Clusters of ionisation in nanometre targets for propane-experiments with a Jet Counter

Further evidence on the reliability of the device called the Jet Counter (JC) for studying the formation of ionisation clusters at the nanometre level are presented. The new experimental data on the distributions of ionisation cluster size originating from a 2-10 nm size target in propane irradiated by 3.8 MeV alpha particles are described. The JC consists of a pulse-operated valve that injects an expanding jet of propane into an interaction chamber, where a sensitive volume in the form of a cylinder is created. The sensitive volume was irradiated by 3.8 MeV alpha particles. The resulting distribution of ion clusters, ranging from 2 to 10 nm in unit density gas, has been measured. A method of determining the efficiency of registration of single propane ions using an ion detector is described. A method of deconvolution of the measured to true cluster size distributions is also given. Finally, the measured cluster size distributions are compared with modelled distributions based on Monte Carlo calculations. The results for propane together with previous ones for nitrogen indicate the JC to be an efficient tool for the investigation of radiation quality at the nanometre level.     

Ionization cluster size distribution for alpha particles: experiment, modelling

The paper presents data for measured ionization cluster size distributions by alpha particles in tissue equivalent media and comparison with the simulated data for liquid water. The experiments were carried out with a beam of 4.6 MeV alpha particles performed in a setup called the JET Counter. The theoretically derived cluster size distributions for alphas particles were obtained using the K-means algorithm. The simulation was carried out by Monte Carlo track structure calculations using cross sections for liquid water. The first moments of cluster size distributions, derived from K-means algorithm as a function of diameter of cluster centroid, were compared with the corresponding moments derived from the experiments for nitrogen and propane targets. It was found that the ratio of the first moments for water to gas targets correlates well with the corresponding ratio of the mean free paths for primary ionization by alpha particles in the two media. It is shown that the cluster size distributions for alpha particles in water, obtained from K-means algorithm, are in agreement with the corresponding distributions measured experimentally in nitrogen or propane gas targets of nanometer sizes.     

Hierarchical modeling of C and Si nano-cluster nucleation utilizing quantum and statistical mechanics

A hierarchical, multi-scale computer model for the nucleation of nano-phase materials from the vapor phase is presented. The model utilizes full solutions to quantum mechanics cluster energy equations for sizes up to 10 atoms, and statistical rate theory for larger cluster sizes. Ab initio and semi-empirical quantum mechanics methods are used to investigate the energetics of Si and C clusters. The results of binding energy and most stable configurations show significant differences between C and Si nano-clusters. Atomic cluster size distributions are obtained from reaction rate theory on the basis of collision frequencies in the vapor phase. Cluster reaction rates are determined from the energetics and vibrational modes, as investigated by quantum mechanics for small sizes. The nucleation and further evolution of the cluster size distribution is modeled by solutions to detailed kinetic equations. This multi-scale model is shown to be a useful computer simulation tool, which can be utilized to design experiments on nano-phase materials with minimum adjustable parameters. This revised version was published online in July 2006 with corrections to the Cover Date.     

Proton-induced frequency distributions of ionization cluster size in propane

The frequency distribution of clustered ionizations produced by a proton beam was measured in a nanodosimetric volume of the size of a DNA segment by means of an ion-counting nanodosimeter in the energy range from 0.4 to 3.5 MeV. In order to meet the needs of the ion-counting nanodosimeter, the accelerator's primary beam was reduced in intensity by means of Rutherford scattering. The comparison between experimental results and Monte Carlo simulations show a good agreement in the energy dependence of the mean cluster size, while the experimental cluster size distributions show a higher amount of large ionization clusters compared with those obtained with the simulations.     

