Accurate and Numerically Efficient r 2 SCAN Meta-Generalized Gradient Approximation
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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
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Testing the r 2 SCAN Density Functional for the Thermodynamic Stability of Solids with and without a van der Waals Correction
Not Available
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Electron correlation and relativistic effects in the excited states of radium monofluoride
Highly accurate and precise electronic structure calculations of heavy radioactive atoms and their molecules are important for several research areas, including chemical, nuclear, and particle physics. Ab initio quantum chemistry can elucidate structural details in these systems that emerge from the interplay of relativistic and electron correlation effects, but the large number of electrons complicates the calculations, and the scarcity of experiments prevents insightful theory-experiment comparisons. Here we report the spectroscopy of the 14 lowest excited electronic states in the radioactive molecule radium monofluoride (RaF), which is proposed as a sensitive probe for searches of new physics. The observed excitation energies are compared with state-of-the-art relativistic Fock-space coupled cluster calculations, which achieve an agreement of ≥99.64% (within ~12 meV) with experiment for all states. Guided by theory, a firm assignment of the angular momentum and term symbol is made for 10 states and a tentative assignment for 4 states. The role of high-order electron correlation and quantum electrodynamics effects in the excitation energies is studied and found to be important for all states.
73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
Enhanced sensitivity for electron affinity measurements of rare elements
The electron affinity (EA), the energy released when a neutral atom binds an additional electron, is a fundamental property of atoms that is governed by electron-electron correlations and is strongly related to an element’s chemical reactivity. However, conventional techniques for EA determination lack the experimental sensitivity to probe very scarce samples. As a result, the EA for the heaviest elements of the periodic table is entirely uncharted. Here, we present a novel technique to determine EAs through Laser Photodetachment Threshold Spectroscopy, performed in an electrostatic ion beam trap to increase the samples’ exposure to laser photons and, thus, improve the experimental signal sensitivity by three orders of magnitude. Moreover, the additional exposure time allows the use of lower-power continuous-wave narrow-band lasers that reduce uncertainties associated with broadening effects induced by the laser bandwidth. By applying this technique, we measure the EA of 35 Cl to be 3.612720(44) eV, achieving state-of-the-art precision while employing five orders of magnitude fewer anions. The demonstrated sensitivity paves the way for systematic EA measurements across isotopic chains - including isotope shifts and hyperfine splittings - and ultimately for the first direct determination of electron affinities in superheavy elements.
Maier, F. M. [Univ. of Greifswald (Germany); Europ↗
Sensitivity of the electronic and magnetic structures of cuprate superconductors to density functional approximations
Abstract We discuss the crystal, electronic, and magnetic structures of La 2− x Sr x CuO 4 (LSCO) for x = 0.0 and x = 0.25 employing 13 density functional approximations, representing the local, semi-local, and hybrid exchange-correlation approximations within the Perdew–Schmidt hierarchy. The meta-generalized gradient approximation (meta-GGA) class of functionals is found to perform well in capturing the key properties of LSCO, a prototypical high-temperature cuprate superconductor. In contrast, the localspin-density approximation, GGA, and the hybrid density functional fail to capture the metal-insulator transition under doping.
36 MATERIALS SCIENCE↗
Emergence of competing electronic states from non-integer nuclear charges
Understanding many-electron phenomena with competing near-degenerate electronic states is of fundamental importance to chemistry and condensed matter physics. One of the most significant challenges for exploring such many-electron phenomena is the necessity for large system sizes in order to realize competing states, far beyond those practical for first-principles methods. Here, we show how allowing non-integer nuclear charges expands the space of computationally tractable electron systems that host competing electronic states. The emergence of competing electronic states from non-integer nuclear charges is exemplified in the simple 2-electron H 2 molecule and used to examine the microscopic structure of doped quasi-1D cuprate chains, showing how non-integer nuclear charges can open a window for first-principles calculations of difficult many-electron phenomena.
