An era of exploring the interactions of high-intensity, hard X-rays with matter has begun with the start-up of a hard-X-ray free-electron laser, the Linac Coherent Light Source (LCLS). Understanding ...how electrons in matter respond to ultra-intense X-ray radiation is essential for all applications. Here we reveal the nature of the electronic response in a free atom to unprecedented high-intensity, short-wavelength, high-fluence radiation (respectively 10(18) W cm(-2), 1.5-0.6 nm, approximately 10(5) X-ray photons per A(2)). At this fluence, the neon target inevitably changes during the course of a single femtosecond-duration X-ray pulse-by sequentially ejecting electrons-to produce fully-stripped neon through absorption of six photons. Rapid photoejection of inner-shell electrons produces 'hollow' atoms and an intensity-induced X-ray transparency. Such transparency, due to the presence of inner-shell vacancies, can be induced in all atomic, molecular and condensed matter systems at high intensity. Quantitative comparison with theory allows us to extract LCLS fluence and pulse duration. Our successful modelling of X-ray/atom interactions using a straightforward rate equation approach augurs favourably for extension to complex systems.
Shifts in rainfall patterns and increasing temperatures associated with climate change are likely to cause widespread forest decline in regions where droughts are predicted to increase in duration ...and severity. One primary cause of productivity loss and plant mortality during drought is hydraulic failure. Drought stress creates trapped gas emboli in the water transport system, which reduces the ability of plants to supply water to leaves for photosynthetic gas exchange and can ultimately result in desiccation and mortality. At present we lack a clear picture of how thresholds to hydraulic failure vary across a broad range of species and environments, despite many individual experiments. Here we draw together published and unpublished data on the vulnerability of the transport system to drought-induced embolism for a large number of woody species, with a view to examining the likely consequences of climate change for forest biomes. We show that 70% of 226 forest species from 81 sites worldwide operate with narrow (,1 megapascal) hydraulic safety margins against injurious levels of drought stress and therefore potentially face long-term reductions in productivity and survival if temperature and aridity increase as predicted for many regions across the globe. Safety margins are largely independent of mean annual precipitation, showing that there is global convergence in the vulnerability of forests to drought, with all forest biomes equally vulnerable to hydraulic failure regardless of their current rainfall environment. These findings provide insight into why drought-induced forest decline is occurring not only in arid regions but also in wet forests not normally considered at drought risk.
A combination of velocity map ion imaging, mass spectrometry, and a laser-based vacuum ultraviolet light source was used to perform a new measurement of the absolute photoionization cross section of ...the propargyl radical. The measurements are in good agreement with the recent determination of Savee et al. J. Chem. Phys. 2012, 136, 134307 , and significantly larger than an earlier determination. The results are discussed and rationalized in terms of some general ideas about absolute photoionization cross sections. The potential utility of these ideas is illustrated by using recent cross section measurements for a number of molecular radicals, including methyl, allyl and 2-propenyl, phenyl, and vinyl.
Improved knowledge of the sorghum transcriptome will enhance basic understanding of how plants respond to stresses and serve as a source of genes of value to agriculture. Toward this goal, Sorghum ...bicolor L. Moench cDNA libraries were prepared from light- and dark-grown seedlings, drought-stressed plants, Colletotrichum-infected seedlings and plants, ovaries, embryos, and immature panicles. Other libraries were prepared with meristems from Sorghum propinquum (Kunth) Hitchc. that had been photoperiodically induced to flower, and with rhizomes from S. propinquum and johnsongrass (Sorghum halepense L. Pers.). A total of 117,682 expressed sequence tags (ESTs) were obtained representing both 3' and 5' sequences from about half that number of cDNA clones. A total of 16,801 unique transcripts, representing tentative UniScripts (TUs), were identified from 55,783 3' ESTs. Of these TUs, 9,032 are represented by two or more ESTs. Collectively, these libraries were predicted to contain a total of approximately 31,000 TUs. Individual libraries, however, were predicted to contain no more than about 6,000 to 9,000, with the exception of light-grown seedlings, which yielded an estimate of close to 13,000. In addition, each library exhibits about the same level of complexity with respect to both the number of TUs preferentially expressed in that library and the frequency with which two or more ESTs is found in only that library. These results indicate that the sorghum genome is expressed in highly selective fashion in the individual organs and in response to the environmental conditions surveyed here. Close to 2,000 differentially expressed TUs were identified among the cDNA libraries examined, of which 775 were differentially expressed at a confidence level of 98%. From these 775 TUs, signature genes were identified defining drought, Colletotrichum infection, skotomorphogenesis (etiolation), ovary, immature panicle, and embryo.
A 3-D reference model for wideband multiple-input multiple-output (MIMO) mobile-to-mobile (M-to-M) channels is reviewed along with its corresponding first- and second-order channel statistics. To ...validate the reference model, an experimental MIMO M-to-M channel-sounding campaign was conducted for M-to-M vehicular communication with vehicles that travel along surface streets and expressways in a metropolitan area. To compare the first- and second-order channel statistics that were obtained from the reference model with those obtained from the empirical measurements, a new maximum-likelihood-based stochastic estimator is derived to extract the relevant model parameters from the measured data. The measured data is processed and compared with the analytical results. The close agreement between the analytically and empirically obtained channel statistics confirms the utility of the proposed reference model and the method for estimating the model parameters.
