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At least 1,333 records · Page 74
All sourcesNASA NTRSDOE OSTI
DOE OSTI2014

THE HIGH-RESOLUTION EXTREME-ULTRAVIOLET SPECTRUM OF N{sub 2} BY ELECTRON IMPACT

We have analyzed high-resolution (FWHM = 0.2 Å) extreme-ultraviolet (EUV, 800-1350 Å) laboratory emission spectra of molecular nitrogen excited by an electron impact at 20 and 100 eV under (mostly) optically thin, single-scattering experimental conditions. A total of 491 emission features were observed from N{sub 2} electronic-vibrational transitions and atomic N I and N II multiplets and their emission cross sections were measured. Molecular emission was observed at vibrationally excited ground-state levels as high as v'' = 17, from the a {sup 1}Π {sub g} , b {sup 1}Π {sub u} , and b'{sup 1}Σ {sub u} {sup +} excited valence states and the Rydberg series c'{sub n} {sub +1} {sup 1}Σ {sub u} {sup +}, c{sub n} {sup 1}Π {sub u} , and o{sub n} {sup 1}Π {sub u} for n between 3 and 9. The frequently blended molecular emission bands were disentangled with the aid of a sophisticated and predictive quantum-mechanical model of excited states that includes the strong coupling between valence and Rydberg electronic states and the effects of predissociation. Improved model parameters describing electronic transition moments were obtained from the experiment and allowed for a reliable prediction of the vibrationally summed electronic emission cross section, including an extrapolation to unobserved emission bands and those that are optically thick in the experimental spectra. Vibrationally dependent electronic excitation functions were inferred from a comparison of emission features following 20 and 100 eV electron-impact collisional excitation. The electron-impact-induced fluorescence measurements are compared with Cassini Ultraviolet Imaging Spectrograph observations of emissions from Titan's upper atmosphere.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2025

Recent advancements in atomic many-body methods for high-precision studies of isotope shifts

The development of atomic many-body methods, capable of incorporating electron correlation effects accurately, is required for isotope shift (IS) studies. In combination with precise measurements, such calculations help to extract nuclear charge radii differences, and to probe for signatures of physics beyond the Standard Model of particle physics. Here, we review here a few recently-developed methods in the relativistic many-body perturbation theory (RMBPT) and relativistic coupled-cluster (RCC) theory frameworks for calculations of IS factors in the highly charged ions (HCIs), and neutral or singly-charged ions, respectively. The results are presented for a wide range of atomic systems in order to demonstrate the interplay between quantum electrodynamics (QED) and electron correlation effects. In view of this, we start our discussions with the RMBPT calculations for a few HCIs by rigorously treating QED effects; then we outline methods to calculate IS factors in the one-valence atomic systems using two formulations of the RCC approach. Then we present calculations for two valence atomic systems, by employing the Fock-space RCC methods. For completeness, we briefly discuss theoretical input required for the upcoming experiments, their possibilities to probe nuclear properties and implications to fundamental physics studies.

QED effects↗
DOE OSTI2017

Electronic structure of ferromagnetic heavy fermion, YbPdSi, YbPdGe, and YbPtGe studied by photoelectron spectroscopy, x-ray emission spectroscopy, and DFT + DMFT calculations

Here, the electronic structures of ferromagnetic heavy fermion Yb compounds of YbPdSi, YbPdGe, and YbPtGe are studied by photoelectron spectroscopy around the Yb 4d–4f resonance, resonant x-ray emission spectroscopy at the Yb L 3 absorption edge, and density functional theory combined with dynamical mean field theory calculations. These compounds all have a temperature-independent intermediate Yb valence with large ${\rm Yb}^{3+}$ and small ${\rm Yb}^{2+}$ components. The magnitude of the Yb valence is evaluated to be YbPtGe $<$ YbPdGe $\lesssim $ YbPdSi, suggesting that YbPtGe is the closest to the quantum critical point among the three Yb compounds. Our results support the scenario of the coexistence of heavy fermion behavior and ferromagnetic ordering which is described by a magnetically-ordered Kondo lattice where the magnitude of the Kondo effect and the RKKY interaction are comparable.

