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At least 37 records · Page 2

Enhancing the accuracy of XPS calculations: Exploring hybrid basis set schemes for CVS-EOMIP-CCSD calculations

Reliable computational methodologies and basis sets for modeling x-ray spectra are essential for extracting and interpreting electronic and structural information from experimental x-ray spectra. In particular, the trade-off between numerical accuracy and computational cost due to the size of the basis set is a major challenge, since molecular orbitals undergo extreme relaxation in the core-hole state. To gain clarity on the changes in electronic structure induced by the formation of a core-hole, the use of sufficiently flexible basis for expanding the orbitals, particularly for the core region, has been shown to be essential. This work focuses on the refinement of core-hole ionized state calculations using the equation-of-motion coupled cluster family of methods through an extensive analysis on the effectiveness of “hybrid” and mixed basis sets. In this investigation, we utilize the CVS-EOMIP-CCSD method in combination and construct hybrid basis sets piecewise from readily available Dunning’s correlation consistent basis sets in order to calculate x-ray ionization energies (IEs) for a set of small gas phase molecules. Our results provide insights into the impact of basis sets on the CVS-EOMIP-CCSD calculations of K-edge IEs of first-row p-block elements. Furthermore, these insights enable us to understand more about the basis set dependence of the core IEs computed and allow us to establish a protocol for deriving reliable and cost-effective theoretical estimates for computing IEs of small molecules containing such elements.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH

Universal reduced basis for the calibration of covariant energy density functionals

The reduced basis method is used to construct a “universal” basis of Dirac orbitals that may be applicable throughout the nuclear chart to calibrate covariant energy density functionals. Relative to the successful development of a reduced basis emulator for the nonrelativistic Schrödinger equation, the Dirac equation adds an extra layer of complexity due to the existence of negative energy states, which complicates building an efficient reduced basis. However, once this problem is mitigated, the resulting reduced basis is able to accurately and efficiently reproduce the high-fidelity model at a fraction of the computational cost. We are confident that the resulting reduced basis will serve as a foundational element in developing rapid and accurate emulators. In turn, these emulators will play a critical role in the Bayesian optimization of covariant energy density functionals.

Bayesian methods

A tale of two polarization paradoxes: The diamagnetic polarization paradox

An accurate calculation of the total polarization charge density in a plasma is essential for a self-consistent determination of the electric field. Yet, the “diamagnetic polarization paradox” refers to the fact that there is a paradoxical factor of 1/2 difference between the pressure-driven “diamagnetic polarization” density calculated using real space drift theory vs action-angle space guiding center and gyrokinetic theory that has not been explained before. Here, we show that both results can be made consistent with one another. Half of the diamagnetic polarization is due to the transformation from the guiding center density to the real space density. The other half is due to the fact that, within the drift kinetic ordering assumptions, the guiding center density should be expressed as the gyroaverage of the density in the limit of vanishing Larmor radius. A comprehensive review of polarization is presented to complete the derivation, and then we derive results that are required for the polarization calculations to agree. Expressions for the diamagnetic polarization density are given that are accurate to first order in amplitude and all orders in gyroradius within the gyrokinetic theory for a constant magnetic field. Applications to Maxwell–Boltzmann particle distribution functions (PDFs), including anisotropic temperature, are presented. Local invariants, like total energy and toroidal momentum, do not generate net polarization effects; the electric and thermodynamic polarizations must precisely cancel. In contrast, anisotropic dependence on the magnetic moment generates a net polarization proportional to the temperature anisotropy. Finally, when sources are present, the equilibrium PDF is approximately the ratio of two orbit averages.

adiabatic theory

Real-Space Quantification of Exciton Localization in Acene Crystals Using Wannier Function Decomposition

Here, we introduce the Wannier function decomposition of excitons (WFDX) method to quantify exciton localization in solids within the ab initio Bethe-Salpeter equation framework. By decomposing each Bloch exciton wave function into products of single-particle electron and hole maximally localized Wannier functions, this real-space approach provides well-defined orbital- and spatial-resolved measures of both Frenkel and charge-transfer excitons at low computational cost. We apply WFDX to excitons in acene crystals, quantifying how the number of rings, the exciton spin state, and the center-of-mass momentum affect spatial localization. Additionally, we show how this real-space representation reflects structural nonsymmorphic symmetries that are hidden in standard reciprocal-space descriptions. We demonstrate how the WFDX framework can be used to efficiently interpolate exciton expansion coefficients in reciprocal-space and outline how it may facilitate evaluation of observables involving position operators, highlighting its potential as a general tool for both analyzing and computing excitonic properties in solids.

