Cluster model of aluminum dense vapor plasma

The chemical model of aluminum vapor plasma, that take into account the formation of neutral and charged clusters, is suggested. Caloric and thermal equations of state and composition of plasma were received using the available information about properties of metal clusters. It is shown, that aluminum vapors are clusterized with decrease of temperature and with increase of density. Pressure dependence on internal energy is calculated and comparison with experimental data is made. The important role of aluminum clusters, especially in an initial phase of the metals vapor heating, is demonstrated. It is shown, that the region of plasma clusterization in gaseous phase agree with known literature data for binodal of vapor-liquid transition from gaseous region. Suggested cluster model may be used to forecast the location of metal vapors binodal. The conductivity of aluminum vapor plasma was calculated. The satisfactory agreement with available experimental data is received.     

Oscillatory regimes of vapor condensation

The problem of the condensation of supersaturated vapor in an open system at a constant rate of production of a monomer and a continuous flow of a carrier gas that removes the products of condensation from the system is considered. It is shown both analytically and by numerical experiment that with a decreasing rate of the carrier gas to below a critical magnitude, the condensation regime becomes oscillatory; namely, time oscillations of the cluster-size distribution in the vapor to be condensed are set in. The cause of the phenomenon is in the suppression of the rate of nucleation and the presence of large clusters.     

Homogeneous nucleation and growth in iron-platinum vapour investigated by molecular dynamics simulation

Homogeneous nucleation and growth from binary metal vapour is investigated by molecular dynamics simulation. It is focused here mainly on the iron-platinum system with a mole fraction of 0.5. The simulations are started in the highly supersaturated vapour phase. Argon is added as carrier gas removing the heat of condensation from the forming clusters. The embedded atom method is employed for modelling of the force field of iron and platinum. The simulation runs are evaluated with respect to the nucleation rate, monomer temperature, monomer amount, and with respect to the size of the largest cluster in the system including possible pure metal clusters. It turns out that depending on the composition of the complete system pure platinum clusters with sizes up to 10 to 15 atoms are formed in addition to binary clusters. Due to the high temperature of these clusters iron atoms less likely condense at the beginning of the particle formation simulation. This leads to temporary difference in the temperatures of the platinum and the iron subsystems, which eventually approach each other when only binary clusters are present. In summary, the results obtained from the cluster statistics show that pure platinum nucleation and growth can take place to some extent within the binary system.     

Morphology evolution of Si nanowires synthesized by gas condensation of SiO without any catalyst

A series of Si nanowires are synthesized at constant temperature of 970 ^○C on Si substrate by gas condensation of pure SiO vapor without any metal catalysts, by controlling the coverage of SiO_x deposits. The morphologies are characterized by scan electron microscopy (SEM) and their evolution during the growth process is observed: from isolated clusters in earlier stage to linked cluster assemblies, and developing to smooth nanowires in the later stage. The growth mechanism is discussed based on the newly proposed clustering-aggregation-sintering model.     

On the mechanism of carbon nanotube formation: II. The kinetics of explosive condensation of carbon molten drops in a metallic catalyst

The preliminary stage of the formation of carbon nanotubes by the vapor-liquid-drop mechanism is considered as applied to the condensation of drops from carbon and metal vapors. The problem of the condensation of molten drops is solved for a wide concentration range for both vapors at a condensation temperature. It is shown that, at very high concentrations of the metal vapor (10¹⁸–10¹⁹ cm⁻³) and high temperatures (about 0.3 eV), peculiar heterogeneous condensation of the drops can occur at huge supersaturation of the carbon vapor and the saturated metal vapor. This problem of the condensation of the binary vapor is of methodical interest. This condensation is shown to be unrealizable in real experiment at the parameters of the carbon and metal vapors; it virtually merges with the homogeneous condensation of the metal vapor. The maximum concentration of the carbon vapor below which carbon condenses into drops and above which carbon condenses into amorphous soot particles is calculated. The calculation makes it possible to propose a new approach to the controlled growth of carbon nanotubes.     

Water condensation kinetics on a hydrophobic surface

Employing thermal desorption spectroscopy, we show that the effective probability of water condensation at low water vapor pressure on an octane film is much below unity at 100-120 K. This unusual finding is related to a small binding energy of H2O monomers on octane (approximately equal to 0.08 eV), requiring the formation of critical water clusters for condensation to occur. This results in strong temperature and impingement-rate dependencies of the water condensation rate and a nonlinear uptake as a function of dose time. All these features are rationalized quantitatively by a kinetic model of water condensation.     

