Experimental evidence of thermal fluctuations on the X-ray absorption near-edge structure at the aluminum K-edge

After a review of temperature-dependent experimental x-ray absorption near-edge structure (XANES) and related theoretical developments, we present the Al K-edge XANES spectra of corundum and beryl for temperature ranging from 300K to 930K. These experimental results provide a first evidence of the role of thermal fluctuation in XANES at the Al K-edge especially in the pre-edge region. The study is carried out by polarized XANES measurements of single crystals. For any orientation of the sample with respect to the x-ray beam, the pre-edge peak grows and shifts to lower energy with temperature. In addition temperature induces modifications in the position and intensities of the main XANES features. First-principles DFT calculations are performed for both compounds. They show that the pre-edge peak originates from forbidden 1s to 3s transitions induced by vibrations. Three existing theoretical models are used to take vibrations into account in the absorption cross section calculations: i) an average of the XANES spectra over the thermal displacements of the absorbing atom around its equilibrium position, ii) a method based on the crude Born-Oppenheimer approximation where only the initial state is averaged over thermal displacements, iii) a convolution of the spectra obtained for the atoms at the equilibrium positions with an approximate phonon spectral function. The theoretical spectra so obtained permit to qualitatively understand the origin of the spectral modifications induced by temperature. However the correct treatment of thermal fluctuation in XANES spectroscopy requires more sophisticated theoretical tools

Exploring the low-lying electronic states of C4H6OS isomers, dihydro-2(3H)-thiophenone and dihydro-3(2H)-thiophenone

PLV also acknowledges his visiting professor position at Federal University of Paraná, Curitiba, Brazil. The authors wish to acknowledge the beam time at the ISA synchrotron, Aarhus University, Denmark. This contribution is also based upon work from the COST Action CA18212-Molecular Dynamics in the GAS phase (MD-GAS), supported by COST (European Cooperation in Science and Technology). DD acknowledges support from the CaPPA project (Chemical and Physical Properties of the Atmosphere) funded by the French National Research Agency (ANR) through the PIA (Programme d'Investissement d'Avenir) under contract no. ANR-10-LABX-005 ; the Région Hauts de France and the Ministère de l'Enseignement Supérieur et de la Recherche (CPER ECRIN) and the European Fund for Regional Economic Development for their financial support. This work was performed using HPC resources from GENCI-TGCC (Grant No. 2023–A0130801859 ) and the Centre de Ressources Informatiques (CRI) of the Université de Lille. Publisher Copyright: © 2024 The Author(s)Results of a detailed study on the electronic state spectroscopy of C4H6OS isomers, dihydro-2(3H)-thiophenone and dihydro-3(2H)-thiophenone, have been obtained from high-resolution vacuum ultraviolet photoabsorption experiments together with quantum chemical calculations. The absolute photoabsorption cross-sections in the 3.7–10.7 eV energy range were obtained at the AU-UV beam line, ASTRID2 synchrotron radiation facility. The absorption spectra exhibit features due to transitions into valence and Rydberg states, superimposed on vibrational fine structure which appear much weaker in the photoabsorption spectrum of dihydro-3(2H)-thiophenone. Assignments have been proposed for some of the absorption bands with the aid of ab initio calculations at the equation-of-motion coupled-cluster singles and doubles level (EOM-CCSD) providing vertical excitation energies and oscillator strengths. The nature of the transitions was assessed by visual inspection of the natural orbitals for each transition and the average values from the electronic radial spatial extents of the electronic cloud. A comparison between the vibrational structure observed in the experimental spectra suggests relevant C[dbnd]O stretching excitations for both molecules, with important CH2 twisting and rocking modes for dihydro-2(3H)-thiophenone and ring stretching modes for dihydro-3(2H)-thiophenone. Photolysis lifetimes from 0 up to 50 km altitude in the Earth's atmosphere for both chemical compounds have been estimated from the absolute photoabsorption cross-sections.publishersversionpublishe