Tao, Zui [University of California, Berkeley, CA (

Many-Body Basis Set Amelioration Method for Incremental Full Configuration Interaction

Incremental full configuration interaction (iFCI) is a polynomial-cost electronic structure method that systematically approaches the FCI limit by employing the method of increments to solve the Schrödinger equation through a many-body expansion. This article introduces the many-body basis set amelioration (MBBSA) method, which is designed to allow iFCI to be applicable to larger atomic orbital basis sets. MBBSA uses a series of inexpensive iFCI calculations to approximate the correlation energy that would be found using a more expensive, highly accurate iFCI calculation. Here, when compared to standard iFCI computations on smaller molecules in triple-zeta and larger basis sets, MBBSA provides approximations to the total and relative energies within chemical accuracy. MBBSA exhibits a reduced cost of between 60-92% when compared to standard iFCI calculations, with larger systems experiencing the largest benefit. Tests of MBBSA on two reactions that involve highly correlated systems, the automerization of cyclobutadiene and a Criegee intermediate reaction, show that MBBSA has practical utility for studying realistic chemistries.

Basis sets

Multi-track reconstruction algorithm in the Mu2e experiment

The Mu2e experiment, under construction at Fermilab, will search for the neutrino-less coherent $\mu^-N\rightarrow e^-N$ conversion in the field of a $^{27}$Al nucleus. Such a process violates lepton flavor conservation. About $60\%$ of muons stopped by an $^{27}$Al nucleus will undergo nuclear capture, while about $40\%$ will decay in orbit. To quantify the conversion probability, we define $R_{\mu e}$, which is given by the ratio between the $\mu^-\rightarrow e^-$ conversion rate and the nuclear capture rate [1]: \begin{equation} R_{\mu e}= \frac{\Gamma\left(\mu^- + N\left(Z,A\right)\rightarrow e^- + N\left(Z,A\right)\right)}{\Gamma\left(\mu^- + N\left(Z,A\right)\rightarrow \nu^-_\mu + N\left(Z-1,A\right)\right)}\,. \end{equation} The upper limit on $R_{\mu e}$ is $7\cdot 10^{-13}$ at $90\%$ CL, set by the SINDRUM II experiment~\cite{SINDRUM II:limit}. The goal of the Mu2e experiment is to reach a sensitivity on $R_{\mu e}$ of $8\cdot 10^{-17}$ at $90\%$ CL. This represents a four-order of magnitude improvement over the current experimental limit. Mu2e will take its first data in 2027. The signature for the muon conversion is a monochromatic electron of $104.97$~\si{\mega\eV}/c, an energy slightly below the muon rest mass. While the main experiment goal is to reconstruct the conversion electron, i.e., an event with a single track, there are motivations to develop an efficient tracking algorithm for reconstructing more simultaneous tracks. This could better constrain the background generated by $p\bar{p}$-annihilation in the Al target and to search for other Beyond the Standard Model processes. In this paper, we present an algorithm designed to reconstruct multi-particle events.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND

Dynamical ejecta from binary neutron star mergers: Impact of a small residual eccentricity and of the equation of state implementation

Predicting the properties of the matter ejected during and after a neutron star merger is crucial to our ability to use electromagnetic observations of these mergers to constrain the masses of the neutron stars, the equation of state of dense matter, and the role of neutron star mergers in the enrichment of the Universe in heavy elements. Furthermore, our ability to reliably provide such predictions is however limited by a broad range of factors, including the finite resolution of numerical simulations, their treatment of magnetic fields, neutrinos, and neutrino-matter interactions, and the approximate modeling of the equation of state of dense matter. In this manuscript, we study specifically the role that a small residual eccentricity and different implementations of the same equation of state have on the matter ejected during the merger of a 1.3M ⊙ –1.4M ⊙ binary neutron star system. We find that a residual eccentricity e ~ 0.01, as measured ~ 4–6 orbits before merger, causes O(25%–30%) changes in the amount of ejected mass, mainly due to changes in the amount of matter ejected as a result of core bounces during merger. We note that O(1%) residual eccentricities have regularly been used in binary neutron star merger simulations as proxy for circular binaries, potentially creating an additional source of error in predictions for the mass of the dynamical ejecta.