Reconstruction of cluster distributions at 100% detection efficiency for a track-nanodosimetric counter through a Bayesian analysis

A Bayesian unfolding has been applied to ionisation distributions due to 5.4 MeV alpha particles in a 20-nm site obtained using Monte Carlo simulations, taking into account different detection efficiency conditions. The ideal case of a target volume with uniform efficiency has been investigated to study the dependence of the reconstruction on prior distributions. A simplified approach has been used to treat the case of a target volume with non-uniformly distributed efficiency, like the sensitive volume of the track-nanodosimetric counter. Our results point out that Bayesian analysis provides a effective tool for reconstructing the true ionisation distributions, well beyond the maximum measured cluster size.     

Experimental tools for track structure investigations: new approaches for dosimetry and microdosimetry

In recent years, several new methods have been developed for track structure investigations. They use macroscopic gas volumes to transfer the results to microscopic dimensions and are based on either the cluster counting principle or on optical methods for full track analysis. The first type of method allows cluster size distributions in nanometre dimensions to be measured. The second type reveals the full topology of the ionisation pattern of tracks or track segments within a volume of a few micrometres with a spatial resolution down to 5 nm. The basic principles of these instruments and their main features are summarised and a selection of results obtained to date are shown.     

Bayesian reconstruction of nanodosimetric cluster distributions at 100% detection efficiency

Ionisation spectra in nanometric volumes at a given distance from a charged particle track are obtained by using electron (or ion) gas detectors, having non-uniformly distributed detection efficiency. Therefore, such spectra should be properly processed in order to reconstruct the frequency distribution of clusters really produced in the detector gas. A Bayesian unfolding has been applied to ionisation distributions due to 5.4 MeV alpha particles in a 20-nm site obtained by Monte Carlo simulations, taking into account different detection efficiency conditions. It will be shown that Bayesian analysis provides a valid tool for reconstructing the true ionisation distributions, well beyond the maximum measured cluster size.     

The formation of ionisation clusters by alpha particles in 'nanometric' volumes of nitrogen: experiment and calculation

Probability distributions of the size of ion clusters created in 'nanometric' cylindrical volumes of nitrogen by single 4.6 MeV alpha particles were measured and compared with those calculated by Monte Carlo simulation. The diameter of the sensitive volume had a mass per area of between 0.015 and 1.3 micrograms.cm-2 which, for a material at unit density, corresponds to a diameter of between 0.15 nm and 13 nm. These nanometre sizes were simulated experimentally in a device called Jet Counter. The measured or calculated cluster size probabilities confirmed that the formation of ionisation clusters along a 'nanometre' track can be characterised by Poisson's distribution only for very small targets. The present ionisation cluster probabilities produced in 'nanometric' volumes, 2 to 10 nm in diameter, are the first ever determined experimentally and confirmed by Monte Carlo simulation.     

New descriptors of radiation quality based on nanodosimetry, a first approach

After a short overview on the latest developments in nanodosimetry, measured frequency distributions of ionisation cluster size caused by 4.6 MeV alpha-particles or low-energy electrons in 'nanometric' volumes of nitrogen are compared with cluster-size distributions for liquid water cylinders that are equal in size to segments of DNA of 10 base-pairs length. Such frequency distributions are, to a greater part, governed by the same basic physical interaction data as those to be expected, if charged particles interact with DNA segments. Quantities derived from ionisation cluster-size distributions should, therefore, behave as a function of radiation quality similarly to the yields of single or double strand breaks in the DNA. To test this assumption, extensive Monte Carlo simulations were performed for electrons in the energy range between 12.5 eV and 100 keV for protons at energies between 0.7 MeV and 250 MeV and for alpha-particles in the energy range between 2 MeV and 100 MeV. The results are then compared with the yields of single- or double-strand breaks in the DNA, taken from the literature.     

Grain size statistics

A method for the computation of spatial grain size distributions from intercept data based on a tetrakaidecahedron grain model is developed. The necessary inverse matrix is presented. The method is applied to a range of metallic and ceramic specimens. The derived distributions are analysed to show that they are not necessarily log-normal. Statistical techniques are applied to determine the minimum sample sizes and these are shown to increase as the distributions become more dispersed. The constant relating the average grain size to the average intercept length is also shown to be sensitive to the grain size distribution.     

