Ion-acoustic waves in a complex plasma with negative ions

Negative ions and negatively charged micro- to nano-meter sized dust grains are ubiquitous in astrophysical as well as industrial processing plasmas. The negative ions can appear in electro-negative plasmas as a result of elementary processes such as dissociative or non-dissociative electron attachment to neutrals. They are usually rather small in number, and in general do not affect the overall plasma behavior. On the other hand, since the dust grains are almost always highly negative, even in small numbers they can take up a considerable proportion of the total negative charge in the system. The presence of dusts can affect the characteristics of most collective processes of the plasma since the charge balance in both the steady and dynamic states can be significantly altered. Another situation that often occurs is that the electron number density becomes small because of their absorption by the dust grains or the discharge walls. In this case the negative ions in the plasma can play a very important role. Here, a self-consistent theory of linear waves in complex laboratory plasmas containing dust grains and negative ions is presented. A comprehensive model for such plasmas including source and sink effects associated with the presence of dust grains and negative ions is introduced. The stationary state of the plasma as well as the dispersion and damping characteristics of the waves are investigated. All relevant processes, such as ionization, diffusion, electron attachment, negative-positive ion recombination, dust charge relaxation, and dissipation due to electron and ion elastic collisions with neutrals and dust particles, as well as charging collisions with the dusts, are taken into consideration.

Suppression of cluster ions during particle formation events in the atmosphere

Cluster ions and charged and neutral nanoparticle concentrations were monitored using a neutral cluster and air ion spectrometer (NAIS) over a period of one year in Brisbane, Australia. The study yielded 242 complete days of usable data, of which particle formation events were observed on 101 days. Small, intermediate and large ion concentrations were evaluated in real time. In the diurnal cycle, small ion concentration was highest during the second half of the night while large ion concentrations were a maximum during the day. The small ion concentration showed a decrease when the large ion concentration increased. Particle formation was generally followed by a peak in the intermediate ion concentration. The rate of increase of intermediate ions was used as the criteria for identifying particle formation events. Such events were followed by a period of growth to larger sizes and usually occurred between 8 am and 2 pm. Particle formation events were found to be related to the wind direction. The gaseous precursors for the production of secondary particles in the urban environment of Brisbane have been shown to be ammonia and sulfuric acid. During these events, the nanoparticle number concentrations in the size range 1.6 to 42 nm, which were normally lower than 1x104 cm-3, often exceeded 5x104 cm-3 with occasional values over 1x105 cm-3. Cluster ions generally occurred in number concentrations between 300 and 600 cm-3 but decreased significantly to about 200 cm-3 during particle formation events. This was accompanied by an increase in the large ion concentration. We calculated the fraction of nanoparticles that were charged and investigated the occurrence of possible overcharging during particle formation events. Overcharging is defined as the condition where the charged fraction of particles is higher than in charge equilibrium. This can occur when cluster ions attach to neutral particles in the atmosphere, giving rise to larger concentrations of charged particles in the short term. Ion-induced nucleation is one of the mechanisms of particle formation in the atmosphere, and overcharging has previously been considered as an indicator of this process. The possible role of ions in particle formation was investigated.

Measurement of small ions near a busy motorway

Combustion sources are well-known sources of electrical ions (Howard, J.B. et al. 1973). Motor vehicles emissions are one of the main sources of ions in urban environments. The presence of charged particles in motor vehicle emissions has been known for many years (Kittelson, 1986; Yu et al, 2004; Jung and Kittelson, 2005). Although these particles are probably charged by the attachment of air ions, there is very little information on the nature, sign and magnitude of the small ions (diameter < 1.6 nm) emitted by motor vehicles and/or present by the sides of roads.

Dispersion of corona ions downwind from a high-voltage power line

Corona discharge is responsible for the small ions found near overhead power lines, and these are capable of modifying the ambient electrical environment such as the dc electric field at ground level (Fews, Wilding et al. 2002). Once produced, small ions quickly attach to aerosol particles in the air, producing ‘large ions’ which are roughly 1 nm to 1 µm in diameter. However, very few studies have reported measurements of ions produced by power lines and its impact on particle charge concentrations. In this present study, the measurements were conducted as a function of normal downwind distance from a 275kV power line for investigating the effect of corona ions on air ions, aerosol particle charge concentration and dc e-filed.