30 DIRECT ENERGY CONVERSION↗
DOE OSTI2020

Topological and thermoelectric properties of double antiperovskite pnictides

Doubling the perovskite cell (double perovskite) has been found to open new possibilities for engineering functional materials, magnetic materials in particular. This route should be applicable to the antiperovskite (aPV) class. In the pnictide based double aPV (2aPV) class introduced here magnetism is very rare, and we address them as new topological materials, possibly with thermoelectric interest. We have found that the 2aPV supercell provides a systematically larger band gap that can serve to inhibit bulk conductivity, and also large spin–orbit coupling for band inversion. We present examples from a broad study of double antiperovskites focusing on the X 6 AA'B 2 configuration, where X is the alkaline earth element and A and B are the group 5A pnictogens. We find that an 'extended s' state at the valence band minimum, described alternatively as a cation valence state or a modulated interstitial planewave state, plays a crucial role in both topological and thermoelectric properties. Several of these compounds may house topological phases, while transport calculations indicate they may also find themselves useful in thermoelectric applications.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2018

Defect induced structural inhomogeneity, ultraviolet light emission and near-band-edge photoluminescence broadening in degenerate In 2 O 3 nanowires

We demonstrate here defect induced changes on the morphology and surface properties of indium oxide (In 2 O 3 ) nanowires and further study their effects on the near-band-edge (NBE) emission, thereby showing the significant influence of surface states on In 2 O 3 nanostructure based device characteristics for potential optoelectronic applications. In 2 O 3 nanowires with cubic crystal structure (c-In 2 O 3 ) were synthesized via carbothermal reduction technique using a gold-catalyst-assisted vapor–liquid–solid method. Onset of strong optical absorption could be observed at energies greater than 3.5 eV consistent with highly n-type characteristics due to unintentional doping from oxygen vacancy ( V O ) defects as confirmed using Raman spectroscopy. A combination of high resolution transmission electron microscopy, x-ray photoelectron spectroscopy and valence band analysis on the nanowire morphology and stoichiometry reveals presence of high-density of VO defects on the surface of the nanowires. As a result, chemisorbed oxygen species can be observed leading to upward band bending at the surface which corresponds to a smaller valence band offset of 2.15 eV. Temperature dependent photoluminescence (PL) spectroscopy was used to study the nature of the defect states and the influence of the surface states on the electronic band structure and NBE emission has been discussed. Lastly, our data reveals significant broadening of the NBE PL peak consistent with impurity band broadening leading to band-tailing effect from heavy doping.

36 MATERIALS SCIENCE↗
DOE OSTI2017

Observation of nodal line in non-symmorphic topological semimetal InBi

Topological nodal semimetal (TNS), characterized by its touching conduction and valence bands, is a newly discovered state of quantum matter which exhibits various exotic physical phenomena. Recently, a new type of TNS called topological nodal line semimetal (TNLS) is predicted where its conduction and valence band form a degenerate one-dimension line which is further protected by its crystal symmetry. In this work, we systematically investigated the bulk and surface electronic structure of the non-symmorphic, TNLS in InBi (which is also a type II Dirac semimetal) with strong spin–orbit coupling by using angle resolved photoemission spectroscopy. By tracking the crossing points of the bulk bands at the Brillouin zone boundary, we discovered the nodal-line feature along the ${{k}}_{{z}}$ direction, in agreement with the ab initio calculations and confirmed it to be a new compound in the TNLS family. Our discovery provides a new material platform for the study of these exotic topological quantum phases and paves the way for possible future applications.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2021

Beyond the Anderson rule: importance of interfacial dipole and hybridization in van der Waals heterostructures