79 ASTRONOMY AND ASTROPHYSICS

Tunable noninteracting free-energy density functionals for high-energy-density physics applications

In this work, we introduce the concept of a tunable noninteracting free-energy density functional and present two examples realized: (i) via a simple one-parameter convex combination of two existing functionals and (ii) via the construction of a generalized gradient approximation (GGA) enhancement factor that contains one free parameter and is designed to satisfy a set of incorporated constraints. Functional (i), constructed as a combination of the local Thomas–Fermi and a pseudopotential-adapted GGA for the noninteracting free-energy, has already demonstrated its practical usability for establishing the high temperature end of the equation of state of deuterium [Phys. Rev. B 104, 144104 (2021)] and CHON resin [Phys. Rev. E 106, 045207 (2022)] for inertial confinement fusion applications. Hugoniot calculations for liquid deuterium are given as another example of how the application of computationally efficient orbital-free density functional theory (OF-DFT) can be utilized with the employment of the developed functionals. Once the functionals have been tuned such that the OF-DFT Hugoniot calculation matches the Kohn–Sham solution at some low-temperature point, agreement with the reference Kohn–Sham results for the rest of the high temperature Hugoniot path is very good with relative errors for compression and pressure on the order of 2% or less.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY

Local conservation of energy in fully implicit PIC algorithms

We consider the issue of strict, fully discrete local energy conservation for a whole class of fully implicit local-charge- and global-energy-conserving particle-in-cell (PIC) algorithms. Earlier studies demonstrated these algorithms feature strict global energy conservation. However, whether a local energy conservation theorem exists (in which the local energy update is governed by a flux balance equation at every mesh cell) for these schemes is unclear. In this study, we show that a local energy conservation theorem indeed exists. We begin our analysis with the 1D electrostatic PIC model without orbit-averaging, and then generalize our conclusions to account for orbit averaging, multiple dimensions, and electromagnetic models (Darwin). In all cases, a temporally, spatially, and particle-discrete local energy conservation theorem is shown to exist, proving that these formulations (as originally proposed in the literature), in addition to being locally charge conserving and globally energy conserving, are strictly locally energy conserving as well. In contrast to earlier proofs of local conservation in the literature, which only considered continuum time, our result is valid for the fully implicit time-discrete version of all models considered, including important features such as orbit averaging. We demonstrate the local-energy-conservation property numerically with a paradigmatic numerical example.

97 MATHEMATICS AND COMPUTING

Solution of the Schrödinger equation for quasi-one-dimensional materials using helical waves

We formulate and implement a spectral method for solving the Schrödinger equation, as it applies to quasi-one-dimensional materials and structures. This allows for computation of the electronic structure of important technological materials such as nanotubes (of arbitrary chirality), nanowires, nanoribbons, chiral nanoassemblies, nanosprings and nanocoils, in an accurate, efficient and systematic manner. Our work is motivated by the observation that one of the most successful methods for carrying out electronic structure calculations of bulk/crystalline systems — the plane-wave method — is a spectral method based on eigenfunction expansion. Our scheme avoids computationally onerous approximations involving periodic supercells often employed in conventional plane-wave calculations of quasi-one-dimensional materials, and also overcomes several limitations of other discretization strategies, e.g., those based on finite differences and atomic orbitals. The basis functions in our method — called helical waves (or twisted waves) — are eigenfunctions of the Laplacian with symmetry adapted boundary conditions, and are expressible in terms of plane waves and Bessel functions in helical coordinates. We describe the setup of fast transforms to carry out discretization of the governing equations using our basis set, and the use of matrix-free iterative diagonalization to obtain the electronic eigenstates. Miscellaneous computational details, including the choice of eigensolvers, use of a preconditioning scheme, evaluation of oscillatory radial integrals and the imposition of a kinetic energy cutoff are discussed. We have implemented these strategies into a computational package called HelicES (Helical Electronic Structure). We demonstrate the utility of our method in carrying out systematic electronic structure calculations of various quasi-one-dimensional materials through numerous examples involving nanotubes, nanoribbons and nanowires. We also explore the convergence properties of our method, and assess its accuracy and computational efficiency by comparison against reference finite difference, transfer matrix method and plane-wave results. We anticipate that our method will find applications in computational nanomechanics and multiscale modeling, for carrying out transport calculations of interest to the field of semiconductor devices, and for the discovery of novel chiral phases of matter that are of relevance to the burgeoning quantum hardware industry.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND

Production of neutron-rich heavy nuclei in deep-inelastic 208 Pb + 208 Pb collisions within the stochastic mean-field theory

In deep-inelastic collisions of heavy nuclei, reaction products with a wide range of mass and charge are produced. Such collisions been considered as a possible way to produce superheavy nuclei, as an alternative to fusion reactions. To provide reliable theoretical predictions, it is desired to develop microscopic approaches that correctly and accurately describe nucleon transfer processes in dissipative collisions of heavy nuclei. The purpose of the present work is (1) to investigate the mechanism of nucleon transfers in dissipative collisions of two heavy nuclei, and (2) to explore possible pathways to produce neutron-rich heavy nuclei, through detailed theoretical analyses of fluctuations and correlations in nucleon transfers in 208 Pb + 208 Pb reactions. Three-dimensional time-dependent Hartree-Fock (TDHF) calculations are performed for the collisions of 208 Pb + 208 Pb at 𝐸 c.m. = 832, 936, and 1040 MeV, using the Skyrme SLy4d energy density functional. To calculate fluctuations and correlations in nucleon transfers, we employ the stochastic mean-field (SMF) theory, and the results are compared with another theoretical framework currently available, the time-dependent random phase approximation (TDRPA). Primary and secondary production cross sections are calculated with the SMF theory combined with a statistical model, GEMINI ++ . Using information of nucleon flow across a neck of colliding nuclei in TDHF calculations, we solve quantal diffusion equations for fluctuations and correlations in nucleon transfers based on the SMF theory. From the SMF calculations, we obtain the time evolution of diffusion coefficients as well as fluctuations and correlations in nucleon transfers for a range of initial orbital angular momenta. We compare the results of the SMF calculations with those of TDRPA, showing that TDRPA tends to predict substantially larger fluctuations and correlations in strongly damped collisions of heavy nuclei, which exhibit complex initial angular momentum dependence, while the SMF results provide almost constant (stable) values. Using the obtained fluctuations and correlations, we calculate primary and secondary production cross sections for the 208 Pb + 208 Pb collisions. From the results, we find that both lighter and heavier reaction products as compared to 208 Pb are produced for a wide region in the 𝑁−𝑍 plane as primary products, thanks to the quantal diffusion mechanism in the dissipative collisions. However, we show that cross sections for production of heavy nuclei with 𝑍 ≳ 90 or 𝑁 ≳ 135 are washed out due to secondary particle evaporation and/or fission processes. On the other hand, we find that there remain sizable cross sections for production of neutron-rich nuclei along 𝑁 = 126 with 𝑍< 82, even after secondary disintegration processes. We demonstrate that the secondary production cross sections depend weakly on incident energies, but lower (higher) energy is slightly preferred for production of nuclei with smaller (larger) atomic numbers as compared to 𝑍 = 82. Here, based on the microscopic SMF calculations, it has been shown that deep-inelastic collisions of heavy nuclei, such as 208 Pb + 208 Pb examined in this study, can be a promising means to produce neutron-rich heavy nuclei along 𝑁=126. Discrepancies between the SMF and TDRPA approaches are left unsolved for future investigations.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS

Unravelling the orbits of cluster galaxy populations according to their dominant gas ionization source

