Self-organized quantum dot arrays : kinetic mapping of adatom capture

Deterministic synthesis of self-organized quantum dot arrays for renewable energy, biomedical, and optoelectronic applications requires control over adatom capture zones, which are presently mapped using unphysical geometric tessellation. In contrast, the proposed kinetic mapping is based on simulated two-dimensional adatom fluxes in the array and includes the effects of nucleation, dissolution, coalescence, and process parameters such as surface temperature and deposition rate. This approach is generic and can be used to control the nanoarray development in various practical applications. © 2009 American Institute of Physics.

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.

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.

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.

Silicon on silicon : self-organized nanotip arrays formed in reactive Ar+H2 plasmas

The formation of arrays of vertically aligned nanotips on a moderately heated (up to 500 degrees C) Si surface exposed to reactive low-temperature radio frequency (RF) Ar+H(2) plasmas is studied. It is demonstrated that the nanotip surface density, aspect ratio and height dispersion strongly depend on the substrate temperature, discharge power, and gas composition. It is shown that nanotips with aspect ratios from 2.0 to 4.0 can only be produced at a higher RF power density (41.7 mW cm(-3)) and a hydrogen content of about 60%, and that larger aspect ratios can be achieved at substrate temperatures of about 300 degrees C. The use of higher (up to 500 degrees C) temperatures leads to a decrease of the aspect ratio but promotes the formation of more uniform arrays with the height dispersion decreasing to 1.5. At lower (approximately 20 mW cm(-3)) RF power density, only semispherical nanodots can be produced. Based on these experimental results, a nanotip formation scenario is proposed suggesting that sputtering, etching, hydrogen termination, and atom/radical re-deposition are the main concurrent mechanisms for the nanostructure formation. Numerical calculations of the ion flux distribution and hydrogen termination profiles can be used to predict the nanotip shapes and are in a good agreement with the experimental results. This approach can be applied to describe the kinetics of low-temperature formation of other nanoscale materials by plasma treatment.

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.

The production of self-organized carbon connections between Ag nanoparticles using atmospheric microplasma synthesis

The formation of long self-organized carbon connections (where the length is much greater than the diameter) between Ag nanoparticles on a Si(1 0 0) surface in atmospheric pressure Ar + CH4 microplasmas is demonstrated. A growth scenario explaining the connection nucleation and growth is proposed, and this is supported by numerical simulations which reveal that the electric field pattern around the growing connections affects the surface diffusion of carbon adatoms, the main driving force for the observed self-organization. Results suggest that the microplasma-generated surface charges can be used as effective controls for the self-organized formation of complex carbon-based nano-networks for integrated nanodevices.

Self-organized carbon connections between catalyst particles on a silicon surface exposed to atmospheric-pressure Ar + CH4 microplasmas

Ag nanoparticles and Fe-coated Si micrograins were separately deposited onto Si(1 0 0) surfaces and then exposed to an Ar + CH4 microplasma at atmospheric pressure. For the Ag nanoparticles, self-organized carbon nanowires, up to 400 nm in length were produced, whereas for the Fe-coated Si micrograins carbon connections with the length up to 100 μm were synthesized on the plasma-exposed surface area of about 0.5 mm2. The experiment has revealed that long carbon connections and short nanowires demonstrate quite similar behavior and structure. While most connections/nanowires tended to link the nearest particles, some wires were found to 'dissolve' into the substrate without terminating at the second particle. Both connections and nanowires are mostly linear, but long carbon connections can form kinks which were not observed in the carbon nanowire networks. A growth scenario explaining the carbon structure nucleation and growth is proposed. Multiscale numerical simulations reveal that the electric field pattern around the growing connections/nanowires strongly affects the surface diffusion of carbon adatoms, the main driving force for the observed self-organization in the system. The results suggest that the microplasma-generated surface charges can be used as effective controls for the self-organized formation of complex carbon-based nano-networks for integrated nanodevices.

Plasma-assisted self-organized growth of uniform carbon nanocone arrays

The self-organized growth of uniform carbon nanocone arrays using low-temperature non-equilibrium Ar + H 2 + CH 4 plasma-enhanced chemical vapor deposition (PECVD) is studied. The experiment shows that size-, shape-, and position-uniform carbon nanocone arrays can develop even from non-uniformly fragmented discontinuous nickel catalyst films. A three-stage scenario is proposed where the primary nanocones grow on large catalyst particles during the first stage, and the secondary nanocones are formed between the primary ones at the second stage. Finally, plasma-related effects lead to preferential growth of the secondary nanocones and eventually a uniform nanopattern is formed. This does not happen in a CVD process with the same gas feedstock and surface temperature. The proposed three-stage growth scenario is supported by the numerical experiment which generates nanocone arrays very similar to the experimentally synthesized nanopatterns. The self-organization process is explained in terms of re-distribution of surface and volumetric fluxes of plasma-generated species in a developing nanocone array. Our results suggest that plasma-related self-organization effects can significantly reduce the non-uniformity of carbon nanostructure arrays which commonly arises from imperfections in fragmented Ni-based catalyst films.