Vertical stacking of two-dimensional materials with weak van der Waals (vdW) interactions has laid the ground for breakthroughs in physics as well as in technological applications. Although vdW interactions dominate interlayer binding, interlayer electronic coupling may not be negligible and can lead to properties beyond the superposition of constituent monolayers. Here, studying heterobilayers of transition-metal dichalcogenides (MQ 2 ; M = Mo, Ni, Pt; Q = S, Se) by means of density functional theory calculations, we show two mechanisms that influence the band gaps of vdW heterostructures beyond the Anderson rule: (1) interfacial hybridization (mainly involving out-of-plane states, such as chalcogen p z -states), which leads to an upshift in the valence band maxima and accordingly a decrease in the band gap. (2) Formation of an interfacial electric dipole, resulting in an effective gap increase in type-II junctions. While the former is material specific, depending on the proximity of p z -states to each other and the valence band maxima, the latter can be generally described using a model based on the charge density decay outside the monolayers and the pristine band edge positions with respect to the vacuum level, irrespective of junction type.

36 MATERIALS SCIENCE↗
DOE OSTI2019

Imaging of transition charge densities involving carbon core excitations by all X-ray sum-frequency generation

X-ray diffraction signals from the time-evolving molecular charge density induced by selective core excitation of chemically inequivalent carbon atoms are calculated. A narrowband X-ray pulse selectively excites the carbon K-edge of the –CH 3 or –CH 2 F groups in fluoroethane (CH 3 –CH 2 F). Each excitation creates a distinct core coherence which depends on the character of the electronic transition. Direct propagation of the reduced single-electron density matrix, using real-time time-dependent density functional theory, provides the time-evolving charge density following interactions with external fields. Here, the interplay between partially filled valence molecular orbitals upon core excitation induces characteristic femtosecond charge migration which depends on the core–valence coherence, and is monitored by the sum-frequency generation diffraction signal.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2025

Attosecond X-Ray Core-Level Chronoscopy of Aromatic Molecules

Attosecond photoemission or photoionization delays are a unique probe of the structure and the electronic dynamics of matter. However, the spectral congestion of valence photoelectron spectra sets fundamental limits to the complexity of systems that can be studied, and the delocalization of valence electron wave functions blurs the spatial origin of the photoelectron wave packet. Using attosecond x-ray pulses from LCLS, we demonstrate the key advantages of measuring core-level delays: The photoelectron spectra remain atomlike, the measurements become element specific, and the observed scattering dynamics originate from a pointlike source when multicenter interference effects are negligible. We exploit these unique features to reveal the effects of changing functional groups (C-H vs N) and symmetry on attosecond scattering dynamics by measuring and calculating the photoionization delays between N−1⁢𝑠 and C−1⁢𝑠 core shells of a series of aromatic azabenzene molecules. Remarkably, the delays increase with the number of nitrogen atoms in the molecule and reveal multiple resonances. We identify two previously unknown mechanisms regulating the associated attosecond dynamics, namely the enhanced confinement of the trapped wave function with the replacement of C-H groups by N atoms and the decrease of the coupling strength among the photoemitted partial waves with increasing symmetry. This study demonstrates the unique opportunities opened by measurements of core-level photoionization delays for unraveling attosecond electron dynamics in complex matter.

Ji, Jia-Bao [Eidgenoessische Technische Hochschule↗
DOE OSTI2026

Skewness-dependent moments of the pion GPD from nonlocal quark-bilinear correlators

We present lattice QCD calculations of the odd Mellin moments of pion valence-quark generalized parton distribution up to fifth order ⟨𝑥 4 ⟩ and for the skewness range [−0.33, 0] using operator product expansion of bilocal quark-bilinear operators. The calculations are performed on an ensemble with lattice spacing 𝑎 = 0.04 fm and valence pion mass 300 MeV, employing boosted pion states with momenta up to 2.428 GeV and momentum transfers reaching 2.748 GeV 2 . We employ ratio-scheme renormalization and next-to-leading logarithmic resummed perturbative matching. At zero skewness, our results are consistent with previous lattice studies. By combining matrix elements at multiple values of skewness and momentum transfer, skewness-dependent moments are obtained through simultaneous polynomiality-constrained fits.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2025

Transverse-momentum-dependent pion structures from lattice QCD: Collins-Soper kernel, soft factor, TMDWF, and TMDPDF