ABSTRACT We investigate the kinematical and dynamical properties of cluster galaxy populations classified according to their dominant source of gas ionization, namely: star-forming (SF) galaxies, optical active galactic nuclei (AGNs), mixed SF plus AGN ionization (transition objects, T), and quiescent (Q) galaxies. We stack 8892 member galaxies from 336 relaxed galaxy clusters to build an ensemble cluster and estimate the observed projected profiles of numerical density and velocity dispersion, $\sigma _P(R)$, of each galaxy population. The MAMPOSSt code and the Jeans equations inversion technique are used to constrain the velocity anisotropy profiles of the galaxy populations in both parametric and non-parametric ways. We find that Q (SF) galaxies display the lowest (highest) typical cluster-centric distances and velocity dispersion values. Transition galaxies are more concentrated and tend to exhibit lower velocity dispersion values than SF galaxies. Galaxies that host an optical AGN are as concentrated as Q galaxies but display velocity dispersion values similar to those of the SF population. MAMPOSSt is able to find equilibrium solutions that successfully recover the observed $\sigma _P(R)$ profile only for the Q, T, and AGN populations. We find that the orbits of all populations are consistent with isotropy in the inner regions, becoming increasingly radial with the distance from the cluster centre. These results suggest that Q galaxies are in equilibrium within their clusters, while SF galaxies have more recently arrived in the cluster environment. Finally, the T and AGN populations appear to be in an intermediate dynamical state between those of the SF and Q populations.

Valk, Greique A. (ORCID:0009000827731299)

Polarization observables in double neutral pion photoproduction

Abstract Measurements of target asymmetries and double-polarization observables for the reaction "Equation missing"<#comment/>are reported. The data were taken with the CBELSA/TAPS experiment at the ELSA facility (Bonn University) using the Bonn frozen-spin butanol ($$\hbox {C}_4\hbox {H}_9$$ C 4 H 9 OH) target, which provided transversely polarized protons. Linearly polarized photons were produced via bremsstrahlung off a diamond crystal. The data cover the photon energy range from "Equation missing"<#comment/>to "Equation missing"<#comment/>and nearly the complete angular range. The results have been included in the BnGa partial wave analysis. Experimental results and the fit agree very well. Observed systematic differences in the branching ratios for decays of "Equation missing"<#comment/>and$${\varDelta ^*}$$ Δ ∗ resonances are attributed to the internal structure of these excited nucleon states. Resonances which can be assigned to SU(6)$$\times $$ × O(3) two-oscillator configurations show larger branching ratios to intermediate states with non-zero intrinsic orbital angular momenta than resonances assigned to one-oscillator configurations.

Physics

Atmospheric pion, kaon, and muon fluxes for sub-orbital experiments

Cosmic rays interacting with the Earth's atmosphere generate extensive air showers, which produce Cherenkov, fluorescence and radio emissions. These emissions are key signatures for detection by ground-based, sub-orbital, and satellite-based telescopes aiming to study high energy cosmic ray and neutrino events. However, detectors operating at ground and balloon altitudes are also exposed to a background of atmospheric charged particles, primarily pions, kaons, and muons, that can mimic or obscure the signals from astrophysical sources. In this work, we use coupled cascade equations to calculate the atmospheric pion, kaon and muon fluxes reaching detectors at various altitudes. Our analysis focuses on energies above 10 GeV, where the influence of the Earth's magnetic field on particle trajectories is minimal. We provide angular and energy-resolved flux estimates and discuss their relevance as background for extensive air shower detection. Furthermore, our results are potentially relevant for interpreting data from current and future balloon-borne experiments such as EUSO-SPB2 and for refining trigger and veto strategies in Cherenkov and fluorescence telescopes.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS

Solution of the linear wave-particle kinetic equation for global modes of arbitrary frequency in a tokamak

