Electron temperature in a decaying molecular nitrogen plasma in the presence of weak electric fields

The electron energy distribution function in an afterglow molecular nitrogen plasma is studied both experimentally and theoretically under the conditions of weak electric fields such that the electron gas is heated by superelastic collisions of electrons with vibrationally excited molecules. Based on the mean electron energy balance, it is established that, depending on the degree of plasma ionization and the vibrational temperature of nitrogen molecules, an afterglow plasma may evolve into two states, differing in electron temperature. This kind of bistability is found to stem from the difference in the main mechanisms for electron energy losses in the two stable states. The prediction that the shape of the electron energy distribution function should change in a jumplike manner when a weak electric field is imposed has been confirmed experimentally.     

Cross sections for low-energy (1-100 eV) electron elastic and inelastic scattering in amorphous ice

We report the integral cross sections per scatterer (i.e. elastic collision, phonon excitations, vibrational excitations, electronic excitations and ionization) for 1-100 eV electron scattering in an amorphous film of ice condensed at a temperature of 14 K. The integral cross sections are determined relative to the total from a two-stream multiple-scattering analysis of the electron energy distribution backscattered from the film. Their energy dependence is obtained from both the analysis of the elastic electron reflectivity as a function of the film thickness and the vibrational electron energy-loss spectra measured for several incident energies and large film thickness. The magnitude and various features found in the energy dependence of the cross sections are discussed, whenever possible, by comparison with data and with scattering mechanisms available in the gas phase. Microcospic effects, which are implicitly included in cross sections determined in this way, are discussed in terms of interference and coherent multiple-scattering contributions among the scattering sites as well as interactions of the scattering sites with their neighbors in the condensed phase.     

Analysis of Data on the Cross Sections for Electron-Impact Ionization and Excitation of Electronic States of Atomic Hydrogen (Review)

A review is given of experimental and theoretical data on the cross sections for ionization, excitation, and deexcitation of atomic hydrogen. The set of the cross sections required to calculate the electron energy distribution function and find the level-to-level rate coefficients needed to solve balance equations for the densities of neutral and charged particles in hydrogen plasma is determined.     

Investigation of the electron energy distribution function in hollow-cathode glow discharges in nitrogen and oxygen

The mechanism for the formation of the inverse electron distribution function is proposed and realized experimentally in a nitrogen plasma of a hollow-cathode glow discharge. It is shown theoretically and experimentally that, for a broad range of the parameters of an N₂ discharge, it is possible to form a significant dip in the profile of the electron distribution function in the energy range ε=2–4 eV and, accordingly, to produce the inverse distribution with df(ε)/d?>0. The formation of a dip is associated with both the vibrational excitation of N₂ molecules and the characteristic features of a hollow-cathode glow discharge. In such a discharge, the applied voltage drops preferentially across a narrow cathode sheath. In the main discharge region, the electric field E is weak (E<0.1 V/cm at a pressure of about p～0.1 torr) and does not heat the discharge plasma. The gas is ionized and the ionization-produced electrons are heated by a beam of fast electrons (with an energy of about 400 eV) emitted from the cathode. A high-energy electron beam plays an important role in the formation of a dip in the profile of the electron distribution function in the energy range in which the cross section for the vibrational excitation of nitrogen molecules is maximum. A plasma with an inverted electron distribution function can be used to create a population inversion in which more impurity molecules and atoms will exist in electronically excited states.     

Possibility of revealing the role of nonresonant energy exchange between electrons and CO molecules at high vibrational levels

An experimental method providing information about the interaction of electrons with excited CO molecules at high vibrational levels is proposed and justified theoretically. The suggested experimental scheme is based on the use of two successive discharge pulses under the conditions prevailing in an electroionization CO laser. The first pulse should ensure a sufficiently high energy input in order for a nonequilibrium vibrational distribution function to form. The second pulse serves to study the effect of the electric current on the vibrational distribution function of excited molecules at high vibrational levels. The theoretical analysis is based on the simultaneous solution of the Boltzmann equation for the electron energy distribution function and the vibrational kinetic equations realistically describing the multiquantum vibrational-vibrational exchange processes. The calculated results show that the sensitivity of the proposed measurement technique promises to be high.     