Optical sizing of immunolabel clusters through multispectral plasmon coupling microscopy

The wavelength dependent scattering cross sections of self-assembled silver nanoparticle clusters of known size (n) were measured on five different wavelength channels between 427 and 510 nm through correlation of multispectral imaging and scanning electron microscopy. A multivariate statistical analysis of the spectral response of this training set provided a correlation between spectral response and cluster size and enabled a classification of new measurements into four distinct nanoparticle association levels (I1-I4) whose compositions were dominated by monomers (I1), dimers (I2), trimers and tetramers (I3), and larger clusters (I4), respectively. One potential application of the optical sizing approach is to map association levels of silver immunolabels on cellular surfaces. We demonstrate the feasibility of this approach using silver immunolabels targeted at the epidermal growth factor receptor on A431 cells in a proof of principle experiment. The ability to measure immunolabel association levels on subcellular length scales in an optical microscope provides new opportunities for experimentally assessing receptor density distributions on living cells in solution.     

Use of fractals and kinetic equations to model thermally induced hillock formation and growth in thin metal films

We investigated the applicability of a model based on fractals and the Smoluchowski kinetic equations to describe hillock formation in thin metal films. We have previously used this model to analyze cluster and ultrafine particle production. We show how to extract two parameters from measured hillock size distributions which may reveal the scaling of the mobility of clusters and vacancies in films with varying hillock size. On the basis of our application of this model to certain data taken from the literature, the model shows considerable potential for being able to provide an internally consistent quantitative basis for monitoring thermally driven mass redistribution processes in metal films.     

Sizing alpha emitting particles of aged plutonium on personal air sampler filters using CR-39 autoradiography

Methods have been developed to assess the size distribution of alpha emitting particles of reactor fuel of known composition captured on air sampler filters. The sizes of uranium oxide and plutonium oxide particles were determined using a system based on CR-39 solid-state nuclear track detectors. The CR-39 plastic was exposed to the deposited particles across a 400 microm airgap. The exposed CR-39 was chemically etched to reveal clusters of tracks radially dispersed from central points. The number and location of the tracks were determined using an optical microscope with an XY motorised table and image analysis software. The sample mounting arrangement allowed individual particles to be simultaneously viewed with their respective track cluster. The predicted diameters correlated with the actual particle diameters, as measured using the optical microscope. The efficacy of the technique was demonstrated with particles of natural uranium oxide (natUO2) of known size, ranging from 4 to 150 microm in diameter. Two personal air sampler (PAS) filters contaminated with actinide particles were placed against CR-39 and estimated to have size distributions of 0.8 and 1.0 microm activity median aerodynamic diameter (AMAD).     

Experimental equivalent cluster-size distributions in nanometric volumes of liquid water

Ionisation cluster-size distributions in nanometric volumes of liquid water were determined for alpha particles at 4.6 and 5.4 MeV by measuring cluster-size frequencies in small gaseous volumes of nitrogen or propane at low gas pressure as well as by applying a suitable scaling procedure. This scaling procedure was based on the mean free ionisation lengths of alpha particles in water and in the gases measured. For validation, the measurements of cluster sizes in gaseous volumes and the cluster-size formation in volumes of liquid water of equivalent size were simulated by Monte Carlo methods. The experimental water-equivalent cluster-size distributions in nitrogen and propane are compared with those in liquid water and show that cluster-size formation by alpha particles in nitrogen or propane can directly be related to those in liquid water.     

Iterative inversion of phase-Doppler-anemometry size distributions from sprays of optically inhomogeneous liquids

Using phase Doppler anemometry (PDA) to investigate sprays of optically inhomogeneous liquids leads to blurred measured size distributions. The blurring function is formed by performance of PDA measurements on single-size droplets generated by a piezoelectric droplet generator. To obtain the undistorted droplet-size distributions, a constrained iterative inversion algorithm is applied. The number of iteration steps to achieve the best possible restoration is determined by the use of synthetically generated data that has noise properties similar to the measured histograms. The obtained size distributions are checked by comparison with undistorted measurement results of an atomized optical homogeneous liquid.     

