Electronic structure of the iron chalcogenide KFeAgTe2 revealed by angle-resolved photoemission spectroscopy
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phonons, thermal conductivity, energy storage (inc↗
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Results for “SPECTROSCOPY”
Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.
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High-precision γ -ray spectroscopy of the cardiac PET imaging isotope Rb 82 and its impact on dosimetry
82 Rb is a positron-emitting isotope used in cardiac positron emission tomography (PET) imaging which has been reported to deliver a significantly lower effective radiation dose than analogous imaging isotopes like 201 Tl and 99m Tc sestamibi. High-quality β-decay data are essential to accurately appraise the total dose received by the patients. A source of 82 Sr was produced at the Brookhaven Linac Isotope Producer (BLIP), transported to Argonne National Laboratory, and studied with the Gammasphere facility. Significant revisions have been made to the level scheme of 82 Kr including 12 new levels, 50 new γ-ray transitions, and the determination of many new spin assignments through angular correlations. Lastly, these new high-quality data allow a precise reappraisal of the β-decay strength function and thus the consequent dose received by patients.
73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
Translational diffusion of water inside hydrophobic carbon micropores studied by neutron spectroscopy and molecular dynamics simulation
When water molecules are confined to nanoscale spacings, such as in the nanometer-size pores of activated carbon fiber (ACF), their freezing point gets suppressed down to very low temperatures (~150 K), leading to a metastable liquid state with remarkable physical properties. Here we have investigated the ambient pressure diffusive dynamics of water in microporous Kynol ACF-10 (average pore size ~11.6 Å, with primarily slit-like pores) from temperature T = 280 K in its stable liquid state down to T = 230 K into the metastable supercooled phase. The observed characteristic relaxation times and diffusion coefficients are found to be, respectively, higher and lower than those in bulk water, indicating a slowing down of the water mobility with decreasing temperature. The observed temperature-dependent average relaxation time (${{\tau}}$) when compared to previous findings indicate that it is the width of the slit pores-not their curvature-that primarily affects the dynamics of water for pore sizes larger than 10 Å. The experimental observations are compared to complementary molecular dynamics simulations of a model system, in which we studied the diffusion of water within the 11.6 Å gap of two parallel graphene sheets. We find generally a reasonable agreement between the observed and calculated relaxation times at the low momentum transfer Q (Q ≤ 0.9 Å -1) . At high Q, however, where localized dynamics becomes relevant, this ideal system does not satisfactorily reproduce the measurements. Consequently, the simulations are compared to the experiments at low Q, where the two can be best reconciled. The best agreement is obtained for the diffusion parameter D associated with the hydrogen-site when a representative stretched exponential function, rather than the standard bimodal exponential model, is used to parametrize the self-correlation function I (Q,t).
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Measurement of Electronic States of PbS Nanocrystal Quantum Dots Using Scanning Tunneling Spectroscopy: The Role of Parity Selection Rules in Optical Absorption
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bio-inspired↗
Accurate predictions of iron redox state in silicate glasses: A multivariate approach using X-ray absorption spectroscopy
Abstract not provided
Dyar, M. Darby↗
First Year PIDDP Report on gamma-ray and x-ray spectroscopy: X-ray remote sensing and in situ spectroscopy for planetary exploration missions and gamma-ray remote sensing and in situ spectroscopy for planetary exploration missions
Detectors that will be used for planetary missions must have their responses calibrated in a reproducible manner. In addition, it is important to characterize a detector system at uneven portions of its life cycle, for example after exposure to different amounts of radiation. A calibration and response characterization facility has been constructed at Schlumberger-Doll Research for all types of gamma- and x-ray detectors that may be used for planetary measurement. This facility is currently being tested. Initial use is expected for the MARS 94 detectors. The facility will then also be available for calibrating other detectors as well as arrays of detectors such as the NEAR detector with its central Nal(TI) crystal surrounded with a large BGO crystal. Cadmium telluride detectors are investigated for applications in space explorations. These detectors show an energy resolution of 5 keV for the 122 keV 57Co line. Earlier reported polarization effects are not observed. The detectors can be used at temperatures up to 100 C, although with reduced energy resolution. The thickness of standard detectors is limited to 2 mm. These detectors become fully efficient at bias voltages above 200 V. Initial results for a 1 cm thick detector show that the quality of the material is inferior to the thinner standard detectors and hole trapping affects the pulse height. A detailed characterization of the detector is in progress. Prototypes of photomultipliers based on a Channel Electron Multiplier (CEM) are being built to study their performance. Such photomultipliers promise better timing characteristics and a higher dynamic range while being more compact and of lower in weight.
