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At least 145 records · Page 8Linked to original sources

Time-resolved intraband electronic relaxation dynamics of Hg(n) (-) clusters (n=7-13,15,18) excited at 1.0 eV.

Time-resolved photoelectron imaging has been used to study the relaxation dynamics of small Hg(n) (-) clusters (n=7-13,15,18) following intraband electronic excitation at 1250 nm (1.0 eV). This study furthers our previous investigation of single electron, intraband relaxation dynamics in Hg(n) (-) clusters at 790 nm by exploring the dynamics of smaller clusters (n=7-10), as well as those of larger clusters (n=11-13,15,18) at a lower excitation energy. We measure relaxation time scales of 2-9 ps, two to three times faster than seen previously after 790 nm excitation of Hg(n) (-), n=11-18. These results, along with size-dependent trends in the absorption cross-section and photoelectron angular distribution anisotropy, suggest significant evolution of the cluster anion electronic structure in the size range studied here. Furthermore, the smallest clusters studied here exhibit 35-45 cm(-1) oscillations in pump-probe signal at earliest temporal delays that are interpreted as early coherent nuclear motion on the excited potential energy surfaces of these clusters. Evidence for evaporation of one or two Hg atoms is seen on a time scale of tens of picoseconds.

Journal Article↗

Vibronic coupling in the excited cationic states of ethylene: simulation of the photoelectron spectrum between 12 and 18 eV.

The effect of vibronic coupling on structure and spectroscopy is investigated in the excited cationic states of ethylene. It is found from equation of motion coupled cluster singles and doubles method for ionization potential electronic structure calculations in a triple-zeta plus double polarization basis set that ethylene in its third (B (2)A(g)) and fourth (C (2)B(2u)) ionized states does not have a stable minimum-energy geometry. The potential-energy surfaces of these states are energetically distinct and well separated at the ground-state geometry of ethylene, but in a geometry optimization as the structure of the ion relaxes, these surfaces end up in conical intersections and finally in the stable equilibrium geometry of the second ionized state (A (2)B(3g)). The topology of the potential-energy surfaces can be clearly understood using a vibronic model Hamiltonian. Furthermore, by diagonalizing this model Hamiltonian, the photoelectron spectrum of ethylene corresponding to the second, third, and fourth ionized states (12-18 eV) is simulated. Spectra from vibronic simulations including up to quartic coupling constants and using various normal-mode basis sets are compared to those from vertical Franck-Condon simulations to understand the importance of vibronic coupling and nonadiabatic effects and to examine the influence of individual normal modes on the spectrum.

Journal Article↗

Experimental and theoretical (e,2e) ionization cross sections for a hydrogen target at 75.3 eV incident energy in a coplanar asymmetric geometry.

Very recently it was shown that the molecular three-body distorted wave (M3DW) approach gives good agreement with the shape of the experimental data for electron-impact ionization of H(2) in a coplanar symmetric geometry, providing the incident electrons have an energy of 35 eV or greater. One of the weaknesses of these studies was that only the shape of the cross section could be compared to experiment, since there was no absolute or relative normalization of the data. Here we report a joint experimental/theoretical study of electron-impact ionization of H(2) in a coplanar asymmetric geometry where the energy of the incident electron was fixed, and different pairs of final state electron energies were used. In this case, the experimental data can be normalized such that only one renormalization factor is required. It is shown that the M3DW is pretty good in agreement with experiment. However, a better treatment of polarization and exchange between the continuum and bound state electrons is required before quantitative agreement between experiment and theory is achieved.

Journal Article↗

Dynamics and fragmentation of van der Waals clusters: (H2O)n, (CH3OH)n, and (NH3)n upon ionization by a 26.5 eV soft x-ray laser.