73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
Solving tricky quantum optics problems with assistance from large language models
The capabilities of modern artificial intelligence (AI) as a “scientific collaborator” are explored by engaging it with three nuanced problems in quantum optics: state populations in optical pumping, resonant transitions between decaying states (the Burshtein effect), and degenerate mirrorless lasing. Through iterative dialogue, the authors observe that AI models–when prompted and corrected–can reason through complex scenarios, refine their answers, and provide expert-level guidance, closely resembling the interaction with an adept colleague. The findings highlight that AI can democratize access to sophisticated modeling and analysis, shifting the focus in scientific practice from technical mastery to the generation and testing of ideas, and reducing the time for completing research tasks from days to minutes.
74 ATOMIC AND MOLECULAR PHYSICS↗
Recent advances in coupled cluster computations of open-shell atomic nuclei
In this contribution, we report on recent progress in coupled-cluster simulations of open-shell atomic nuclei using interactions consistently derived from chiral effective field theory. In particular, we compare different coupled-cluster approaches by computing binding energies and electric dipole polarizabilities in medium-mass calcium isotopes.
Marino, Francesco [Johannes Gutenberg Univ., Mainz↗
Examining the order-of-limits problem and lattice constant performance of the Tao–Mo functional
In their recent communication a semi-local density functional derived from the density matrix expansion of the exchange hole localised by a general coordinate transformation. We show that the order-of-limits problem present in the functional, dismissed as harmless in the original publication, causes severe errors in predicted phase transition pressures. We also show that the claim that lattice volume prediction accuracy exceeds that of existing similar functionals was based on comparison to reference data that misses anharmonic zero-point expansion and consequently overestimates accuracy. Here, by highlighting these omissions, we give a more accurate assessment of the Tao-Mo functional and show a possible direction for resolving the order-of-limits problem.
71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
r 2 SCAN-D4: Dispersion corrected meta-generalized gradient approximation for general chemical applications
We combine a regularized variant of the strongly constrained and appropriately normed semilocal density functional with the latest generation semi-classical London dispersion correction. The resulting density functional approximation r 2 SCAN-D4 has the speed of generalized gradient approximations while approaching the accuracy of hybrid functionals for general chemical applications. We demonstrate its numerical robustness in real-life settings and benchmark molecular geometries, general main group and organo-metallic thermochemistry, and non-covalent interactions in supramolecular complexes and molecular crystals. Main group and transition metal bond lengths have errors of just 0.8%, which is competitive with hybrid functionals for main group molecules and outperforms them for transition metal complexes. The weighted mean absolute deviation (WTMAD2) on the large GMTKN55 database of chemical properties is exceptionally small at 7.5 kcal/mol. This also holds for metal organic reactions with an MAD of 3.3 kcal/mol. The versatile applicability to organic and metal–organic systems transfers to condensed systems, where lattice energies of molecular crystals are within the chemical accuracy (errors <1 kcal/mol).
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Construction of meta-GGA functionals through restoration of exact constraint adherence to regularized SCAN functionals
The strongly constrained and appropriately normed (SCAN) meta-GGA exchange–correlation functional is constructed as a chemical environment-determined interpolation between two separate energy densities: one describes single-orbital electron densities accurately and another describes slowly varying densities accurately. To conserve constraints known for the exact exchange–correlation functional, the derivatives of this interpolation vanish in the slowly varying limit. While theoretically convenient, this choice introduces numerical challenges that degrade the functional’s efficiency. We have recently reported a modification to the SCAN meta-GGA, termed restored-regularized-SCAN (r 2 SCAN) , that introduces two regularizations into SCAN, which improve its numerical performance at the expense of not recovering the fourth order term of the slowly varying density gradient expansion for exchange. Here, we show the derivation of a progression of density functional approximations [regularized SCAN (rSCAN), r++SCAN, r 2 SCAN, and r 4 SCAN] with increasing adherence to exact conditions while maintaining a smooth interpolation. The greater smoothness of r 2 SCAN seems to lead to better general accuracy than the additional exact constraint of SCAN or r 4 SCAN does.