Vibrational distribution of nitrogen molecules in the C3Πu state in a near-surface microwave plasma in nitrogen at pressures of 1–5 Torr

The radiation of the second positive nitrogen system has been used to study the spatial dependence of the vibrational distribution of nitrogen molecules in the C³Π_u state in the near-surface plasma layer of an electrode microwave discharge in nitrogen at pressures of 1–5 Torr. It has been shown that the vibrational distribution changes at a scale of 100 μm. It has been concluded that this state is populated owing to the electron impact from the ground state. The possibility of using the local approximation for the electron energy distribution function to explain the experimental results has been analyzed.     

Pink splash of active nitrogen in the discharge afterglow

Results are presented from experimental studies of the glow dynamics of active nitrogen in the stage of its excitation by a current pulse and during the discharge afterglow. The mechanism is proposed for the generation of a light splash in a highly activated nitrogen after the end of its pulsed excitation. The key role in the generation of this splash is played by the D-V processes, by which the dissociation energy is transferred to the vibrational degrees of freedom in the course of recombination of nitrogen atoms, and the V-E processes, by which the vibrational energy of highly excited molecules N₂(X, v ≥ 25–27) is transferred to the emitting electronic states N₂(B, v) after the V-V delay. Results of simulations based on the mechanism proposed are also presented.     

Cross section calculations for electron scattering from DNA and RNA bases

Differential and integral cross sections for elastic electron collisions with uracil, cytosine, guanine, adenine and thymine have been calculated using the independent atom method with a static-polarization model potential for incident energies ranging from 50 to 4000 eV. Total cross sections for single electron-impact ionization of selected DNA and RNA bases have also been calculated with the binary-encounter-Bethe model from the ionization threshold up to 5000 eV. Cross sections within the investigated energy range, can be related to the molecular symmetry, the number of target electrons and molecular size; elastic and ionization processes are most efficient for guanine and adenine molecules, while the lowest cross sections were obtained for the uracil molecule. The ionization cross sections for cytosine, thymine, adenine and guanine are compared with those recently obtained with a semi-classical and binary-encounter-Bethe formalisms. No theoretical and experimental data for elastic electron scattering from DNA and RNA bases are available, but comparisons with calculations for molecules of similar size and geometry allows the validity of the theoretical approach to be verified.     

Diagnostics of a nonequilibrium nitrogen plasma from the emission spectra of the second positive system of N2

A method is proposed for determining the electron density N _e and the electric field E in the non-equilibrium nitrogen plasma of a low-pressure discharge from the spectra of the second positive system of N₂. The method is based on measuring the specific energy deposition in the plasma and the distribution of nitrogen molecules over the vibrational levels of the C ³Π _u state, as well as on modeling this distribution for a given energy deposition. The fitting parameters of the model are the values of N _e and E. A kinetic model of the processes governing the steady-state density of the C ³Π _u nitrogen molecules is developed. The testing of this method showed it to be quite reliable. The method is of particular interest for diagnosing electrodeless discharges and provides detailed information on the processes occurring in the discharge plasma. Preliminary data are obtained on the plasma parameters in a cavity microwave discharge and an electrode microwave discharge. In particular, it is found that the electric field in an electrode microwave discharge in nitrogen is lower than that in a hydrogen discharge. This effect is shown to be produced by stepwise and associative processes with the participation of excited particles in nitrogen.     

Cross sections for low-energy (10-50 eV) electron damage to DNA

We report direct measurements of the formation of single-, double- and multiple strand breaks in pure plasmid DNA as a function of exposure to 10-50 eV electrons. The effective cross sections to produce these different types of DNA strand breaks were determined and were found to range from approximately 10(-17) to 3 x 10(-15) cm(2). The total effective cross section and the effective range for destruction of supercoiled DNA extend from 3.4 to 4.4 x 10(-15) cm(2) and 12 to 14 nm, respectively, over the range 10-50 eV. The variation of the effective cross sections with electron energy is discussed in terms of the electron's inelastic mean free path, penetration depth, and dissociation mechanisms, including resonant electron capture; the latter is found to dominate the effective cross sections for single- and double-strand breaks at 10 eV. The most striking observations are that (1) supercoiled DNA is approximately one order of magnitude more sensitive to the formation of double-strand breaks by low-energy electrons than is relaxed circular DNA, and (2) the dependence of the effective cross sections on the incident electron energy is unrelated to the corresponding ionization cross sections. This finding suggests that the traditional notion that radiobiological damage is related to the number of ionization events would not apply at very low energies.     