Mahdavi, M.↗
Structural origins of the electronic properties of materials via time-resolved infrared spectroscopy
Time-resolved mid-infrared (TRIR) spectroscopy offers new opportunities to investigate how the molecular and structural properties of optoelectronic materials influence their electronic and transport states. This capability emerges from the ability to measure low energy electronic transitions in the mid-infrared that are related to delocalized states in materials and to simultaneously detect the vibrational properties of the materials that influence those states. Furthermore, the ability to simultaneously measure electronic and vibrational transitions in materials offers unprecedented opportunities to correlate structural dynamics of materials with their electronic and transport properties. Here, these capabilities are introduced by first describing the basic principles of TRIR spectroscopy used to examine electronic processes in materials. Then, several applications of TRIR spectroscopy are described in which measurements of the vibrational spectra of electronic excited states are probed as a means to correlate the structural properties of materials with the delocalization of their electronic states. In one example, exciton localization mechanisms in organic semiconductors are probed through vibrational spectra of the molecules in their excited states and correlated with their crystalline packing arrangements. Another example highlights the use of TRIR spectroscopy to examine singlet fission reaction dynamics through a combination of low energy electronic transitions and the vibrational spectra that are unique to the electronic states involved in the reaction. Finally, the use of TRIR spectroscopy to investigate charge carrier localization mechanisms in lead-halide perovskites is described, followed by an outlook of future applications of the technique in optoelectronic materials research.
36 MATERIALS SCIENCE↗
Simulating Ru L 3 -Edge X-ray Absorption Spectroscopy with Time-Dependent Density Functional Theory: Model Complexes and Electron Localization in Mixed-Valence Metal Dimers
Ruthenium L3-edge X-ray absorption (XA) spectroscopy probes unoccupied 4d orbitals of the metal atom and is increasingly being used to investigate the local electronic structure in ground and excited electronic states of Ru complexes. The simultaneous development of computational tools for simulating Ru L3-edge spectra is crucial for interpreting the spectral features at a molecular level. This study demonstrates that time-dependent density functional theory (TDDFT) is a viable and predictive tool for simulating ruthenium L3-edge XA spectroscopy. We systematically investigate the effects of exchange correlation functional and implicit and explicit solvent interactions on a series of RuII and RuIII complexes in their ground and electronic excited states. The TDDFT simulations reproduce all of the experimentally observed features in Ru L3-edge XA spectra within the experimental resolution (0.4 eV). Our simulations identify ligand-specific charge transfer features in complicated Ru L3-edge spectra of [Ru(CN)6]4- and RuII polypyridyl complexes illustrating the advantage of using TDDFT in complex systems. We conclude that the B3LYP functional most accurately predicts the transition energies of charge transfer features in these systems. We use our TDDFT approach to simulate experimental Ru L3-edge XA spectra of transition metal mixed-valence dimers of the form [(NC)5MII-CN-RuIII(NH3)5] (where M = Fe or Ru) dissolved in water. Our study determines the spectral signatures of electron delocalization in Ru L3-edge XA spectra. We find that the inclusion of explicit solvent molecules is necessary for reproducing the spectral features and the experimentally determined valencies in these mixed-valence complexes. This study validates the use of TDDFT for simulating Ru 2p excitations using popular quantum chemistry codes and providing a powerful interpretive tool for equilibrium and ultrafast Ru L3-edge XA spectroscopy.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Selective Host-Guest Interaction between Metal Ions and Metal-Organic Frameworks Using Dynamic Nuclear Polarization Enhanced Solid-State NMR Spectroscopy
The host–guest interaction between metal ions (Pt²⁺ and Cu²⁺) and a zirconium metal–organic framework (UiO-66-NH₂) was explored using dynamic nuclear polarization-enhanced ¹⁵N{¹H} CPMAS NMR spectroscopy supported by X-ray absorption spectroscopy and density functional calculations. The combined experimental results conclude that each Pt²⁺ coordinates with two NH₂ groups from the MOF and two Cl⁻ from the metal precursor, whereas Cu²⁺ do not form chemical bonds with the NH₂ groups of the MOF framework. Density functional calculations reveal that Pt²⁺ prefers a square-planar structure with the four ligands and resides in the octahedral cage of the MOF in either cis or trans configurations.