We present the first lattice quantum chromodynamics (QCD) calculation of the pion valence-quark transverse-momentum-dependent parton distribution function (TMDPDF) within the framework of large-momentum effective theory (LaMET). Using correlators fixed in the Coulomb gauge (CG), we computed the quasi-TMD beam function for a pion with a mass of 300 MeV, a fine lattice spacing of 𝑎 =0.06 fm, and multiple large momenta up to 3 GeV. The intrinsic soft functions in the CG approach are extracted from form factors with large momentum transfer, and as a byproduct, we also obtain the corresponding Collins-Soper (CS) kernel. Our determinations of both the soft function and the CS kernel agree with perturbation theory at small transverse separations (𝑏 ⊥ ) between the quarks. At larger 𝑏 ⊥ , the CS kernel remains consistent with recent results obtained using both CG and gauge-invariant TMD correlators in the literature. By combining next-to-leading logarithmic factorization of the quasi-TMD beam function and the soft function, we obtain an 𝑥-dependent pion valence-quark TMDPDF for transverse separations 𝑏 ⊥ ≳1 fm. Interestingly, we find that the 𝑏 ⊥ dependence of the phenomenological parametrizations of TMDPDF for moderate values of 𝑥 are in reasonable agreement with our QCD determinations. In addition, we present results for the transverse-momentum-dependent wave function for a heavier pion with 670 MeV mass.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2026

First simultaneous global QCD analysis of kaon and pion parton distributions with lattice QCD constraints

We perform the first simultaneous global QCD analysis of pion and kaon parton distribution functions (PDFs) constrained by pion- and kaon-induced Drell-Yan (DY) and leading neutron electroproduction data together with lattice QCD data on pion and kaon PDF moments. The analysis indicates a softer valence u ¯ distribution in the K − than in the π − and a significantly more peaked valence s -quark density in K − compared with the u ¯ . The effective exponent governing the high- x behavior of the PDF is found to be larger for u ¯ in the kaon, β u ¯ K − = 1.6 ( 2 ) , than in the pion, β u ¯ π − = 1.16 ( 4 ) , in the range 0.7 ≤ x ≤ 0.95 . From the gluon momentum fractions, we find the pion’s gluon content accounts for ≈ 1 / 3 of the mass budget of the pion at μ = 2 GeV , but only ≈ 1 / 4 for the kaon.

Barry, P. C. [Argonne National Laboratory] (ORCID:↗
DOE OSTI2019

Hypermetallic polar molecules for precision measurements

Laser cooling is a powerful method to control molecules for applications in precision measurement, as well as quantum information, many-body physics, and fundamental chemistry. However, many optically-active metal centers in valence states which are promising for these applications, especially precision measurement, are difficult to laser cool. In order to extend the control afforded by laser cooling to a wider array of promising atoms, we consider the use of small, hypermetallic molecules that contain multiple metal centers. We provide a detailed analysis of YbCCCa and YbCCAl as prototypical examples with different spin multiplicities, and consider their feasibility for precision measurements making use of the heavy Yb atom. We find that these molecules are linear and feature metal-centered valence electrons, and study the complex hybridization and spin structures that are relevant to photon cycling and laser cooling. Our findings suggest that this hypermetallic approach may be a versatile tool for experimental control of metal species that do not otherwise efficiently cycle photons, and could present a new polyatomic platform for state-of-the-art precision measurements.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2019

Spatiotemporal analysis of a final-state shape resonance in interferometric photoemission from Cu(111) surfaces