A tabletop soft x-ray laser is applied for the first time as a high energy photon source for chemical dynamics experiments in the study of water, methanol, and ammonia clusters through time of flight mass spectroscopy. The 26.5 eV/photon laser (pulse time duration of approximately 1 ns) is employed as a single photon ionization source for the detection of these clusters. Only a small fraction of the photon energy is deposited in the cluster for metastable dissociation of cluster ions, and most of it is removed by the ejected electron. Protonated water, methanol, and ammonia clusters dominate the cluster mass spectra. Unprotonated ammonia clusters are observed in the protonated cluster ion size range 2< or =n< or =22. The unimolecular dissociation rate constants for reactions involving loss of one neutral molecule are calculated to be (0.6-2.7)x10(4), (3.6-6.0)x10(3), and (0.8-2.0)x10(4) s(-1) for the protonated water (9< or =n< or =24), methanol (5< or =n< or =10), and ammonia (5< or =n< or =18) clusters, respectively. The temperatures of the neutral clusters are estimated to be between 40 and 200 K for water clusters (10< or =n< or =21), and 50-100 K for methanol clusters (6< or =n< or =10). Products with losses of up to five H atoms are observed in the mass spectrum of the neutral ammonia dimer. Large ammonia clusters (NH(3))(n) (n>3) do not lose more than three H atoms in the photoionization/photodissociation process. For all three cluster systems studied, single photon ionization with a 26.5 eV photon yields near threshold ionization. The temperature of these three cluster systems increases with increasing cluster size over the above-indicated ranges.

Journal Article↗

Formation and distribution of neutral vanadium, niobium, and tantalum oxide clusters: single photon ionization at 26.5 eV.

Neutral vanadium, niobium, and tantalum oxide clusters are studied by single photon ionization employing a 26.5 eV/photon soft x-ray laser. During the ionization process the metal oxide clusters are almost free of fragmentation. The most stable neutral clusters of vanadium, niobium, and tantalum oxides are of the general form (MO2)0,1(M2O5)y. M2O5 is identified as a basic building unit for these three neutral metal oxide species. Each cluster family (Mm, m=1,...,9) displays at least one oxygen deficient and/or oxygen rich cluster stoichiometry in addition to the above most stable species. For tantalum and niobium families with even m, oxygen deficient clusters have the general formula (MO2)2(M2O5)y. For vanadium oxide clusters, oxygen deficient clusters are detected for all cluster families Vm (m=1,[ellipsis (horizontal)],9), with stable structures (VO2)x(V2O5)y. Oxygen rich metal oxide clusters with high ionization energies (IE>10.5 eV, 118 nm photon) are detected with general formulas expressed as (MO2)2 (M2O5)y O1,2,3. Oxygen rich clusters, in general, have up to three attached hydrogen atoms, such as VO3H1,2, V2O5H1,2, Nb2O5H1,2, etc.

Journal Article↗

Use of ev loci as a measure of inbreeding in domestic fowls.

1. The endogenous avian leukosis virus (ev) loci present in 9 lines of domestic fowls have been partially characterised and the average heterozygosity of the loci in each line calculated. 2. Using these data an estimate of the coefficient of inbreeding of the lines was derived; this estimate of the extent of inbreeding is compared with the mating history of the lines. 3. This method provides the first means of directly assessing the degree of inbreeding of fowl lines: assumptions implicit in the method are discussed.

Animals↗

Additivity of detector responses of a portable direct-reading 10.2 eV photoionization detector and a flame ionization gas chromatograph for atmospheres of multicomponent organics: use of PID/FID ratios.

The H-Nu PI-101 with a photoionization detector (PID) of 10.2 eV and the Century OVA-128 equipped with a flame ionization detector (FID) were evaluated for the additivity of their responses to a defined mixture of dissimilar organic vapors at a 0 and 90% relative humidity (RH). The responses of both instruments were additive as long as the effect of RH was accounted for with the PID. The PI-101 was not as precise as the Century OVA-128 for 90% RH atmospheres. PID/FID ratios did not change in the presence of 90% RH as long as the effect of RH also was accounted for in the PID reading.

Chemistry Techniques, Analytical↗

Inference of a 7.75 eV lower limit in the ultraviolet pumping of interstellar polycyclic aromatic hydrocarbon cations with resulting unidentified infrared emissions.