Probing the FQR and NDH activities involved in cyclic electron transport around Photosystem I by the 'afterglow' luminescence

Far-red illumination of plant leaves for a few seconds induces a delayed luminescence rise, or afterglow, that can be measured with the thermoluminescence technique as a sharp band peaking at around 40-45 degrees C. The afterglow band is attributable to a heat-induced electron flow from the stroma to the plastoquinone pool and the PSII centers. Using various Arabidopsis and tobacco mutants, we show here that the electron fluxes reflected by the afterglow luminescence follow the pathways of cyclic electron transport around PSI. In tobacco, the afterglow signal relied mainly on the ferredoxin-quinone oxidoreductase (FQR) activity while the predominant pathway responsible for the afterglow in Arabidopsis involved the NAD(P)H dehydrogenase (NDH) complex. The peak temperature T(m) of the afterglow band varied markedly with the light conditions prevailing before the TL measurements, from around 30 degrees C to 45 degrees C in Arabidopsis. These photoinduced changes in Tm followed the same kinetics and responded to the same light stimuli as the state 1-state 2 transitions. PSII-exciting light (leading to state 2) induced a downward shift while preillumination with far-red light (inducing state 1) caused an upward shift. However, the light-induced downshift was strongly inhibited in NDH-deficient Arabidopsis mutants and the upward shift was cancelled in plants durably acclimated to high light, which can perform normal state transitions. Taken together, our results suggest that the peak temperature of the afterglow band is indicative of regulatory processes affecting electron donation to the PQ pool which could involve phosphorylation of NDH. The afterglow thermoluminescence band provides a new and simple tool to investigate the cyclic electron transfer pathways and to study their regulation in vivo.     

Accurate electron inelastic cross sections and stopping powers for liquid water over the 0.1-10 keV range based on an improved dielectric description of the Bethe surface

Electron inelastic cross sections and stopping powers for liquid water over the 0.1-10 keV range are presented based on a recently developed dielectric response model for liquid water (D. Emfietzoglou, F. Cucinotta and H. Nikjoo, Radiat. Res. 164, 202-211, 2005) that is consistent with the experimental data over the whole energy-momentum plane. Both exchange and second-order Born corrections are included in a material-specific way using the dielectric functions of liquid water. The numerical results are fitted by simple analytic functions to facilitate their further use. Compared to previous studies, differential cross sections are shifted toward smaller energy losses resulting in smaller inelastic and stopping cross sections with differences reaching, on average, the approximately 20% and approximately 50% level, respectively. Contrary to higher energies, it is shown that the dispersion model for the momentum dependence of the dielectric functions (Bethe ridge) is as important as the optical model used. Within the accuracy of the experimental data (a few percent) upon which our dielectric model is based, the calculations are "exact" to first order, while the uncertainty of the results beyond first order is estimated at the 5-10% level. The present work overcomes the limitations of Bethe's theory at low energies by a self-consistent account of inner-shell effects and may serve to extend the ICRU electron stopping power database for liquid water down to 100 eV with a level of uncertainty similar to that for the higher-energy values.     

Comparison and assessment of electron cross sections for Monte Carlo track structure codes.