Suppression of cluster ions during rapidly increasing particle number concentration events in the environment

We show that the cluster ion concentration (CIC) in the atmosphere is significantly suppressed during events that involve rapid increases in particle number concentration (PNC). Using a neutral cluster and air ion spectrometer, we investigated changes in CIC during three types of particle enhancement processes – new particle formation, a bushfire episode and an intense pyrotechnic display. In all three cases, the total CIC decreased with increasing PNC, with the rate of decrease being greater for negative CIC than positive. We attribute this to the greater mobility, and hence the higher attachment coefficient, of negative ions over positive ions in the air. During the pyrotechnic display, the rapid increase in PNC was sufficient to reduce the CIC of both polarities to zero. At the height of the display, the negative CIC stayed at zero for a full 10 min. Although the PNCs were not significantly different, the CIC during new particle formation did not decrease as much as during the bushfire episode and the pyrotechnic display. We suggest that the rate of increase of PNC, together with particle size, also play important roles in suppressing CIC in the atmosphere.

Impact of particle formation on atmospheric ions and particle number concentrations in an urban environment

A measurement campaign was conducted from 3 to 19 December 2012 at an urban site of Brisbane, Australia. Size distribution of ions and particle number concentrations were measured to investigate the influence of particle formation and biomass burning on atmospheric ion and particle concentrations. Overall ion and particle number concentrations during the measurement period were found to be (-1.2 x 103 cm-3 | +1.6 x 103 cm-3) and 4.4 x 103, respectively. The results of correlation analysis between concentrations of ions and nitrogen oxides indicated that positive and negative ions originated from similar sources, and that vehicle exhaust emissions had a more significant influence on intermediate/large ions, while cluster ions rapidly attached to larger particles once emitted into the atmosphere. Diurnal variations in ion concentration suggested the enrichment of intermediate and large ions on new particle formation event days, indicating that they were involved in the particle formation processes. Elevated total ions, particularly larger ions, and particle number concentrations were found during biomass burning episodes. This could be due to the attachment of cluster ions onto accumulation mode particles or production of charged particles from biomass burning, which were in turn transported to the measurement site. The results of this work enhance scientific understanding of the sources of atmospheric ions in an urban environment, as well as their interactions with particles during particle formation processes.

Comparison of charged nanoparticle concentrations near busy roads and overhead high-voltage power lines

Overhead high-voltage power lines are known sources of corona ions. These ions rapidly attach to aerosols to form charged particles in the environment. Although the effect of ions and charged particles on human health is largely unknown, much attention has focused on the increasing exposure as a result of the expanding power network in urban residential areas. However, it is not widely known that a large number of charged particles in urban environments originate from motor vehicle emissions. In this study, for the first time, we compare the concentrations of charged nanoparticles near busy roads and overhead power lines. We show that large concentrations of both positive and negative charged nanoparticles are present near busy roadways and that these concentrations commonly exceed those under high-voltage power lines. We estimate that the concentration of charged nanoparticles found near two freeways carrying around 120 vehicles per minute exceeded the corresponding maximum concentrations under two corona-emitting overhead power lines by as much as a factor of 5. The difference was most pronounced when a significant fraction of traffic consisted of heavy-duty diesel vehicles which typically have high particle and charge emission rates.

Diffusion of flexible, charged, nanoscopic molecules in solution: Size and pH dependence for PAMAM dendrimer

In order to understand self-diffusion (D) of a charged, flexible, and porous nanoscopic molecule in water, we carry out very long, fully atomistic molecular dynamics simulation of PAMAM dendrimer up to eight generations in explicit salt water under varying pH. We find that while the radius of gyration (R-g) varies as N-1/3, the self-diffusion constant (D) scales, surprisingly, as N-alpha, with alpha=0.39 at high pH and 0.5 at neutral pH, indicating a dramatic breakdown of Stokes-Einstein relation for diffusion of charged nanoscopic molecules. The variation in D as a function of radius of gyration demonstrates the importance of treating water and ions explicitly in the diffusion process of a flexible nanoscopic molecule. In agreement with recent experiments, the self-diffusion constant increases with pH, revealing the importance of dielectric friction in the diffusion process. The shape of a dendrimer is found to fluctuate on a nanosecond time scale. We argue that this flexibility (and also the porosity) of the dendrimer may play an important role in determining the mean square displacement of the dendrimer and the breakdown of the Stokes-Einstein relation between diffusion constant and the radius.