Effect of temperature on structural transformations of nickel nanoclusters

The gas-phase condensation of nickel nanoclusters is simulated by the molecular dynamics method with the use of tight-binding potentials. It is revealed that subsequent heating of the synthesized clusters to temperatures of 400–500 K leads to a substantial improvement of their internal structure with a hexagonal close-packed phase predominating. Upon heating of the nanoparticles above the melting point and subsequent gradual cooling, the formation of a cluster structure depends strongly on the cooling rate. The inference is made that heating of the nanoclusters synthesized from a gas phase can be used for the controlled formation of nickel nanoparticles with a predicted structure.     

Atom deposition on surface clusters: thin film growth on Pd(111)

We have studied the vapor phase deposition of single metal atoms on two-dimensional clusters at the Pd(111) surface. The system considered here are heptamers and dodecamers for the substrate temperature of 100 K. Using molecular dynamics simulations with the corrected effective medium potentials for Pd, Cu and Rh, we have found that an adatom either diffuses on the cluster or incorporates itself into the cluster depending on the size of clusters and the kind of metals in the gas/cluster system. We also discovered that incorporation of a deposited gas atom into a surface cluster at 100 K was not a consequence of the reduction of the barrier heights at the step edges and that the type of post-impact dynamics for hexagonal heptamers depends on the impact point.     

On energy transfer and generation of an electric current in the vicinity of an electrode dipped in an electrolyte and strongly heated by a current passing through it

Processes occurring when a metal electrode dipped in an electrolyte is heated by intense evaporation of the electrolyte are considered in terms of a physically rigorous model. Based on the Onsager principle of least energy dissipation rate in nonequilibrium processes, the fractions of thermal energy that are spent on heating and evaporating the electrolyte and on heating the vapor are found. The energy is released within the vapor-gas sheath when an electric current flows between the electrode and electrolyte surface. It is found that the electrolyte vapor temperature exceeds 1300 K. Analytical expressions are derived for the vapor-gas sheath thickness, the electrolyte vapor pressure, and the velocity of the vapor escaping the discharge zone. It is shown that field evaporation of thermally activated negative ions from the electrolyte surface cannot provide an electric current with densities found in experiments but is responsible for the generation of free electrons near the electrolyte surface. These electrons arise when the ions decay via collisions with excited molecules.     

Synthesis of Cu nanoparticles by condensation from the gas phase

A series of computer experiments was conducted by the raw material evaporation and subsequent condensation to determine the most efficient regimes of copper nanoparticles synthesis. By variation of the cooling rate of the metal vapor the formation of Cu clusters were studied. The computer experiments showed the influence of different final temperatures on the shape of the resultant particles. This allowed to determine the conditions for a predominant formation of worm-like clusters of a spherical shape in the gas phase synthesis.     

Simulation on the Effect of Brownian Motion on Nanoparticle Trajectories in a Pulsed Microplasma Cluster Source

We describe a simulation of the nanoparticle trajectories in a pulsed cluster beam source. Clusters, formed by condensation of atomic vapor in a helium bath, and considered here as rigid spheres having a diameter of 1.5nm, were tracked during their travel inside the source cavity, an aerodynamic lens, and a cylindrical nozzle. Steady state supersonic laminar flow of helium is considered in an axi-symmetric geometry aiming to simulate, within some limitations, the conditions under which cluster formation takes place in a pulsed microplasma cluster source. In spite of the unsteady nature of the pulsed source, the time scale characterizing particle motion in the flow field is significantly smaller than the characteristic time constant for the evolution of gas pressure in the source. For this reason, a steady simulation can shed some light on the understanding of processes governing nanoparticle motion in a pulsed vaporization source. The extent to which the Brownian diffusion can affect the particle extraction from the source is investigated. Simulations have shown that the Brownian motion perturbs the clusters from the trajectories dictated by the carrier gas and increases the rate of cluster deposition on the source internal walls. However, it does not hinder the aerodynamic focalization produced by the lens even in nano-size cluster regime. This result is qualitatively confirmed by experiment.     

