25 research outputs found
Unified treatment of recoil and Doppler broadening in molecular high-energy photoemission
Doppler and recoil effects are an integral part of the photoemission process at the high kinetic energies reached in hard x-ray photo-electron spectroscopy (HAXPES) and have a major effect on the observed lineshape, resulting in broadening, energy losses and discrete excitations. These effects can be modeled with a high degree of detail for small systems like diatomic molecules, for larger systems such treatment is often superfluous as the fine spectral features are not observable. We present a united description of the Doppler and recoil effects for arbitrary polyatomic systems and offer an approximate description of the recoil- and Doppler-modified photoemission spectral lineshape as a practical tool in the analysis of HAXPES spectra of core-level photoemission. The approach is tested on the examples of carbon dioxide and pentane molecules. The C and O 1s photoelectron spectra of CO2 in gas phase were also measured at 2.3 and 7.0 keV photon energy at Synchrotron SOLEIL and the spectra were analyzed using the model description. The limitations and applicability of the approach to adsorbates, interfaces and solids is briefly discussed
Calcium signals can freely cross the nuclear envelope in hippocampal neurons: somatic calcium increases generate nuclear calcium transients
<p>Abstract</p> <p>Background</p> <p>In hippocampal neurons, nuclear calcium signaling is important for learning- and neuronal survival-associated gene expression. However, it is unknown whether calcium signals generated by neuronal activity at the cell membrane and propagated to the soma can unrestrictedly cross the nuclear envelope to invade the nucleus. The nuclear envelope, which allows ion transit via the nuclear pore complex, may represent a barrier for calcium and has been suggested to insulate the nucleus from activity-induced cytoplasmic calcium transients in some cell types.</p> <p>Results</p> <p>Using laser-assisted uncaging of caged calcium compounds in defined sub-cellular domains, we show here that the nuclear compartment border does not represent a barrier for calcium signals in hippocampal neurons. Although passive diffusion of molecules between the cytosol and the nucleoplasm may be modulated through changes in conformational state of the nuclear pore complex, we found no evidence for a gating mechanism for calcium movement across the nuclear border.</p> <p>Conclusion</p> <p>Thus, the nuclear envelope does not spatially restrict calcium transients to the somatic cytosol but allows calcium signals to freely enter the cell nucleus to trigger genomic events.</p
Model of Stationary Diffusion with Absorption In Domains With Fine-Grained Random Boundaries
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Isotope effects in dynamics of water isotopologues induced by core ionization at an x-ray free-electron laser
Dynamical response of water exposed to x-rays is of utmost importance in a wealth of science areas. We exposed isolated water isotopologues to short x-ray pulses from a free-electron laser and detected momenta of all produced ions in coincidence. By combining experimental results and theoretical modeling, we identify significant structural dynamics with characteristic isotope effects in H2O2+, D2O2+, and HDO2+, such as asymmetric bond elongation and bond-angle opening, leading to two-body or three-body fragmentation on a timescale of a few femtoseconds. A method to disentangle the sequences of events taking place upon the consecutive absorption of two x-ray photons is described. The obtained deep look into structural properties and dynamics of dissociating water isotopologues provides essential insights into the underlying mechanisms
Deregulation of lncRNA HIST1H2AG-6 and AIM1-3 in peripheral blood mononuclear cells is associated with newly diagnosed type 2 diabetes
Formulation for Oral Delivery of Lactoferrin Based on Bovine Serum Albumin and Tannic Acid Multilayer Microcapsules
We thank A*STAR, Singapore and Ministry of Business, Innovation and Employment, New Zealand, SG-NZ Foods for Health Grant for financial support of this work (Project 1414024010). The work was also supported by Ministry of Education and Science of the Russian Federation as grant No. 14.Z50.31.0004 to support scientific research projects implemented under the supervision of leading scientists at Russian institutions and Russian institutions of higher education. E.K. and M.V.N. acknowledge financial support by the A*STAR Graduate Academy, Singapore. O.A.S. is thankful to Scholarship of President of Russian Federation for training abroad in 2016/17 academic year
UV-induced dissociation of CH2BrI probed by intense femtosecond XUV pulses
The ultraviolet (UV)-induced dissociation and photofragmentation of gas-phase CH2BrI molecules induced by intense femtosecond extreme ultraviolet (XUV) pulses at three different photon energies are studied by multi-mass ion imaging. Using a UV-pump — XUV-probe scheme, charge transfer between highly charged iodine ions and neutral CH2Br radicals produced by C—I bond cleavage is investigated. In earlier charge-transfer studies, the center of mass of the molecules was located along the axis of the bond cleaved by the pump pulse. In the present case of CH2BrI, this is not the case, thus inducing a rotation of the fragment. We discuss the influence of the rotation on the charge transfer process using a classical over-the-barrier model. Our modeling suggests that, despite the fact that the dissociation is slower due to the rotational excitation, the critical interatomic distance for charge transfer is reached faster. Furthermore, we suggest that charge transfer during molecular fragmentation may be modulated in a complex way
Time-resolved inner-shell photoelectron spectroscopy: From a bound molecule to an isolated atom
Due to its element and site specificity, inner-shell photoelectron spectroscopy is a widely used technique to probe the chemical structure of matter. Here, we show that time-resolved inner-shell photoelectron spectroscopy can be employed to observe ultrafast chemical reactions and the electronic response to the nuclear motion with high sensitivity. The ultraviolet dissociation of iodomethane ( CH 3 I ) is investigated by ionization above the iodine 4 d edge, using time-resolved inner-shell photoelectron and photoion spectroscopy. The dynamics observed in the photoelectron spectra appear earlier and are faster than those seen in the iodine fragments. The experimental results are interpreted using crystal-field and spin-orbit configuration interaction calculations, and demonstrate that time-resolved inner-shell photoelectron spectroscopy is a powerful tool to directly track ultrafast structural and electronic transformations in gas-phase molecules
Coulomb-explosion imaging of concurrent photodissociation dynamics
The dynamics following laser-induced molecular photodissociation of gas-phase CH2BrI at 271.6 nm were investigated by time-resolved Coulomb-explosion imaging using intense near-IR femtosecond laser pulses. The observed delay-dependent photofragment momenta reveal that CH2BrI undergoes C-I cleavage, depositing 65.6% of the available energy into internal product states, and that absorption of a second UV photon breaks the C-Br bond of CH2Br. Simulations confirm that this mechanism is consistent with previous data recorded at 248 nm, demonstrating the sensitivity of Coulomb-explosion imaging as a real-time probe of chemical dynamics