Guo, Zhiyong↗
New developments in high pressure x-ray spectroscopy beamline at High Pressure Collaborative Access Team
The 16 ID-D (Insertion Device - D station) beamline of the High Pressure Collaborative Access Team at the Advanced Photon Source is dedicated to high pressure research using X-ray spectroscopy techniques typically integrated with diamond anvil cells. The beamline provides X-rays of 4.5-37 keV, and current available techniques include X-ray emission spectroscopy, inelastic X-ray scattering, and nuclear resonant scattering. Here, the recent developments include a canted undulator upgrade, 17-element analyzer array for inelastic X-ray scattering, and an emission spectrometer using a polycapillary half-lens. Recent development projects and future prospects are also discussed.
47 OTHER INSTRUMENTATION↗
High resolution spectroscopy of jet cooled phenyl radical: The ν{sub 1} and ν{sub 2} a{sub 1} symmetry C–H stretching modes
A series of CH stretch modes in phenyl radical (C{sub 6}H{sub 5}) has been investigated via high resolution infrared spectroscopy at sub-Doppler resolution (∼60 MHz) in a supersonic discharge slit jet expansion. Two fundamental vibrations of a{sub 1} symmetry, ν{sub 1} and ν{sub 2}, are observed and rotationally analyzed for the first time, corresponding to in-phase and out-of-phase symmetric CH stretch excitation at the ortho/meta/para and ortho/para C atoms with respect to the radical center. The ν{sub 1} and ν{sub 2} band origins are determined to be 3073.968 50(8) cm{sup −1} and 3062.264 80(7) cm{sup −1}, respectively, which both agree within 5 cm{sup −1} with theoretical anharmonic scaling predictions based on density functional B3LYP/6-311g++(3df,3dp) calculations. Integrated band strengths for each of the CH stretch bands are analyzed, with the relative intensities agreeing remarkably well with theoretical predictions. Frequency comparison with previous low resolution Ar-matrix spectroscopy [A. V. Friderichsen et al., J. Am. Chem. Soc. 123, 1977 (2001)] reveals a nearly uniform Δν ≈ + 10-12 cm{sup −1} blue shift between gas phase and Ar matrix values for ν{sub 1} and ν{sub 2}. This differs substantially from the much smaller red shift (Δν ≈ − 1 cm{sup −1}) reported for the ν{sub 19} mode, and suggests a simple physical model in terms of vibrational mode symmetry and crowding due to the matrix environment. Finally, the infrared phenyl spectra are well described by a simple asymmetric rigid rotor Hamiltonian and show no evidence for spectral congestion due to intramolecular vibrational coupling, which bodes well for high resolution studies of other ring radicals and polycyclic aromatic hydrocarbons. In summary, the combination of slit jet discharge methods with high resolution infrared lasers enables spectroscopic investigation of even highly reactive combustion and interstellar radical intermediates under gas phase, jet-cooled (T{sub rot} ≈ 11 K) conditions.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Hyperfine structures and isotopic shifts of uranium transitions using tunable laser spectroscopy of laser ablation plumes
We report isotopic shifts and hyperfine structures of selected U transitions employing tunable spectroscopy viz: laser-induced fluorescence and laser absorption spectroscopy of laser ablation plumes. The laser-produced plasmas were produced during ns laser ablation on a natural U metal which contains 0.7% 235U. Our results show that isotopic shifts between 238U and 235U are entangled with hyperfine structures of 235U. The isotopic ratio obtained using laser-induced fluorescence is affected by optical saturation effect. Time-resolved laser absorption spectroscopy is carried out for evaluating the optical absorption and estimating the hyperfine constants.