The purpose of this study was to make an intercomparison and assessment of cross sections for electrons in water used in electron track structure codes. This study is intended to shed light on the extent to which the differences between the input data and physical and chemical assumptions influence the outcome in biophysical modeling of radiation effects. Ionization cross sections and spectra of secondary electrons were calculated by various theories. The analyses were carried out for water vapor cross sections, as these are more abundant and readily available. All suitable published experimental total ionization cross sections were fitted by an appropriate function and used for generation of electron tracks. Three sets of compiled data were used for comparison of total excitation cross sections and mean excitation energy. The tracks generated by a Monte Carlo track code, using various combinations of cross sections, were compared in terms of radial distributions of interactions and point kernels. The spectrum of secondary electrons emitted by the ionization process was found to be the factor that has the most influence on these quantities. A different set of cross sections for excitation and elastic scattering did not affect the electron track structure as much as did ionization cross sections. It is concluded that all codes, using different cross sections and in different phase, currently used for biophysical modeling exhibit close similarities for energy deposition in larger size targets while appreciable differences are observed in B-DNA-size targets. We recommend fitted functions to all available suitable experimental data for the total ionization and elastic cross sections. We conclude that most codes produce tracks in reasonable agreement with the macroscopic quantities such as total stopping power and total yield of strand breaks. However, we predict differences in frequencies of clustering in tracks from the different models.     

Probing the FQR and NDH activities involved in cyclic electron transport around Photosystem I by the ‘afterglow’ luminescence

Far-red illumination of plant leaves for a few seconds induces a delayed luminescence rise, or afterglow, that can be measured with the thermoluminescence technique as a sharp band peaking at around 40-45 °C. The afterglow band is attributable to a heat-induced electron flow from the stroma to the plastoquinone pool and the PSII centers. Using various Arabidopsis and tobacco mutants, we show here that the electron fluxes reflected by the afterglow luminescence follow the pathways of cyclic electron transport around PSI. In tobacco, the afterglow signal relied mainly on the ferredoxin-quinone oxidoreductase (FQR) activity while the predominant pathway responsible for the afterglow in Arabidopsis involved the NAD(P)H dehydrogenase (NDH) complex. The peak temperature T_m of the afterglow band varied markedly with the light conditions prevailing before the TL measurements, from around 30 °C to 45 °C in Arabidopsis. These photoinduced changes in T_m followed the same kinetics and responded to the same light stimuli as the state 1-state 2 transitions. PSII-exciting light (leading to state 2) induced a downward shift while preillumination with far-red light (inducing state 1) caused an upward shift. However, the light-induced downshift was strongly inhibited in NDH-deficient Arabidopsis mutants and the upward shift was cancelled in plants durably acclimated to high light, which can perform normal state transitions. Taken together, our results suggest that the peak temperature of the afterglow band is indicative of regulatory processes affecting electron donation to the PQ pool which could involve phosphorylation of NDH. The afterglow thermoluminescence band provides a new and simple tool to investigate the cyclic electron transfer pathways and to study their regulation in vivo.     

Transverse glow discharges in supersonic air and methane flows

Transverse glow discharges in supersonic air and methane flows are studied both experimentally and theoretically. The experiments show that a diffuse volume discharge filling the whole cross section of the flow can easily be initiated in air, whereas a diffuse discharge in a methane flow shows a tendency to transition into a constricted mode. The electron transport coefficients (mobility and drift velocity) and the kinetic coefficients (such as collisional excitation rates of the vibrational levels of a methane molecule, as well as dissociation and ionization rates) are calculated by numerically solving the Boltzmann equation for the electron energy distribution function. The calculated coefficients are used to estimate the parameters of the plasma and the electric field in the positive column of a discharge in methane.     

Calculation on spectrum of direct DNA damage induced by low-energy electrons including dissociative electron attachment

In this work, direct DNA damage induced by low-energy electrons (sub-keV) is simulated using a Monte Carlo method. The characteristics of the present simulation are to consider the new mechanism of DNA damage due to dissociative electron attachment (DEA) and to allow determining damage to specific bases (i.e., adenine, thymine, guanine, or cytosine). The electron track structure in liquid water is generated, based on the dielectric response model for describing electron inelastic scattering and on a free-parameter theoretical model and the NIST database for calculating electron elastic scattering. Ionization cross sections of DNA bases are used to generate base radicals, and available DEA cross sections of DNA components are applied for determining DNA-strand breaks and base damage induced by sub-ionization electrons. The electron elastic scattering from DNA components is simulated using cross sections from different theoretical calculations. The resulting yields of various strand breaks and base damage in cellular environment are given. Especially, the contributions of sub-ionization electrons to various strand breaks and base damage are quantitatively presented, and the correlation between complex clustered DNA damage and the corresponding damaged bases is explored. This work shows that the contribution of sub-ionization electrons to strand breaks is substantial, up to about 40–70%, and this contribution is mainly focused on single-strand break. In addition, the base damage induced by sub-ionization electrons contributes to about 20–40% of the total base damage, and there is an evident correlation between single-strand break and damaged base pair A–T.     