On formation, growth and concentrations of air ions

Aerosol particles have effect on climate, visibility, air quality and human health. However, the strength of which aerosol particles affect our everyday life is not well described or entirely understood. Therefore, investigations of different processes and phenomena including e.g. primary particle sources, initial steps of secondary particle formation and growth, significance of charged particles in particle formation, as well as redistribution mechanisms in the atmosphere are required. In this work sources, sinks and concentrations of air ions (charged molecules, cluster and particles) were investigated directly by measuring air molecule ionising components (i.e. radon activity concentrations and external radiation dose rates) and charged particle size distributions, as well as based on literature review. The obtained results gave comprehensive and valuable picture of the spatial and temporal variation of the air ion sources, sinks and concentrations to use as input parameters in local and global scale climate models. Newly developed air ion spectrometers (Airel Ltd.) offered a possibility to investigate atmospheric (charged) particle formation and growth at sub-3 nm sizes. Therefore, new visual classification schemes for charged particle formation events were developed, and a newly developed particle growth rate method was tested with over one year dataset. These data analysis methods have been widely utilised by other researchers since introducing them. This thesis resulted interesting characteristics of atmospheric particle formation and growth: e.g. particle growth may sometimes be suppressed before detection limit (~ 3 nm) of traditional aerosol instruments, particle formation may take place during daytime as well as in the evening, growth rates of sub-3 nm particles were quite constant throughout the year while growth rates of larger particles (3-20 nm in diameter) were higher during summer compared to winter. These observations were thought to be a consequence of availability of condensing vapours. The observations of this thesis offered new understanding of the particle formation in the atmosphere. However, the role of ions in particle formation, which is not well understood with current knowledge, requires further research in future.

Pure Coulomb explosions of highly charged methane clusters investigated by a simple electrostatic model

The pure Coulomb explosions of the methane clusters (CA(4))(n), (light atom A = H or D) have been investigated by a simplified electrostatic model for both a single cluster and an ensemble of clusters with a given cluster size distribution. The dependence of the energy of ions produced from the explosions on cluster size and the charge state of the carbon ions has been analysed. It is found that, unlike the average proton energy which increases with the charge q of the carbon ions, the average deuteron energy tends to saturate as q becomes larger than 4. This implies that when the laser intensity is sufficiently high for the (CD4)(n) to be ionized to a charge state of (C4+D4+)(n), the neutron yield from a table-top laser-driven Coulomb explosion of deuterated methane clusters (CD4)(n) could be increased significantly by increasing the interaction volume rather than by increasing the laser intensity to produce the higher charge state (C6+D4+)(n). The flight-time spectra of the carbon ions and the light ions have also been studied.

Effects of self energy of the ions on the double layer structure and properties at the dielectric interface

Although numerous theoretical efforts have been put forth, a systematic, unified and predictive theoretical framework that is able to capture all the essential physics of the interfacial behaviors of ions, such as the Hofmeister series effect, Jones-Ray effect and the salt effect on the bubble coalescence remain an outstanding challenge. The most common approach to treating electrostatic interactions in the presence of salt ions is the Poisson-Boltzmann (PB) theory. However, there are many systems for which the PB theory fails to offer even a qualitative explanation of the behavior, especially for ions distributed in the vicinity of an interface with dielectric contrast between the two media (like the water-vapor/oil interface). A key factor missing in the PB theory is the self energy of the ion.

In this thesis, we develop a self-consistent theory that treats the electrostatic self energy (including both the short-range Born solvation energy and the long-range image charge interactions), the nonelectrostatic contribution of the self energy, the ion-ion correlation and the screening effect systematically in a single framework. By assuming a finite charge spread of the ion instead of using the point-charge model, the self energy obtained by our theory is free of the divergence problems and gives a continuous self energy across the interface. This continuous feature allows ions on the water side and the vapor/oil side of the interface to be treated in a unified framework. The theory involves a minimum set of parameters of the ion, such as the valency, radius, polarizability of the ions, and the dielectric constants of the medium, that are both intrinsic and readily available. The general theory is first applied to study the thermodynamic property of the bulk electrolyte solution, which shows good agreement with the experiment result for predicting the activity coefficient and osmotic coefficient.

Next, we address the effect of local Born solvation energy on the bulk thermodynamics and interfacial properties of electrolyte solution mixtures. We show that difference in the solvation energy between the cations and anions naturally gives rise to local charge separation near the interface, and a finite Galvani potential between two coexisting solutions. The miscibility of the mixture can either increases or decreases depending on the competition between the solvation energy and translation entropy of the ions. The interfacial tension shows a non-monotonic dependence on the salt concentration: it increases linearly with the salt concentration at higher concentrations, and decreases approximately as the square root of the salt concentration for dilute solutions, which is in agreement with the Jones-Ray effect observed in experiment.