Equilibrium structures and shapes of clusters on metal fcc(111) surfaces

Using embedded-atom-method potentials, the lower-energy structures (LESs) of adatom clusters are obtained directly on a series of metal fcc(111) surfaces by the method based on the genetic algorithm. The structural features, energy distributions, number of LESs and their differences on different surfaces are discussed and explained in terms of the nearest-neighbor and next-nearest-neighbor (NN, NNN) adatom-adatom interactions, and the edge-type difference. When the energetic preference for one edge type over another is slight, e.g., on Ag(111), only one type of structure is included, and it does not change with the increment of cluster size. However, when there is a strong energetic preference for one of the edge types, e.g., on Pt(111), an interesting phenomenon of structure replacement is revealed, by which the structures in the LES group deviate more and more from the configuration with the maximum number of NN bonds as the cluster size increases. The structure replacement also finally leads to the shape of the two-dimensional island on Pt(111) being quite distinct from that on Ag(111). Based on these results, the general trend of the variation of lower-energy structures with cluster size is discussed further for other metal fcc(111) surfaces.     

Sizing nanoparticles by time-of-flight spectrometry

Time-of-flight (TOF) spectrometry utilizing scattered light detection of particles passing discrete detection locations in an accelerating gas jet is used for rapid measurement of highly-resolved size distributions of dry powder, gas- or liquid-borne particles having diameter > 300 nm. Extension of the measurement range of this technique to include nanoparticles (< 100 nm diameter) is investigated using a theoretical model to predict the reduction in minimum, scattered-light-detectable, particle size, a limit which restricts present TOF instruments to particles above 300 nm diameter. A single set of preliminary measured data are compared with the theoretical-model predictions. Together, these results indicate that a TOF spectrometer can provide rapid, highly-resolved particle size distribution measurement of nanoparticle powders and suspensions down to ≈ 50 nm diameter.     

Life Test Sampling Plans for Normal and Lognormal Distributions

Sampling plans for truncated life tests from the normal and lognormal distributions are obtained. The tables of this paper give the minimum sample size necessary to assure a certain mean or median life when the experiment time is tied in advance. The modification necessary to assure any other quantile (percentile) of the distributions is obtained. Thus, sampling plans for establishing other percentiles of the distributions are shown to be obtainable from the tables of this paper. The operating characteristic functions of these plans are obtained and for a wide range of values of practical interest these functions are graphed in order to facilitate selection of an appropriate plan in a given situation. Producer's risk is discussed and a table is given for the ratio of the true median life to the specified median life (or the difference between the true mean lie and the specified mean life) to insure that the producer's risk does not exceed α = .l0, .05. An approximation is given for the minimum sample size. The use of tables and graphs is illustrated by examples.     

Nanostructuring of InP surface by low-energy ion beam irradiation

The InP nanodots of size 55 to 100 nm and height 25 to 30 nm have been synthesized by low-energy Ar+-ion irradiation with different ion energies. Sizes and size distributions of the dots strongly depend on growth conditions. Rapid thermal annealed (RTA) of the patterned surface shows cluster formation for annealing temperature 400 degrees C and above. Raman investigations reveal optical phonon softening due to correlation length shortening and broadening of the optical modes from the patterned surface. The softening is due to confinement of phonons in embedded nanocrystallites within the patterned surface along with surface nanodots, and broadening is attributed to their size distributions, which increases with increase in ion energy. The lattice damage recovery is observed from the patterned surface subjected to RTA, which exhibits upward shift of the LO and TO phonons due to the presence of complex interfacial stress, associated with the removal of crystal defects with RTA.