Double-resonance excitation of molecular nitrogen, N
2
, via selected rotational levels of the
, v′ = 0 state has been used to probe the first two bands in the new Ogawa series M. Ogawa, Can. J. ...Phys. 42, 1087 (1964), which lie above the first ionisation threshold of the molecule. These bands are rotationally unresolved in room-temperature and jet-cooled absorption spectra, but the double-resonance technique allows a rotational analysis and first confirmation of the assignment as transitions to n = 4 members of the (A
2
Π
u
)ndπ, v Rydberg series. In principle, the probe transition from the
, v = 0 level to these Rydberg states corresponds to a two-electron transition, and this aspect of the results is explored. Finally, velocity map imaging allows a determination of the photoelectron branching fractions and angular distributions, providing insight into the electronic autoionisation dynamics.
The synovium is the major target tissue of inflammatory arthritides such as rheumatoid arthritis. The study of synovial tissue has advanced considerably throughout the past few decades from ...arthroplasty and blind needle biopsy to the use of arthroscopic and ultrasonographic technologies that enable easier visualization and improve the reliability of synovial biopsies. Rapid progress has been made in using synovial tissue to study disease pathogenesis, to stratify patients, to discover biomarkers and novel targets, and to validate therapies, and this progress has been facilitated by increasingly diverse and sophisticated analytical and technological approaches. In this Review, we describe these approaches, and summarize how their use in synovial tissue research has improved our understanding of rheumatoid arthritis and identified candidate biomarkers that could be used in disease diagnosis and stratification, as well as in predicting disease course and treatment response.
Photoionization of C4H5 Isomers Hartweg, S; Loison, J.-C; Boyé-Péronne, S ...
The journal of physical chemistry. A, Molecules, spectroscopy, kinetics, environment, & general theory,
07/2020, Letnik:
124, Številka:
29
Journal Article
Recenzirano
Odprti dostop
Single-photon, photoelectron–photoion coincidence spectroscopy is used to record the mass-selected ion spectra and slow photoelectron spectra of C4H5 radicals produced by the abstraction of hydrogen ...atoms from three C4H6 precursors by fluorine atoms generated by a microwave discharge. Three different C4H5 isomers are identified, with the relative abundances depending on the nature of the precursor (1-butyne, 1,2-butadiene, and 1,3-butadiene). The results are compared with our previous work using 2-butyne as a precursor Hrodmarsson, H. R. J. Phys. Chem. A 2019, 123, 1521−1528 . The slow photoelectron spectra provide new information on the three radical isomers that is in good agreement with previous experimental and theoretical results Lang, M. J. Phys. Chem. A 2015, 119, 3995−4000 ; Hansen, N. J. Phys. Chem. A 2006, 110, 3670–3678 . The energy scans of the C4H5 photoionization signal are recorded with substantially better resolution and signal-to-noise ratio than those in earlier work, allowing the observation of autoionizing resonances based on excited states of the C4H5 cation. Photoelectron images recorded at several energies are also reported, providing insight into the decay processes of these excited states. Finally, in contrast to the earlier work using 2-butyne as a precursor, where H-atom abstraction was the only observed process, F- and H-atom additions to the present precursors are also observed through the detection of C4H6F, C4H5F, and C4H7.
New capabilities at X-ray free-electron laser facilities allow the generation of two-colour femtosecond X-ray pulses, opening the possibility of performing ultrafast studies of X-ray-induced ...phenomena. Particularly, the experimental realization of hetero-site-specific X-ray-pump/X-ray-probe spectroscopy is of special interest, in which an X-ray pump pulse is absorbed at one site within a molecule and an X-ray probe pulse follows the X-ray-induced dynamics at another site within the same molecule. Here we show experimental evidence of a hetero-site pump-probe signal. By using two-colour 10-fs X-ray pulses, we are able to observe the femtosecond time dependence for the formation of F ions during the fragmentation of XeF2 molecules following X-ray absorption at the Xe site.
We have studied the photodissociation dynamics of anisole (C6H5OCH3) at 193 nm and determined the absolute photoionization cross-section of the phenoxy radical at 118.2 nm (10.486 eV) relative to the ...known cross-section of the methyl radical. Even at this energy, there is extensive fragmentation of the phenoxy radical upon photoionization, which is attributed to ionizing transitions that populate low-lying excited electronic states of the cation. For phenoxy radicals with less than ∼1 eV of internal energy, we find a cross-section for the production of the phenoxy cation of 14.8 ± 3.8 Mb. For radicals with higher internal energy, dissociative ionization is the dominant process, and for internal energies of ∼2.7–3.7 eV, we find a total cross-section (photoionization plus dissociative ionization) of 22.3 ± 4.1 Mb. The results are discussed relative to the recently reported photoionization cross-section of phenol.
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