, correlation energy↗
Exact constraints and appropriate norms in machine-learned exchange-correlation functionals
Machine learning techniques have received growing attention as an alternative strategy for developing general-purpose density functional approximations, augmenting the historically successful approach of human-designed functionals derived to obey mathematical constraints known for the exact exchange-correlation functional. More recently, efforts have been made to reconcile the two techniques, integrating machine learning and exact-constraint satisfaction. We continue this integrated approach, designing a deep neural network that exploits the exact constraint and appropriate norm philosophy to de-orbitalize the strongly constrained and appropriately normed (SCAN) functional. The deep neural network is trained to replicate the SCAN functional from only electron density and local derivative information, avoiding the use of the orbital-dependent kinetic energy density. The performance and transferability of the machine-learned functional are demonstrated for molecular and periodic systems.
Artificial neural networks↗
Morphogenesis of spin cycloids in a noncollinear antiferromagnet
Pattern formation in spin systems with continuous-rotational symmetry (CRS) provides a powerful platform to study emergent complex magnetic phases and topological defects in condensed-matter physics. However, its understanding and correlation with unconventional magnetic order along with high-resolution nanoscale imaging are challenging. Here, we employ scanning nitrogen vacancy (NV) magnetometry to unveil the morphogenesis of spin cycloids at both the local and global scales within a single ferroelectric domain of (111)-oriented BiFeO 3 , which is a noncollinear antiferromagnet, resulting in formation of a glassy labyrinthine pattern. We find that the domains of locally oriented cycloids are interconnected by an array of topological defects and exhibit isotropic energy landscape predicted by first-principles calculations. We propose that the CRS of spin-cycloid propagation directions within the (111) drives the formation of the labyrinthine pattern and the associated topological defects such as antiferromagnetic skyrmions. Unexpectedly, reversing the as-grown ferroelectric polarization from [$\overline{1}$ $\overline{1}$ $\overline{1}$] to [111] produces a noncycloidal NV image contrast which ¯ could be attributed to either the emergence of a uniformly magnetized state or a reversal of the cycloid polarity. These findings highlight that (111)-oriented BiFeO 3 is not only important for studying the fascinating subject of pattern formation but could also be utilized as an ideal platform for integrating novel topological defects in the field of antiferromagnetic spintronics.
magnetoelectric↗
Suppression of pair beam instabilities in a laboratory analogue of blazar pair cascades
The generation of dense electron–positron pair beams in the laboratory can enable direct tests of theoretical models of γ-ray bursts and active galactic nuclei. We have successfully achieved this using ultrarelativistic protons accelerated by the Super Proton Synchrotron at (CERN). In the first application of this experimental platform, the stability of the pair beam is studied as it propagates through a meter-length plasma, analogous to TeV γ-ray-induced pair cascades in the intergalactic medium. It has been argued that pair beam instabilities disrupt the cascade, thus accounting for the observed lack of reprocessed GeV emission from TeV blazars. If true, this would remove the need for a moderate strength intergalactic magnetic field to explain the observations. We find that the pair beam instability is suppressed if the beam is not perfectly collimated or monochromatic, hence the lower limit to the intergalactic magnetic field inferred from γ-ray observations of blazars is robust.
blazar jets↗
Motivations for early high-profile FRIB experiments
This white paper is the result of a collaboration by many of those that attended a workshop at the facility for rare isotope beams (FRIB), organized by the FRIB Theory Alliance (FRIB-TA), on ‘Theoretical Justifications and Motivations for Early High-Profile FRIB Experiments’. It covers a wide range of topics related to the science that will be explored at FRIB. After a brief introduction, the sections address: section 2: Overview of theoretical methods, section 3: Experimental capabilities, section 4: Structure, section 5: Near-threshold Physics, section 6: Reaction mechanisms, section 7: Nuclear equations of state, section 8: Nuclear astrophysics, section 9: Fundamental symmetries, and section 10: Experimental design and uncertainty quantification.