Nuclear break-up of 11Be

The break-up of 11Be was studied at 41AMeV using a secondary beam of 11Be from the GANIL facility on a 48Ti target by measuring correlations between the 10Be core, the emitted neutrons and gamma rays. The nuclear break-up leading to the emission of a neutron at large angle in the laboratory frame is identified with the towing mode through its characteristic n-fragment correlation. The experimental spectra are compared with a model where the time dependent Schrodinger equation (TDSE) is solved for the neutron initially in the 11 Be. A good agreement is found between experiment and theory for the shapes of neutron experimental energies and angular distributions. The spectroscopic factor of the 2s orbital is tentatively extracted to be 0.46+-0.15. The neutron emission from the 1p and 1d orbitals is also studied

Test of the Running of αs\alpha_s in τ\tau Decays

The $\tau$ decay rate into hadrons of invariant mass smaller than $\sqrt{s_0}\gg\Lambda_{\rm QCD}$ can be calculated in QCD assuming global quark--hadron duality. It is shown that this assumption holds for $s_0>0.7$~GeV$^2$. From measurements of the hadronic mass distribution, the running coupling constant $\alpha_s(s_0)$ is extracted in the range 0.7~GeV$^2<s_0<m_\tau^2$. At $s_0=m_\tau^2$, the result is $\alpha_s(m_\tau^2)=0.329\pm 0.030$. The running of $\alpha_s$ is in good agreement with the QCD prediction.Comment: 9 pages, 3 figures appended; shortened version with new figures, to appear in Physical Review Letters (April 1996

Measurements of hydrogen cyanide (HCN) and acetylene (C2H2) from the Infrared Atmospheric Sounding Interferometer (IASI)

Hydrogen cyanide (HCN) and acetylene (C2H2) are ubiquitous atmospheric trace gases with medium lifetime, which are frequently used as indicators of combustion sources and as tracers for atmospheric transport and chemistry. Because of their weak infrared absorption, overlapped by the CO2 Q branch near 720 cm−1, nadir sounders have up to now failed to measure these gases routinely. Taking into account CO2 line mixing, we provide for the first time extensive measurements of HCN and C2H2 total columns at Reunion Island (21° S, 55° E) and Jungfraujoch (46° N, 8° E) in 2009–2010 using observations from the Infrared Atmospheric Sounding Interferometer (IASI). A first order comparison with local ground-based Fourier transform InfraRed (FTIR) measurements has been carried out allowing tests of seasonal consistency which is reasonably captured, except for HCN at Jungfraujoch. The IASI data shows a greater tendency to high C2H2 values. We also examine a nonspecific biomass burning plume over austral Africa and show that the emission ratios with respect to CO agree with previously reported values

Electronic state spectroscopy of methyl formate probed by high resolution VUV photoabsorption, He(I) photoelectron spectroscopy and ab initio calculations

The first ab initio calculations of the vertical excitation energies and oscillator strengths are presented for the neutral electronic transitions of methyl formate, C2H4O2. The highest resolution VUV photoabsorption spectrum of the molecule yet reported is presented over the wavelength range 115 to 310 nm (10.8 to 4.0 eV) revealing several new spectral features. Valence and Rydberg transitions and their associated vibronic series, observed in the photoabsorption spectrum, have been assigned in accordance with new theoretical results. The calculations have been carried out to determine the excitation energies of the lowest energy ionic states of methyl formate and are compared with a newly recorded He(I) photoelectron spectrum (10.4 to 17.0 eV). New vibrational structure is observed in the first photoelectron band. The photoabsorption cross-sections have been used to calculate the photolysis lifetime of methyl formate in the upper stratosphere (20-50 km)