Thermodynamics of supersaturated vapor nucleation on molecular condensation nuclei

A key problem in the theory of a supersaturated vapor nucleation on molecular condensation nuclei (namely, the work of formation and the equilibrium concentrations of clusters) is considered. To calculate these quantities using the structural models of clusters, which are better suited for this purpose than the classical droplet model, we derive the equation connecting the work of transfer of a molecular condensation nucleus from the gas phase to a homogeneous cluster with a change in the number of contacts between molecules, occurring in the course of this transfer, and with the work of rupture of individual contacts.     

The effect of dissociation energies on thin film nucleation kinetics

Dissociation energies of small clusters have for the first time been incorporated into a set of rate equations to calculate nucleation rate, cluster density and condensation coefficients for thin film nucleation. Without considering dimers and larger clusters to be mobile, good quantitative agreement was obtained between the theoretical predictions described in this paper and the experimental results of Velfe et al. for Au deposition on NaCl [Thin Solid Films 98 (1982) 115]. The major findings of this study are: (1) the Au dimer dissociation energy is much smaller than has previously been assumed and (2) steady state with equilibrium monomer density is generally not a valid assumption for condensation on a defect-free substrate. It is also found that current use of rate equations violates the mass balance law.     

超声喷流氩氢混合团簇特性研究

利用瑞利散射方法研究了超声喷流Ar-CH4混合团簇和超声喷流Ar-H2混合团簇的特性.通过测量不同混合比例和不同背压下所形成混合团簇的散射信号发现,当用Ar气和CH4的混合气体进行超声喷流时很容易形成Ar-CH4混合团簇,当Ar气含量为50%时混合团簇尺度最大且大于相同气压下纯Ar团簇尺度和纯CH4团簇尺度.实验发现,与纯H2团簇只能在低温条件下获得不同,常温下即可形成Ar-H2混合团簇,实现了常温下含氢团簇的获取,从而有效降低了制备成本.在H2含量大于40%时混合团簇开始形成并在60%时达到最大尺度.含氢(氘)混合团簇在氢(氘)团簇的基础上引入了更重的异核Ar元素,在激光氘团簇聚变实验中它将进一步加速氘离子从而获得更高的能量,并具有更高的中子产额和聚变效率.     

On diffusion mixing of vapor and gas

A self-similar solution is obtained for a one-dimensional problem of diffusion mixing of vapor and gas, which is followed by condensation process. Two limiting cases of mixing are considered: in the first one, the vapor and gas occupy in their initial states the volumes of semi-infinite extension, in the second case, the vapor has a semi-infinite extension, and constant values of temperature and gas concentration are maintained at its boundary. The peculiarities of the temperature and concentration fields are analysed versus the vapor and gas temperatures, and the temperature values are found, at which the mixing occurs with the condensate formation.     

Mechanisms of small clusters production by short and ultra-short laser ablation

The mechanisms involved into the formation of clusters by pulsed laser ablation are studied both numerically and experimentally. To facilitate the model validation by comparison with experimental results, the time and length scales of the simulation are considerably increased. This increase is achieved by using a combination of molecular dynamics (MD) and the direct simulation Monte Carlo (DSMC) methods. The combined MD-DSMC model is then used to compare the relative contribution of the two channels of the cluster production by laser ablation: (i) direct cluster ejection upon the laser-material interaction, and (ii) collisional sticking and aggregation in the ablated gas flow. Calculation results demonstrate that both of these mechanisms play a role. The initial cluster ejection provides cluster precursors thus eliminating the three-body collision bottleneck in the cluster growth process. The presence of clusters thus facilitates the following collisional condensation and evaporation processes. The rates of these processes become considerable, leading to the modification of not only the plume cluster composition, but also the dynamics of the plume expansion. Calculation results explain several recent experimental findings.     

Silicon-riched-oxide cluster assembled nanostructures formed by low energy cluster beam deposition

Free beam of silicon oxide nanoclusters is produced by a gas aggregation source from SiO precursor. Due to the disproportionation reaction during the condensation of SiO vapor the generated clusters are Si-riched. The clusters are collimated to be a fine beam and deposited on the substrate at room temperature. The microstructures of the cluster-based nanofilm are characterized by TEM. It is shown that with appropriate impacting parameters, Si-riched oxide nanofilms assembled from uniformly distributed isolated clusters can be obtained. And the clusters can self-organize into partially densely ordered packing within local domains. XPS spectra are taken to analyze the chemical components of the nanofilms. Photoluminescence from the Si-riched oxide nanofilms has also been observed.