Plasma-driven self-organization of Ni nanodot arrays on Si(100)

The results of the combined experimental and numerical study suggest that nonequilibrium plasma-driven self-organization leads to better size and positional uniformity of nickel nanodot arrays on a Si(100) surface compared with neutral gas-based processes under similar conditions. This phenomenon is explained by introducing the absorption zone patterns, whose areas relative to the small nanodot sizes become larger when the surface is charged. Our results suggest that strongly nonequilibrium and higher-complexity plasma systems can be used to improve ordering and size uniformity in nanodot arrays of various materials, a common and seemingly irresolvable problem in self-organized systems of small nanoparticles. © 2008 American Institute of Physics.

Deterministic nanoassembly : Neutral or plasma route?

It is shown that, owing to selective delivery of ionic and neutral building blocks directly from the ionized gas phase and via surface migration, plasma environments offer a better deal of deterministic synthesis of ordered nanoassemblies compared to thermal chemical vapor deposition. The results of hybrid Monte Carlo (gas phase) and adatom self-organization (surface) simulation suggest that higher aspect ratios and better size and pattern uniformity of carbon nanotip microemitters can be achieved via the plasma route. © 2006 American Institute of Physics.

Plasma-assisted self-sharpening of platelet-structured single-crystalline carbon nanocones

A mechanism and model for the vertical growth of platelet-structured vertically aligned single-crystalline carbon nanostructures by the formation of graphene layers on a flat top surface are proposed and verified experimentally. It is demonstrated that plasma-related effects lead to self-sharpening of tapered nanocones to form needlelike nanostructures, in a good agreement with the predicted dependence of the radius of a nanocone's flat top on the incoming ion flux and surface temperature. The growth mechanism is relevant to a broad class of nanostructures including nanotips, nanoneedles, and nanowires and can be used to improve the predictability of nanofabrication processes. © 2007 American Institute of Physics.

Uniformity of postprocessing of dense nanotube arrays by neutral and ion fluxes

The advantages of using low-temperature plasma environments for postprocessing of dense nanotube arrays are shown by means of multiscale hybrid numerical simulations. By controlling plasma-extracted ion fluxes and varying the plasma and sheath parameters, one can selectively coat, dope, or functionalize different areas on nanotube surfaces. Conditions of uniform deposition of ion fluxes over the entire nanotube surfaces are obtained for different array densities. The plasma route enables a uniform processing of lateral nanotube surfaces in very dense (with a step-to-height ratio of 1:4) arrays, impossible via the neutral gas process wherein radical penetration into the internanotube gaps is poor. © 2006 American Institute of Physics.

Control of core-shell structure and elemental composition of binary quantum dots

The possibility of initial stage control of the elemental composition and core/shell structure of binary SiC quantum dots by optimizing temporal variation of Si and C incoming fluxes and surface temperatures is shown via hybrid numerical simulations. Higher temperatures and influxes encourage the formation of a stoichiometric outer shell over a small carbon-enriched core, whereas lower temperatures result in a larger carbon-enriched core, Si-enriched undershell, and then a stoichiometric SiC outer shell. This approach is generic and is applicable to a broad range of semiconductor materials and nanofabrication techniques. © 2007 American Institute of Physics.

Plasma-controlled adatom delivery and (re)distribution: Enabling uninterrupted, low-temperature growth of ultralong vertically aligned single walled carbon nanotubes

Large-scale (∼109 atoms) numerical simulations reveal that plasma-controlled dynamic delivery and redistribution of carbon atoms between the substrate and nanotube surfaces enable the growth of ultralong single walled carbon nanotubes (SWCNTs) and explain the common experimental observation of slower growth at advanced stages. It is shown that the plasma-based processes feature up to two orders of magnitude higher growth rates than equivalent neutral-gas systems and are better suited for the SWCNT synthesis at low nanodevice friendly temperatures. © 2008 American Institute of Physics.

Hydrogen in plasma-nanofabrication : selective control of nanostructure heating and passivation

The possibility of independent control of the surface fluxes of energy and hydrogen-containing radicals, thus enabling selective control of the nanostructure heating and passivation, is demonstrated. In situ energy flux measurements reveal that even a small addition of H2 to low-pressure Ar plasmas leads to a dramatic increase in the energy deposition through H recombination on the surface. The heat release is quenched by a sequential addition of a hydrocarbon precursor while the surface passivation remains effective. Such selective control offers an effective mechanism for deterministic control of the growth shape, crystallinity, and density of nanostructures in plasma-aided nanofabrication. © 2010 American Institute of Physics.

Nanopore processing in dielectric materials and dielectric template-assisted nanoarray synthesis : using pulsed bias to enhance process throughput and precision

An effective technique to improve the precision and throughput of energetic ion condensation through dielectric nanoporous templates and reduce nanopore clogging by using finely tuned pulsed bias is proposed. Multiscale numerical simulations of ion deposition show the possibility of controlling the dynamic charge balance on the upper template's surface to minimize ion deposition on nanopore sidewalls and to deposit ions selectively on the substrate surface in contact with the pore opening. In this way, the shapes of nanodots in template-assisted nanoarray fabrication can be effectively controlled. The results are applicable to various processes involving porous dielectric nanomaterials and dense nanoarrays.

Self-organized vertically aligned single-crystal silicon nanostructures with controlled shape and aspect ratio by reactive plasma etching

The formation of vertically aligned single-crystalline silicon nanostructures via "self-organized" maskless etching in Ar+ H 2 plasmas is studied. The shape and aspect ratio can be effectively controlled by the reactive plasma composition. In the optimum parameter space, single-crystalline pyramid-like nanostructures are produced; otherwise, nanocones and nanodots are formed. This generic nanostructure formation approach does not involve any external material deposition. It is based on a concurrent sputtering, etching, hydrogen termination, and atom/radical redeposition and can be applied to other nanomaterials.