Next, we investigate the image effects on the double layer structure and interfacial properties near a single charged plate. We show that the image charge repulsion creates a depletion boundary layer that cannot be captured by a regular perturbation approach. The correct weak-coupling theory must include the self-energy of the ion due to the image charge interaction. The image force qualitatively alters the double layer structure and properties, and gives rise to many non-PB effects, such as nonmonotonic dependence of the surface energy on concentration and charge inversion. The image charge effect is then studied for electrolyte solutions between two plates. For two neutral plates, we show that depletion of the salt ions by the image charge repulsion results in short-range attractive and long-range repulsive forces. If cations and anions are of different valency, the asymmetric depletion leads to the formation of an induced electrical double layer. For two charged plates, the competition between the surface charge and the image charge effect can give rise to like- charge attraction.

Then, we study the inhomogeneous screening effect near the dielectric interface due to the anisotropic and nonuniform ion distribution. We show that the double layer structure and interfacial properties is drastically affected by the inhomogeneous screening if the bulk Debye screening length is comparable or smaller than the Bjerrum length. The width of the depletion layer is characterized by the Bjerrum length, independent of the salt concentration. We predict that the negative adsorption of ions at the interface increases linearly with the salt concentration, which cannot be captured by either the bulk screening approximation or the WKB approximation. For asymmetric salt, the inhomogeneous screening enhances the charge separation in the induced double layer and significantly increases the value of the surface potential.

Finally, to account for the ion specificity, we study the self energy of a single ion across the dielectric interface. The ion is considered to be polarizable: its charge distribution can be self-adjusted to the local dielectric environment to minimize the self energy. Using intrinsic parameters of the ions, such as the valency, radius, and polarizability, we predict the specific ion effect on the interfacial affinity of halogen anions at the water/air interface, and the strong adsorption of hydrophobic ions at the water/oil interface, in agreement with experiments and atomistic simulations.

The theory developed in this work represents the most systematic theoretical technique for weak-coupling electrolytes. We expect the theory to be more useful for studying a wide range of structural and dynamic properties in physicochemical, colloidal, soft-matter and biophysical systems.

A method on theoretical simulation of chromosome breaks in cells exposed to heavy ions

Background. The aim of this study is to assess an easy and quick method on simulating chromosome breaks in cells exposed to heavy charged particles. Methods. The theoretical value of chromosome break was calculated, and the validated comparison with the experimental value by using a premature chromosome condensation technique was done. Results. A good consistence was found to be appeared between the theoretical and experimental value. Conclusions. This suggested that a higher relative biological effectiveness of heavy ions was closely correlated with its physical characteristics and besides, a safe approach on predicting chromosome breaks in cells exposed to heavy ions at off-line environment come to be considered. Furthermore, three key factors influencing the theoretical simulation was investigated and discussed.

The coulomb potential energy effect on the intensity of the characteristic lines at highly charged ion incendence on Al surface

The Al atomic characteristic spectral lines were induced by the impact of Ar-40(q+) ions (8 <= q <= 16; kinetic energy 150 keV) on Al surface. The result shows that by Penning impinging and resonant capture, the ion energy is deposited on the Al surface to excite the target atom, which is different from light excitation. Not only are the transitions betweem electronic configurations of the atomic complex excited, but the enhancing tendency of the characteristic spectral line intensity is consistent with the enhancing tendency of the coulomb potential energy of the incident ions with increasing charged states.

Correlation between initial chromatid damage and survival of various cell lines exposed to heavy charged particles

The biophysical characteristics of heavy ions make them a rational source of radiation for use in radiotherapy of malignant tumours. Prior to radiotherapy treatment, a therapeutic regimen must be precisely defined, and during this stage information on individual patient radiosensitivity would be of very great medical value. There are various methods to predict radiosensitivity, but some shortfalls are difficult to avoid. The present study investigated the induction of chromatid breaks in five different cell lines, including one normal liver cell line (L02), exposed to carbon ions accelerated by the heavy ion research facility in Lanzhou (HIRFL), using chemically induced premature chromosome condensation (PCC). Previous studies have reported the number of chromatid breaks to be linearly related to the radiation dose, but the relationship between cell survival and chromatid breaks is not clear. The major result of the present study is that cellular radiosensitivity, as measured by D-0, is linearly correlated with the frequency of chromatid breaks per Gy in these five cell lines. We propose that PCC may be applied to predict radiosensitivity of tumour cells exposed to heavy ions.

X-ray spectra induced in highly charged Ar-40(q+) interacting with Au surface

By use of optical spectrum technology, the spectra of X-ray induced by highly charged Ar-40(q+) ions interacting with Au surface have been studied. The results show that the argon K alpha X-ray were emitted from the hollow atoms formed below the surface. There is a process of multi-electron exciting in neutralization of the Ar16+ ion, with electronic configuration 1s(2) in its ground state below the solid surface. The yield of the projectile K alpha X-ray is related to its initial electronic configuration, and the yield of the target X-ray is related to the projectile kinetic energy.