73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
Metrics and extrapolation of resonant magnetic perturbation thresholds for ELM suppression
This large database study of resonant magnetic perturbation (RMP) edge localized mode (ELM) suppression thresholds in the AUG, DIII-D, EAST, and KSTAR tokamaks details the key strengths and weaknesses of RMP metrics. The RMP ELM suppression database used for this work contains plasma information at the time of transition from ELMing to ELM suppressed states where a clear experimental threshold is identified. The experimental threshold distributions are compared for five metrics: (1) the island overlap width, (2) pedestal top Chirikov overlap, (3) peeling edge displacement, (4) pedestal top resonant drive, and (5) edge dominant mode overlap. The distributions, the regularity of the dependence on RMP coil currents, and the sensitivities of a given metric to equilibrium reconstruction details are compared. The overlap metric proves to be a good compromise between including the appropriate plasma response physics and maintaining a numerical robustness. This quantity does not exhibit clear power-law scalings for projection, but machine learning can assist in predicting thresholds within the existing parameter ranges and providing uncertainty quantification of those predictions. Two new first-principles models, one utilizing a threshold from the non-linear Modified Rutherford equation evaluated at the pedestal top and one utilizing the SLAYER code to calculate the linear tearing threshold from torque balance, offer possible paths to extrapolation beyond the existing database parameter space.
70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
Lifetimes of two- and four-neutron-hole states in 204 Pb and 206 Pb
The centroid-shift method was used to determine half-lives of excited levels in 204 Pb and 206 Pb. For the states with 𝐼 𝜋 = 12 + , 17 − , and 19 − in 204 Pb, values of 𝑇 1/2 = 4.9(3), 3.9(3), and 0.9(3) ns, respectively, were determined. The half-life of the 𝐼 𝜋 = 9 − level in 206 Pb was measured to be 1.1(3) ns. In 204 Pb, the 12 + state arises from two neutron holes in the 𝑖 13/2 subshell, while the 17 − and 19 − levels are built on 𝜈(𝑖$^{−3}_{13/2}$, 𝑝$^{−1}_{1/2}$) and 𝜈(𝑖$^{−3}_{13/2}$, 𝑓$^{−1}_{5/2}$) four-neutron-hole configurations, respectively. The 9 − state in 206 Pb results from a 𝜈(𝑖$^{−1}_{13/2}$, 𝑓${−1}_{5/2}$) excitation. As a result, the transition probabilities for the decay of these isomeric levels are reasonably consistent with the expected single-particle values, and these states are described well by shell-model calculations using the kshell code with the KHHE interaction.
190 ≤ A ≤ 219↗
Measurements of β -delayed proton emitters in the region of 100 Sn
An experiment on neutron-deficient nuclei in the region of doubly magic 100 Sn was carried out at the Radioactive Ion Beam Factory (RIBF) at the RIKEN Nishina Center in Japan. 𝑁 ≈ 𝑍 ≈ 50 nuclei were produced following fragmentation of an intense primary 124 Xe beam and implanted in the Advanced Implantation Detector Array silicon setup for the first study of proton-rich nuclei with this system at RIKEN. Measurements of the 𝛽-delayed proton emitter decay half-lives, branching ratios and proton energy spectra of nuclei in the region of 100 Sn were performed, with improved precision in many cases. New results for the energy spectrum of 101 Sn are presented, where a 2.03(5)-MeV peak was observed. In conclusion, these results are compared to shell-model calculations, using the recent precise measurement of the 101 In proton separation energy are presented.
Appleton, C. J. [Univ. of Edinburgh, Scotland (Uni↗