The linear response of a plasma to perturbations of arbitrary frequency and wavelength is derived for any axisymmetric magnetized toroidal plasma. An explicit transformation to action-angle coordinates is achieved using orthogonal magnetic coordinates and the Littlejohn Lagrangian, establishing the validity of this result to arbitrary order in normalized Larmor radius. The global resonance condition for compressional modes is clarified in more detail than in previous works, confirming that the poloidal orbit-average of the cyclotron frequency gives the desired result at lowest order in Larmor radius. The global plasma response to the perturbation at each resonance is captured by a poloidal and gyroaverage of the perturbing potential. A “global gyroaveraging” of the potential is a natural by-product of this analysis which takes into account the changing of the magnetic field over an orbit. The resonance condition depends on two arbitrary integers which completely separately capture the effects poloidal non-uniformity and finite Larmor radius in generating sidebands. We learn that poloidal sidebands generated for compressional modes are dominated by the change in gyrofrequency over the orbit, which is very different to shear modes where the gyrofrequency only contributes via a finite Larmor radius effect. This increases the number of bounce harmonics required to compute the linear drive, giving a more complicated resonance map. An example calculation is given comparing resonance of shear and compressional modes in a published DIII-D case.

Compressional

Spin–orbit torque in a three-fold-symmetric bilayer and its effect on magnetization dynamics

Field-free switching of perpendicular magnetization has previously been observed in an epitaxial L1 1 -ordered CoPt/CuPt bilayer and attributed to spin–orbit torque (SOT) arising from the crystallographic 3m point group of the interface. Using a first-principles nonequilibrium Green's function formalism combined with the Anderson disorder model, we calculate the angular dependence of the SOT in a CoPt/CuPt bilayer and find that the magnitude of the 3m SOT is about 20% of the conventional dampinglike SOT. We further study the magnetization dynamics in perpendicularly magnetized films in the presence of 3m SOT and Dzyaloshinskii–Moriya interaction, using the equations of motion for domain wall dynamics and micromagnetic simulations. For systems where strong interfacial DMI results in the Néel character of domain walls, we find that a very large current density is required to achieve deterministic switching, because reorientation of the magnetization inside the domain wall is necessary to induce the switching asymmetry. For thicker films with relatively weak interfacial DMI and the Bloch character of domain walls, deterministic switching is possible at much smaller current densities, which may explain the recent experimental findings.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND

Prediction of the Wave Normal Angle of Proton‐Band EMIC Waves Near Geosynchronous Orbit

We investigate how the wave normal angle (WNA) and polarization of proton-band electromagnetic ion cyclotron (EMIC) waves change as they travel from their source to Earth. This paper marks a significant milestone as the first full-wave simulation of proton-band EMIC waves reflecting from the ionosphere. Our findings show that the WNA can change rapidly during propagation, primarily due to plasma inhomogeneities, such as variations in the Alfvén speed. The wave polarization is strongly related to the WNA, consistent with theory. Newly generated EMIC waves near the equator propagate with a WNA of 0° , then the WNA gradually shifts to 90° as they move toward Earth. In contrast, reflecting waves having 90° of WNA at Earth maintain a relatively larger WNA even near the magnetic equator. As a result, only the newly generated waves close to the source, where the magnetic latitude is less than approximately 20° , show left-handed polarization, while linear polarization remains dominant throughout the rest of the propagation.

EMIC wave

Hybridization of Excited Interlayer Excitons with Intralayer Excitons in Transition-Metal Dichalcogenide Heterostructures: Interplay of Orbital and Structural Symmetry

Hybridization between interlayer exciton (ILX) and intralayer excitons offers a powerful route to engineer light–matter interactions in transition-metal dichalcogenide (TMDC) heterostructures, yet the underlying mechanism and selection rules remain elusive. Here we probe exciton hybridization in MoTe2/MoSe2 heterobilayers under a tunable out-of-plane electric field and observe distinct avoided crossings in the electric-field dependent reflection spectra. We associate them with coupling between excited ILX states, including the 2p and 2s Rydberg states, and MoTe2 intralayer exciton. Supported by ab initio GW plus Bethe-Salpeter equation (GW-BSE) calculations, we identify the hybridizing states and establish optical selection rules based on the effective angular momentum of the exciton states. These findings highlight the role of excitonic binding in the observed hybridization, rather than that of simple band-mixing models, and provide a new pathway for brightening high-energy dark states.

Yao, Helen [Department of Materials Science and En