The discrete infrared features known as the unidentified infrared (UIR) bands originating in starburst regions of other galaxies, and in H II regions and planetary nebulae within the Milky Way, are widely thought to be the result of ultraviolet pumped infrared fluorescence of polycyclic aromatic hydrocarbon (PAH) molecules and ions. These UIR emissions are estimated to account for 10%-30% of the total energy emitted by galaxies. Laboratory absorption spectra including the vacuum ultraviolet region, as described in this paper, show a weakening of the intensity of absorption features as the population of cations increases, suggesting that strong pi* <-- pi transitions are absent in the spectra of PAH cations. This implies a lower energy bound for ultraviolet photons that pump infrared emissions from such ions at 7.75 eV, an amount greater than previously thought. The implications include size and structure limitations on the PAH molecules and ions which are apparent constituents of the interstellar medium. Also, this might affect estimations of the population of early-type stars in regions of rapid star formation.

Astronomy↗

Response of thermoluminescent lithium fluoride (TLD-100) to photon beams of 275, 400, 500, 600, 730, 900, 1200, 1500, and 2500 eV.

LiF:Mg,Ti (TLD-100) extruded ribbons and cleaved crystals were exposed to monoenergetic photons of 275-2550 eV energy to determine their potential usefulness as radiation dosimeters for radiobiology experiments at these energies. The radiation source was synchrotron radiation from the 1 GeV electron storage ring, Aladdin. The authors report TLD response and glow curves for He- and air-annealed dosimeters. The undesirable effects of air annealing increase with decreasing photon penetration in the dosimeter. Under certain experimental conditions, UV radiation produced anomalous bleaching of high-temperature traps. The crystals and the chips presented a supralinear response, Supralinearity factors were determined to be of the order of 1.5 for crystals, and 1.7 for the chips. The authors' results indicate that TLDs are a reliable means to monitor the total energy deposited in irradiated cells and are now used routinely for radiobiology cell irradiations.

Biophysical Phenomena↗

A Monte Carlo track structure code for electrons (approximately 10 eV-10 keV) and protons (approximately 0.3-10 MeV) in water: partitioning of energy and collision events.

An event-by-event Monte Carlo simulation code for track structure studies is described. In the present form the code transports protons (approximately 0.3-10 MeV) and electrons (approximately 10 eV-10 keV) in a water medium in the gas phase approximation. For the type of particles and energy range considered, ionization, electronic excitation and electron elastic scattering are the most important collision events accounted for in the transport simulation. Efforts were made to ensure that the analytic representation of the various interaction cross sections rests on well established experimental data and theory. For example, the secondary-electron spectrum as well as partial and total ionization cross sections are represented by a semitheoretical formulation combining Bethe's asymptotic expansion and binary-encounter theory. Binding effects for five levels of ionization and eight levels of electronic excitation of the water molecule are explicitly considered. The validity of the model cross sections is examined against available experimental data and theoretical predictions from other similar studies. Results pertaining to the partitioning of energy loss and interaction events for the first-collision probability and nanometre-size track segments are presented.

Electrons↗

Development of a sub-eV resolution soft-X-ray spectrometer for a transmission electron microscope.

We constructed a grazing-incidence soft-X-ray spectrometer for a transmission electron microscope. The spectrometer, which was composed of a grating and a CCD detector, was attached to a JEM2000FX transmission electron microscope. B K-emission spectra of hexagonal boron-nitride, which give the density of states of the valence band of the material, were obtained with an energy resolution of about 0.6 eV.

Letter↗

Modelling of DNA damage induced by energetic electrons (100 eV to 100 keV).

Modelling and calculations are presented for the spectrum of initial DNA damage produced by 100 eV to 100 keV energetic electrons. Analysis of the initial spectrum of damage, based upon the source (direct energy deposition and reactions with diffusing OH radicals) and complexity of damage, indicates that the majority of the interactions cause no damage to DNA and any damage that does occur is most likely to be a simple single strand break (SSB). The fraction of complex damage for energetic electrons is lower than that induced by low energy electrons and ultrasoft X rays but still represents an appreciable fraction (20-30%) of the total double strand breaks (DSBs). Relative yields of strand breaks are investigated for dependence on the assumed energy deposition threshold and on the probability of the hydroxyl radicals to produce a single strand break. The ratio of direct to indirect damage does not change significantly across the electron energy range investigated and the values lie well within the experimental data. The direct energy deposition in DNA represents a larger proportion of the damage although the contribution from the hydroxyl radicals is also substantial, both in terms of the absolute yield of the breaks and the complexity of the damage.