Classical molecular dynamics simulation of the photoinduced electron transfer dynamics of plastocyanin.

Classical molecular dynamics simulations are used to investigate the nuclear motions associated with photoinduced electron transfer in plastocyanin. The blue copper protein is modeled using a molecular mechanics potential; potential parameters for the copper-protein interactions are determined using an x-ray crystallographic structure and absorption and resonance Raman spectra. Molecular dynamics simulations yield a variety of information about the ground (oxidized) and optically excited (charge-transfer) states: 1) The probability distribution of the potential difference between the states, which is used to determine the coordinate and energy displacements, places the states well within the Marcus inverted region. 2) The two-time autocorrelation function of the difference potential in the ground state and the average of the difference potential after instantaneous excitation to the excited state are very similar (confirming linear response in this system); their decay indicates that vibrational relaxation occurs in about 1 ps in both states. 3) The spectral densities of various internal coordinates begin to identify the vibrations that affect the optical transition; the spectral density of the difference potential correlation function should also prove useful in quantum simulations of the back electron transfer. 4) Correlation functions of the protein atomic motions with the difference potential show that the nuclear motions are correlated over a distance of more than 20 A, especially along proposed electron transport paths.     

A rapid method for assessing the distribution of gold labeling on thin sections.

Particulate gold labeling on ultrathin sections is in widespread use for antigen localization at the EM level. To extend the usefulness of gold labeling technology, we are evaluating different methods for sampling and estimating quantities of gold labeling. Here we present a simple, rapid, and unbiased method for assessing the relative pool sizes of immunogold labeling distributed over different cell compartments. The method uses a sampling approach developed for stereology in which a regular array of microscopic fields or linear scans is positioned randomly on labeled sections. From these readouts, gold particles are counted and assigned to identifiable cell structures to construct a gold labeling frequency distribution of those labeled compartments. Here we use ultrathin cryosections labeled for a range of different proteins and for a signaling lipid. We show by scanning labeled sections at the electron microscope that counting 100-200 particles on each of two grids is sufficient to obtain a reproducible and rapid assessment of the pattern of labeling proportions over 10-16 compartments. If more precise estimates of labeling proportions over individual compartments are required (e.g., to achieve coefficients of error of 10-20%), then 100-200 particles need to be counted over each compartment of interest.     

Studies on thylakoid phosphorylation and noncyclic electron transport

The effect of thylakoid phosphorylation on noncyclic electron transport in spinach chloroplasts was investigated by measuring both the reduction of nicotinamide adenine dinucleotide phosphate (NADP) and the steady-state redox level of the primary electron acceptor quinone of photosystem II (Q) during electron flow to NADP. These data are compared with the theoretical predictions for an electron transport model which relates both the redox levels of Q and the photosystem II optical cross section to the overall velocity of noncyclic electron flow. It is demonstrated that transfer of 15-20% of the photosystem II antenna to photosystem I may stimulate electron flow to NADP only if Q is less than 60-70% oxidized (this condition exists with our thylakoids, even at extremely low absorption fluxes, when the illumination is not specifically enriched in photosystem I absorbed wavelengths); in phosphorylated thylakoids the steady-state redox level Q is substantially shifted to a more oxidized one (measurements of this parameter using light of different wavelengths quantitatively support the idea that thylakoid phosphorylation leads to increased photosystem I and decreased photosystem II cross sections); thylakoid phosphorylation leads to stimulated noncyclic electron flow to NADP only when the increased photosystem I antenna is able to bring about large increases in the steady-state level of oxidized Q.