recursive definitions of the perturbation series of the Green’s function are derived, which can be combined with the well-known recursion for the self-energy. Six general-order algorithms of MBGF are developed, each implementing one of the three recursions, the ΔMPn method (where n is the perturbation order) [S. Hirata et al., J. Chem. Theory Comput. 11, 1595 (2015)], the automatic generation and interpretation of diagrams, or the numerical differentiation of the exact Green’s function with a perturbation-scaled Hamiltonian. They all display the identical, nondivergent perturbation series except ΔMPn, which agrees with MBGF in the diagonal and frequency-independent approximations at 1 ≤ n ≤ 3 but converges at the full-configuration-interaction (FCI) limit at n=∞ (unless it diverges). Numerical data of the perturbation series are presented for Koopmans and non-Koopmans states to quantify the rate of convergence towards the FCI limit and the impact of the diagonal, frequency-independent, or ΔMPn approximation. The diagrammatic linkedness and thus size-consistency of the one-particle Green’s function and self-energy are demonstrated at any perturbation order on the basis of the algebraic recursions in an entirely time-independent (frequency-domain) framework. The trimming of external lines in a one-particle Green’s function to expose a self-energy diagram and the removal of reducible diagrams are also justified mathematically using the factorization theorem of Frantz and Mills. Equivalence of ΔMPn and MBGF in the diagonal and frequency-independent approximations at 1 ≤ n ≤ 3 is algebraically proven, also ascribing the differences at n = 4 to the so-called semi-reducible and linked-disconnected diagrams

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

An efficient method to integrate polynomials over polytopes and curved solids

Here in this paper, we present an efficient approach to compute the integral of monomials and polynomials over polyhedra and regions defined by parametric curved boundary surfaces. We use Euler's theorem for homogeneous functions in combination with Stokes's theorem to reduce the integration of a monomial over a three-dimensional solid to its boundary. If the solid is a polytope, through a recursive application of these theorems, the integral is further reduced to just the evaluation of the monomial and its derivatives at the vertices of the polytope. The present approach is simpler than existing techniques that rely on repeated use of the divergence theorem, which require the antiderivative of the monomials and the projection of these functions onto hyperplanes. For convex and nonconvex polytopes, our approach does not introduce any approximation for the integration of monomials. For curved solid regions bounded by surfaces that admit a parameterization, the same approach yields simplified formulas to compute the integral of any homogeneous function, including monomials. For surfaces parameterized by polynomial surfaces (such as Bezier surface triangles and B-spline patches), the method yields machine-precision accuracy for the volumetric integration of monomials with an appropriate quadrature rule. Numerical examples over regions bounded by polynomial surfaces and rational surfaces are presented to establish the accuracy and efficiency of the method.

97 MATHEMATICS AND COMPUTING↗

Unsteady fluid flow in a slightly curved pipe: A comparative study of a matched asymptotic expansions solution with a single analytical solution

The present work is motivated by the fact that blood flow in the aorta and the main arteries is governed by large finite values of the Womersley number α and for such values of α there is not any analytical solution in the literature. The existing numerical solutions, although accurate, give limited information about the factors that affect the flow, whereas an analytical approach has an advantage in that it can provide physical insight to the flow mechanism. Having this in mind, we seek analytical solution to the equations of the fluid flow driven by a sinusoidal pressure gradient in a slightly curved pipe of circular cross section when the Womersley number varies from small finite to infinite values. Initially the equations of motion are expanded in terms of the curvature ratio δ and the resulting linearized equations are solved analytically in two ways. In the first, we match the solution for the main core to that for the Stokes boundary layer. This solution is valid for very large values of α. In the second, we derive a straightforward single solution valid to the entire flow region and for 8 ≤ α < ∞, a range which includes the values of α that refer to the physiological flows. Each solution contains expressions for the axial velocity, the stream function, and the wall stresses and is compared to the analogous forms presented in other studies. The two solutions give identical results to each other regarding the axial flow but differ in the secondary flow and the circumferential wall stress, due to the approximations employed in the matched asymptotic expansion process. The results on the stream function from the second solution are in agreement with analogous results from other numerical solutions. The second solution predicts that the atherosclerotic plaques may develop in any location around the cross section of the aortic wall unlike to the prescribed locations predicted by the first solution. In addition, it gives circumferential wall stresses augmented by approximately 100% with respect to the matched asymptotic expansions, a factor that may contribute jointly with other pathological factors to the faster aging of the arterial system and the possible malfunction of the aorta.

42 ENGINEERING↗