Simulation and visualization of self-assembled nanodevice networks synthesized via plasma–surface interaction

Using advanced visualization techniques, a comprehensive visualization of all the stages of the self-organized growth of internetworked nanostructures on plasma-exposed surface has been made. Atomistic kinetic Monte Carlo simulation for the initial stage of deposition, with 3-D visualization of the whole system and half-tone visualization of the density field of the adsorbed atoms, makes it possible to implement a multiscale predictive modeling of the development of the nanoscale system.

The path to stoichiometric composition of III–V binary quantum dots through plasma/ion-assisted self-assembly

Semiconductor III-V quantum dots (QDs) are particularly enticing components for the integration of optically promising III-V materials with the silicon technology prevalent in the microelectronics industry. However, defects due to deviations from a stoichiometric composition [group III: group V = 1] may lead to impaired device performance. This paper investigates the initial stages of formation of InSb and GaAs QDs on Si(1 0 0) through hybrid numerical simulations. Three situations are considered: a neutral gas environment (NG), and two ionized gas environments, namely a localized ion source (LIS) and a background plasma (BP) case. It is shown that when the growth is conducted in an ionized gas environment, a stoichiometric composition may be obtained earlier in the QD as compared to a NG. Moreover, the stoichiometrization time, tst, is shorter for the BP case compared to the LIS scenario. A discussion of the effect of ion/plasma-based tools as well as a range of process conditions on the final island size distribution is also included. Our results suggest a way to obtain a deterministic level of control over nanostructure properties (in particular, elemental composition and size) during the initial stages of growth which is a crucial step towards achieving highly tailored QDs suitable for implementation in advanced technological devices.

Effect of elemental composition and size on electron confinement in self-assembled SiC quantum dots : a combinatorial approach

A high level of control over quantum dot (QD) properties such as size and composition during fabrication is required to precisely tune the eventual electronic properties of the QD. Nanoscale synthesis efforts and theoretical studies of electronic properties are traditionally treated quite separately. In this paper, a combinatorial approach has been taken to relate the process synthesis parameters and the electron confinement properties of the QDs. First, hybrid numerical calculations with different influx parameters for Si1-x Cx QDs were carried out to simulate the changes in carbon content x and size. Second, the ionization energy theory was applied to understand the electronic properties of Si1-x Cx QDs. Third, stoichiometric (x=0.5) silicon carbide QDs were grown by means of inductively coupled plasma-assisted rf magnetron sputtering. Finally, the effect of QD size and elemental composition were then incorporated in the ionization energy theory to explain the evolution of the Si1-x Cx photoluminescence spectra. These results are important for the development of deterministic synthesis approaches of self-assembled nanoscale quantum confinement structures.

Deterministic control of plasma-assembled self-organized Ge/Si quantum dot arrays

Self-assembly of size-uniform and spatially ordered quantum dot (QD) arrays is one of the major challenges in the development of the new generation of semiconducting nanoelectronic and photonic devices. Assembly of Ge QD (in the ∼5-20 nm size range) arrays from randomly generated position and size-nonuniform nanodot patterns on plasma-exposed Si (100) surfaces is studied using hybrid multiscale numerical simulations. It is shown, by properly manipulating the incoming ion/neutral flux from the plasma and the surface temperature, the uniformity of the nanodot size within the array can be improved by 34%-53%, with the best improvement achieved at low surface temperatures and high external incoming fluxes, which are intrinsic to plasma-aided processes. Using a plasma-based process also leads to an improvement (∼22% at 700 K surface temperature and 0.1 MLs incoming flux from the plasma) of the spatial order of a randomly sampled nanodot ensemble, which self-organizes to position the dots equidistantly to their neighbors within the array. Remarkable improvements in QD ordering and size uniformity can be achieved at high growth rates (a few nms) and a surface temperature as low as 600 K, which broadens the range of suitable substrates to temperature-sensitive ultrathin nanofilms and polymers. The results of this study are generic, can also be applied to nonplasma-based techniques, and as such contributes to the development of deterministic strategies of nanoassembly of self-ordered arrays of size-uniform QDs, in the size range where nanodot ordering cannot be achieved by presently available pattern delineation techniques.

Tailoring the composition of self-assembled Si1−xCx quantum dots : simulation of plasma/ion-related controls

Precise control of composition and internal structure is essential for a variety of novel technological applications which require highly tailored binary quantum dots (QDs) with predictable optoelectronic and mechanical properties. The delicate balancing act between incoming flux and substrate temperature required for the growth of compositionally graded (Si1-xC x; x varies throughout the internal structure), core-multishell (discrete shells of Si and C or combinations thereof) and selected composition (x set) QDs on low-temperature plasma/ion-flux-exposed Si(100) surfaces is investigated via a hybrid numerical simulation. Incident Si and C ions lead to localized substrate heating and a reduction in surface diffusion activation energy. It is shown that by incorporating ions in the influx, a steady-state composition is reached more quickly (for selected composition QDs) and the composition gradient of a Si1-xCx QD may be fine tuned; additionally (with other deposition conditions remaining the same), larger QDs are obtained on average. It is suggested that ionizing a portion of the influx is another way to control the average size of the QDs, and ultimately, their internal structure. Advantages that can be gained by utilizing plasma/ion-related controls to facilitate the growth of highly tailored, compositionally controlled quantum dots are discussed as well.