Gamma-Ray Burst Sequences in Hardness Ratio-Peak Energy Plane

The narrowness of the distribution of the peak energy of $\nu F_{\nu}$ spectrum of gamma-ray bursts (GRBs) and the unification of GRB population are great puzzles yet to be solved. We investigate the two puzzles based on the global spectral behaviors of different GRB population in the $HR-E_{\rm{p}}$ plane (HR the spectral hardness ratio) with BATSE and HETE-2 observations. It is found that long GRBs and XRFs observed by HETE-2 seem to follow the same sequence in the $HR-E_{\rm{p}}$ plane, with the XRFs at the low end of this sequence. The long and short GRBs observed by BATSE follow significantly different sequences in the $HR-E_{\rm p}$ plane, with most of the short GRBs having a larger hardness ratio than the long GRBs at a given $E_{\rm{p}}$. These results indicate that the global spectral behaviors of the long GRB sample and the XRF sample are similar, while that of short GRBs is different. The short GRBs seem to be a unique subclass of GRBs, and they are not the higher energy extension of the long GRBs (abridged).Comment: 9 pages, 3 figure

Syzygies in equivariant cohomology for non-abelian Lie groups

We extend the work of Allday-Franz-Puppe on syzygies in equivariant cohomology from tori to arbitrary compact connected Lie groups G. In particular, we show that for a compact orientable G-manifold X the analogue of the Chang-Skjelbred sequence is exact if and only if the equivariant cohomology of X is reflexive, if and only if the equivariant Poincare pairing for X is perfect. Along the way we establish that the equivariant cohomology modules arising from the orbit filtration of X are Cohen-Macaulay. We allow singular spaces and introduce a Cartan model for their equivariant cohomology. We also develop a criterion for the finiteness of the number of infinitesimal orbit types of a G-manifold.Comment: 28 pages; minor change

Formation scenarios for the young stellar associations between galactic longitudes l = 280-360 deg

We investigate the spatial distribution, the space velocities and age distribution of the pre-main sequence (PMS) stars belonging to Ophiuchus, Lupus and Chamaeleon star-forming regions (SFRs), and of the young early-type star members of the Scorpius-Centaurus OB association. These young stellar associations extend over the galactic longitude range from 280 deg. to 360 deg., and are at a distance interval of around 100 and 200 pc. This study is based on a compilation of distances, proper motions and radial velocities from the literature for the kinematic properties, and of basic stellar data for the construction of Hertzsprung-Russel diagrams. Although there was no well-known OB association in Chamaeleon, the distances and the proper motions of a group of 21 B- and A-type stars, taken from the Hipparcos Catalogue, lead us to propose that they form a young association. We show that the young early-type stars of the OB associations and the PMS stars of the SFRs follow a similar spatial distribution, i.e., there is no separation between the low and the high-mass young stars. We find no difference in the kinematics nor in the ages of these two populations studied. We analyze the different scenarios for the triggering of large-scale star-formation that have been proposed up to now, and argue that most probably we are observing a spiral arm that passes close to the Sun. The alignment of young stars and molecular clouds and the average velocity of the stars in the opposite direction to the Galactic rotation agree with the expected behavior of star formation in nearby spiral arms.Comment: 14 pages, 14 postscript figures, accepted for publication in A&

The OSACA Database and a Kinematic Analysis of Stars in the Solar Neighborhood

We transformed radial velocities compiled from more than 1400 published sources, including the Geneva--Copenhagen survey of the solar neighborhood (CORAVEL-CfA), into a uniform system based on the radial velocities of 854 standard stars in our list. This enabled us to calculate the average weighted radial velocities for more than 25~000 HIPPARCOS stars located in the local Galactic spiral arm (Orion arm) with a median error of +-1 km/s. We use these radial velocities together with the stars' coordinates, parallaxes, and proper motions to determine their Galactic coordinates and space velocities. These quantities, along with other parameters of the stars, are available from the continuously updated Orion Spiral Arm CAtalogue (OSACA) and the associated database. We perform a kinematic analysis of the stars by applying an Ogorodnikov-Milne model to the OSACA data. The kinematics of the nearest single and multiple main-sequence stars differ substantially. We used distant (r\approx 0.2 kpc) stars of mixed spectral composition to estimate the angular velocity of the Galactic rotation -25.7+-1.2 km/s/kpc, and the vertex deviation,l=13+-2 degrees, and detect a negative K effect. This negative K effect is most conspicuous in the motion of A0-A5 giants, and is equal to K=-13.1+-2.0 km/s/kpc.Comment: 16 pages, 8 figure