Computer Simulation↗

Electron beam transport in heterogeneous slab media from MeV down to eV.

An optimized Monte Carlo method based on the null collision technique and on the treatment of individual interactions is used for the simulation of the electron transport in multilayer materials from high energies (MeV or several hundred of keV) down to low cutoff energies (between 1 and 10 eV). In order to better understand the electron transport and the energy deposition at the interface in the composite application framework, two layer materials are considered (carbon and polystyrene with densities of 1.7 g cm(-3) and 1.06 g cm(-3), respectively) under two slab or three slab configurations as, e.g. a thin layer of carbon sandwiched between two polystyrene layers. The electron-matter cross-sections (electron-carbon and electron-polystyrene) used in the case of pure material (carbon and polystyrene) as well as our Monte-Carlo code have been first validated. The boundary interface layer is considered without any mean free path truncation and with a rigorous treatment of the backscattered and also the forward scattered electrons from one layer to another. The large effect of the choice of a low cutoff energy and the dissociation process consideration are also clearly shown in the heterogeneous multi-layer media more particularly on the secondary electron emission, inelastic collision number and energy spectra.

Carbon↗

Proximity functions for electrons from 100 eV to 10 MeV.

The objective of this study is to provide a set of proximity functions for electrons from 100 eV to 10 MeV. Numerical results of differential proximity functions are given graphically. The complete data set is available electronically upon request from the authors. The results can serve as a convenient database for anyone performing microdosimetric calculations in radiation fields of electrons. For mixed fields of electrons, the proximity functions can easily be derived from the proximity functions of monoenergetic electrons presented here.

Computer Simulation↗

Evidence for changing of cosmic ray composition between 10(17) and 10(18) eV from multicomponent measurements

The average mass composition of cosmic rays with primary energies between 10(17) and 10(18) eV has been studied using a hybrid detector consisting of the High Resolution Fly's Eye (HiRes) prototype and the MIA muon array. Measurements have been made of the change in the depth of shower maximum and the muon density as a function of energy. The results show that the composition is changing from a heavy to lighter mix as the energy increases.

Journal Article↗

Limits on the existence of heavy neutrinos in the range 50-1000 eV from the study of the 187Re beta decay.

We analyzed the spectrum of the 187Re beta decay, obtained with a cryogenic microcalorimeter, searching for heavy neutrinos in the mass range 50-1000 eV. No evidence has been found for them and the upper limits on the mixing angle with a zero-mass neutrino are reported. Upper limits of 9x10(-3) at 1000 eV/c(2), 1.2x10(-2) at 500 eV/c(2), 4.4x10(-2) at 200 eV/c(2), and 0.116 at 100 eV/c(2) at 95% C.L. have been obtained. These upper limits are a factor of 2 to 4 lower than the current limits reported in the literature.

Journal Article↗

Neutrinos of energy approximately 10(16) eV from gamma-ray bursts in pulsar wind bubbles.

The supranova model for gamma-ray bursts (GRBs) is becoming increasingly more popular. In this scenario the GRB occurs weeks to years after a supernova explosion, and is located inside a pulsar wind bubble (PWB). Protons accelerated in the internal shocks that emit the GRB may interact with the external PWB photons producing pions which decay into approximately 10(16) eV neutrinos. A km(2) neutrino detector would observe several events per year correlated with the GRBs.

Journal Article↗

DNA strand breaks induced by 0-4 eV electrons: the role of shape resonances.

Collisions of 0-4 eV electrons with thin DNA films are shown to produce single strand breaks. The yield is sharply structured as a function of electron energy and indicates the involvement of pi* shape resonances in the bond breaking process. The cross sections are comparable in magnitude to those observed in other compounds in the gas phase in which pi* electrons are transferred through the molecule to break a remote bond. The results therefore support aspects of a theoretical study by Barrios et al. [J. Phys. B 106, 7991 (2002)]] indicating that such a mechanism could produce strand breaks in DNA.

Biophysical Phenomena↗