Photoemission from solid targets includes the excitation and motion of electrons inside the substrate, followed by their propagation in vacuum and detection. It thus depends on the electronic band structure of the solid in the two distinct spectral domains of bound initial and continuum final states. While the imprint of the static (initial-state) valence electronic structure of solids on photoemission spectra is routinely examined in standard photoemission spectroscopy in the energy domain, state-of-the-art time-resolved photoelectron spectroscopy allows, in addition, the scrutiny of photoelectron propagation in the electronic continuum. Within a quantum-mechanical model for attosecond time-resolved interferometric photoelectron emission from solids, we calculated photoemission spectra as a function of the delay between the exciting primary attosecond pulse train and assisting infrared (IR) laser pulse. Accounting for final-state interactions of the photoelectron with the IR laser electric field and the periodic substrate, our numerical results for interferometric photoemission from the 3d-valence band of Cu(111) surfaces show a striking resonantly enhanced sideband yield at photoelectron kinetic energies near 24 eV, in conjunction with a pronounced increase of the photoelectron wave-function amplitude inside the solid on a length scale of a few nanometers. In this work, this resonant shift of final-state photoelectron-probability density towards the bulk can be interpreted as an increase in the photoelectron propagation time in the solid and is commensurate with the resonantly enhanced spectral sideband-phase shifts observed in recent two-pathway two-photon interference spectra by Kasmi et al.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2020

Attosecond XUV probing of vibronic quantum superpositions in Br 2 +

Ultrafast laser excitation can create coherent superpositions of electronic states in molecules and trigger ultrafast flow of electron density on a few femtosecond timescale. While recent attosecond experiments have addressed real-time observation of these primary photochemical processes, the underlying roles of simultaneous nuclear motions and how they modify and disturb the valence electronic motion remain uncertain. In this work, we investigate coherent electronic-vibrational dynamics induced among multiple vibronic levels of ionic bromine (Br 2 + ), including both spin-orbit (X 2 Π 3/2,g – X 2 Π 1/2,g ) and valence (A 2 Π 3/2,u – 4 Σ 3/2,u ) electronic superpositions, using attosecond transient absorption spectroscopy. Decay, revival, and apparent frequency shifts of electronic coherences are measured via characteristic quantum beats on the Br-3d core-level absorption signals. Quantum-mechanical simulations attribute the observed electronic decoherence to broadened phase distributions of nuclear wave packets on anharmonic potentials. Molecular vibronic structure is further revealed to be imprinted as discrete progressions in electronic beat frequencies. These results provide a future basis to interpret complex charge-migration dynamics in polyatomic systems.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2016

Fully differential single-photon double photoionization of atomic magnesium

The valence-shell double ionization of atomic magnesium is calculated using a grid-based representation of the 3s 2 electron configuration in the presence of a fully occupied frozen-core configuration of the remaining ten electrons. Atomic orbitals are constructed from an underlying finite-element discrete variable representation that facilitates accurate representation of the interaction between the inner-shell electrons with those entering the continuum. Length and velocity gauge results are compared with recent theoretical calculations and experimental measurements for the total double-, single-, and triple-differential cross sections, particularly at the photon energy of 55.49 eV for the last one. Comparison between the similar processes of double ionization of the ns 2 atoms helium, beryllium, and magnesium further illuminates the role of valence-shell electron correlation in atomic targets with heliumlike electronic configurations and symmetry.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2018

Thorium-doped CsI: Implications for the thorium nuclear clock transition

For 229m Th isomer nucleus with an anomalously low nuclear excitation energy, E$\star$ (currently accepted value of 7.8 ± 0.5 eV), the bound internal conversion (BIC) decay process is caused by the excitation of a valence electron that is sensitive to the electronic structure of the atomic-sized neighborhood. For this, we analyze an experiment where an impacting Th ion is neutralized by a negatively charged ion-receiving cesium iodide (CsI) surface, to obtain the minimal nuclear excitation energy E$\star\atop{min}$ necessary for BIC promotion of a Th-impurity valence electron in a CsI matrix. We analyze two cases: CsI with Th deposited into the bulk and with Th deposited on the CsI surface. In the bulk we consider band gap effects while on the surface we consider the work function. The energy to pull the electron to the surface is 1.5 – 2.2 eV depending on the surface plane, while to promote to the conduction band in the bulk it is 1.5 eV. Therefore we conclude that the Th-surface interaction can significantly reduce the lower E$\star$ bound of 6.3 eV, as estimated from the direct observation of the Th-clock transition [von der Wense et al., Nature (London) 533, 47 (2016)]. We suggest coating the multichannel plate with differing materials leading to different Th-impurity gaps and work functions can further narrow the E$\star$ uncertainty interval.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