Hierarchical multilevel arrays of self-assembled gold nanoparticles : Control of resistivity-temperature dependence

The possibility to control the electric resistivity-temperature dependence of the nanosized resistive components made using hierarchical multilevel arrays of self-assembled gold nanoparticles prepared by multiple deposition/annealing is demonstrated. It is experimentally shown that the hierarchical three-level patterns, where the nanoparticles of sizes ranging from several nanometers to several tens of nanometer play a competitive roles in the electric conductivity, demonstrate sharp changes in the activation energy. These patterns can be used for the precise tuning of the resistivity-temperature behavior of nanoelectronic components.

Increased size selectivity of Si quantum dots on SiC at low substrate temperatures : an ion-assisted self-organization approach

A simple, effective, and innovative approach based on ion-assisted self-organization is proposed to synthesize size-selected Si quantum dots (QDs) on SiC substrates at low substrate temperatures. Using hybrid numerical simulations, the formation of Si QDs through a self-organization approach is investigated by taking into account two distinct cases of Si QD formation using the ionization energy approximation theory, which considers ionized in-fluxes containing Si3+ and Si1+ ions in the presence of a microscopic nonuniform electric field induced by a variable surface bias. The results show that the highest percentage of the surface coverage by 1 and 2 nm size-selected QDs was achieved using a bias of -20 V and ions in the lowest charge state, namely, Si1+ ions in a low substrate temperature range (227-327 °C). As low substrate temperatures (≤500 °C) are desirable from a technological point of view, because (i) low-temperature deposition techniques are compatible with current thin-film Si-based solar cell fabrication and (ii) high processing temperatures can frequently cause damage to other components in electronic devices and destroy the tandem structure of Si QD-based third-generation solar cells, our results are highly relevant to the development of the third-generation all-Si tandem photovoltaic solar cells.

Disentangling fluxes of energy and matter in plasma-surface interactions : effect of process parameters

The possibility to discriminate between the relative importance of the fluxes of energy and matter in plasma-surface interaction is demonstrated by the energy flux measurements in low-temperature plasmas ignited by the radio frequency discharge (power and pressure ranges 50-250 W and 8-11.5 Pa) in Ar, Ar+ H2, and Ar+ H2 + CH4 gas mixtures typically used in nanoscale synthesis and processing of silicon- and carbon-based nanostructures. It is shown that by varying the gas composition and pressure, the discharge power, and the surface bias one can effectively control the surface temperature and the matter supply rates. The experimental findings are explained in terms of the plasma-specific reactions in the plasma bulk and on the surface.

Tailoring carbon nanotips in the plasma-assisted chemical vapor deposition: Effect of the process parameters

Carbon nanotips have been synthesized from a thin carbon film deposited on silicon by bias-enhanced hot filament chemical vapor deposition under different process parameters. The results of scanning electron microscopy indicate that high-quality carbon nanotips can only be obtained under conditions when the ion flux is effectively drawn from the plasma sustained in a CH4 + NH3 + H2 gas mixture. It is shown that the morphology of the carbon nanotips can be controlled by varying the process parameters such as the applied bias, gas pressure, and the NH3 / H2 mass flow ratios. The nanotip formation process is examined through a model that accounts for surface diffusion, in addition to sputtering and deposition processes included in the existing models. This model makes it possible to explain the major difference in the morphologies of the carbon nanotips formed without and with the aid of the plasma as well as to interpret the changes of their aspect ratio caused by the variation in the ion/gas fluxes. Viable ways to optimize the plasma-based process parameters to synthesize high-quality carbon nanotips are suggested. The results are relevant to the development of advanced plasma-/ion-assisted methods of nanoscale synthesis and processing.

Analysis of photoluminescence background of Raman spectra of carbon nanotips grown by plasma-enhanced chemical vapor deposition

Carbon nanotips with different structures were synthesized by plasma-enhanced hot filament chemical vapor deposition and plasma-enhanced chemical vapor deposition using different deposition conditions, and they were investigated by scanning electron microscopy and Raman spectroscopy. The results indicate that the photoluminescence background of the Raman spectra is different for different carbon nanotips. Additionally, the Raman spectra of the carbon nanotips synthesized using nitrogen-containing gas precursors show a peak located at about 2120 cm-1 besides the common D and G peaks. The observed difference in the photoluminescence background is related to the growth mechanisms, structural properties, and surface morphology of a-C:H and a-C:H:N nanotips, in particular, the sizes of the emissive tips.

Effect of doping with Co and/or Cu on electronic structure and optical properties of ZnO

This paper reports on ab initio numerical simulations of the effect of Co and Cu dopings on the electronic structure and optical properties of ZnO, pursued to develop diluted magnetic semiconductors vitally needed for spintronic applications. The simulations are based upon the Perdew-Burke-Enzerh generalized gradient approximation on the density functional theory. It is revealed that the electrons with energies close to the Fermi level effectively transfer only between Cu and Co ions which substitute Zn atoms, and are located in the neighbor sites connected by an O ion. The simulation results are consistent with the experimental observations that addition of Cu helps achieve stable ferromagnetism of Co-doped ZnO. It is shown that simultaneous insertion of Co and Cu atoms leads to smaller energy band gap, redshift of the optical absorption edge, as well as significant changes in the reflectivity, dielectric function, refractive index, and electron energy loss function of ZnO as compared to the doping with either Co or Cu atoms. These highly unusual optical properties are explained in terms of the computed electronic structure and are promising for the development of the next-generation room-temperature ferromagnetic semiconductors for future spintronic devices on the existing semiconductor micromanufacturing platform.