(020.3260) Isotope shifts↗
Reactive intermediates in {sup 4}He nanodroplets: Infrared laser Stark spectroscopy of dihydroxycarbene
Singlet dihydroxycarbene (HOC{sup ¨}OH) is produced via pyrolytic decomposition of oxalic acid, captured by helium nanodroplets, and probed with infrared laser Stark spectroscopy. Rovibrational bands in the OH stretch region are assigned to either trans,trans- or trans,cis-rotamers on the basis of symmetry type, nuclear spin statistical weights, and comparisons to electronic structure theory calculations. Stark spectroscopy provides the inertial components of the permanent electric dipole moments for these rotamers. The dipole components for trans, trans- and trans, cis-rotamers are (μ{sub a}, μ{sub b}) = (0.00, 0.68(6)) and (1.63(3), 1.50(5)), respectively. The infrared spectra lack evidence for the higher energy cis,cis-rotamer, which is consistent with a previously proposed pyrolytic decomposition mechanism of oxalic acid and computations of HOC{sup ¨}OH torsional interconversion and tautomerization barriers.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Synchrotron-based double imaging photoelectron/photoion coincidence spectroscopy of radicals produced in a flow tube: OH and OD
We present a microwave discharge flow tube coupled with a double imaging electron/ion coincidence device and vacuum ultraviolet (VUV) synchrotron radiation. The system has been applied to the study of the photoelectron spectroscopy of the well-known radicals OH and OD. The coincidence imaging scheme provides a high selectivity and yields the spectra of the pure radicals, removing the ever-present contributions from excess reactants, background, or secondary products, and therefore obviating the need for a prior knowledge of all possible byproducts. The photoelectron spectra encompassing the X{sup 3}Σ{sup −} ground state of the OH{sup +} and OD{sup +} cations have been extracted and the vibrational constants compared satisfactorily to existing literature values. Future advantages of this approach include measurement of high resolution VUV spectroscopy of radicals, their absolute photoionization cross section, and species/isomer identification in chemical reactions as a function of time.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Optical spectroscopy of molecular junctions: Nonequilibrium Green’s functions perspective
We consider optical spectroscopy of molecular junctions from the quantum transport perspective when radiation field is quantized and optical response of the system is simulated as photon flux. Using exact expressions for photon and electronic fluxes derived within the nonequilibrium Green function (NEGF) methodology and utilizing fourth order diagrammatic perturbation theory (PT) in molecular coupling to radiation field, we perform simulations employing realistic parameters. Results of the simulations are compared to the bare PT which is usually employed in studies on nonlinear optical spectroscopy to classify optical processes. We show that the bare PT violates conservation laws, while flux conserving NEGF formulation mixes optical processes.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Applications of Doppler-free saturation spectroscopy for edge physics studies (invited)
Doppler-free saturation spectroscopy provides a very powerful method to obtain detailed information about the electronic structure of the atom through measurement of the spectral line profile. This is achieved through a significant decrease in the Doppler broadening and essentially an elimination of the instrument broadening inherent to passive spectroscopic techniques. In this paper we present the technique and associated physics of Doppler-free saturation spectroscopy in addition to how one selects the appropriate transition. Simulations of H{sub δ} spectra are presented to illustrate the increased sensitivity to both electric field and electron density measurements.
46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
The charge exchange recombination spectroscopy diagnostic on the upgraded Lithium Tokamak eXperiment (LTX-β)
The Lithium Tokamak eXperiment has undergone an upgrade to LTX-β, a major part of which is the addition of neutral beam injection (NBI). NBI has allowed for a new charge exchange recombination spectroscopy (CHERS) system to be installed in order to measure impurity concentrations, ion temperature, and toroidal velocity. Previously on LTX measuring these parameters relied on passive spectroscopy and inversion techniques and had large uncertainty. The CHERS system has 52 total views, split into four groups of 13, half facing toward the beam and half symmetrically facing away from the beam, so the background non-beam related emission can be simultaneously subtracted. Both sets of views sample a major radius of 27-59 cm, with resolution through the beam of 1.5-2.5 cm. LTX-β is expected to have its magnetic axis near 35 cm, with minor radii of 18-23 cm. Three separate spectrometers will be used for the diagnostic, giving the system great flexibility to simultaneously measure emission from multiple impurity lines. The viewing optics are f/1.8, allowing all of the spectrometers to be fully illuminated. Design and calibration of the system as well as the advantages of various configurations of the spectrometers will be highlighted.
Elliott, Drew↗