Changing planar thin film growth into self-assembled island formation by adjusting experimental conditions

Illustrated in this paper are two examples of altering planar growth into self-assembled island formation by adapting experimental conditions. Partial oxidation, undersaturated solution and high temperature change Frank-Van der Merwe (FM) growth of Al0.3Ga0.7As in liquid phase epitaxy (LPE) into isolated island deposition. Low growth speed, high temperature and in situ annealing in molecular beam epitaxy (MBE) cause the origination of InAs/GaAs quantum dots (QDs) to happen while the film is still below critical thickness in Stranski-Krastanow (SK) mode. Sample morphologies are characterized by scanning electron microscopy (SEM) or atomic force microscopy (AFM). It is suggested that such achievements are of value not only to fundamental researches but also to spheres of device applications as well. (c) 2004 Elsevier B.V. All rights reserved.

Size quantization effects in InAs self-assembled islands on InP(001) at the onset of 2D-to-3D transition

Photoluminescence spectroscopy has been used to investigate self-assembled InAs islands in InAlAs grown on InP(0 0 1) by molecular beam epitaxy, in correlation with transmission electron microscopy. The nominal deposition of 3.6 monolayers of InAs at 470 degrees C achieves the onset stage of coherent island formation. In addition to one strong emission around 0.74 eV, the sample displaces several emission peaks at 0.87, 0.92. 0.98, and 1.04 eV. Fully developed islands that coexist with semi-finished disk islands account for the multipeak emission. These results provide strong evidence of size quantization effects in InAs islands. (C) 1999 Elsevier Science B.V. All rights reserved.

Effects of growth interruption on self-assembled InAs/GaAs islands

The effect of growth interruption on the InAs deposition and its subsequent growth as self-assembled island structures, in particular the material transport process of the InAs layers has been investigated by photoluminescence and transmission electron microscopy measurements. InAs material in structures with only coherent islands transfers from the wetting layer to the formed islands and the growth interruption causes a red shift of PL peak energy. On the other hand, the PL peak shifts to higher energy in structures containing simultaneously coherent and noncoherent islands with dislocations. In this case, the noncoherent islands capture InAs material from the surrounding wetting layer as well as coherent islands, which casues a reduction in the size of these islands. The variations in the PL intensity and line width are also discussed. (C) 1998 Elsevier Science B.V. All rights reserved.

Distinct two dimensional lateral ordering of self-assembled quantum dots

We report a quantum dot (QD) ensemble structure in which the in-plane arrangements of the dots are in a hexagonal way while the dots are also vertically aligned. Such a distinct lateral ordering of QDs is achieved on a planar GaAs(l 0 0) rather than on a prepatterned substrate by strain-mediated multilayer vertical stacking of the QDs. The analysis indicates that the strain energy of the lateral island-island interaction is minimum for arrangement of the hexagonal ordering. The ordered dots demonstrate strong photoluminescence (PL) emission at room temperature (RT) and the full width at half maximum of PL peak at RT is only 50 meV. (C) 2007 Elsevier B.V. All rights reserved.

Structural and optical properties of self-assembled InAs/GaAs quantum dots covered by InxGa1-xAs (0 <= x <= 0.3)

Optical and structural investigations of InAs quantum dots (QDs) covered by InxGa1-xAs (0 less than or equal to x less than or equal to 0.3) overgrowth layer have been systematically reported. The decrease of strain in the growth direction of InAs quantum dots covered by InGaAs layer instead of GaAs is demonstrated by transmission electron microscopy experiments. In addition, the atomic force microscopy measurement shows that the surface of InAs islands with 3-nm-thick In0.2Ga0.8As becomes flatter. However, the InGaAs islands nucleate on the top of quantum dots during the process of InAs islands covered with In0.3Ga0.7As. The significant redshift of the photoluminescence peak energy and reduction of photoluminescence linewidth of InAs quantum dots covered by InGaAs are observed. The energy gap change of InAs QDs covered by InGaAs could be explained in terms of reducing strain, suppressing compositional mixing, and increasing island height. (C) 2000 American Institute of Physics. [S0021-8979(00)04018-4].

Effect of In-mole-fraction in InGaAs overgrowth layer on self-assembled InAs/GaAs quantum dots

We have studied the optical and structural properties of InAs/GaAs QDs covered by InxGa1-xAs (0 less than or equal to x less than or equal to 0.3) layer using transmission electron microscopy, photoluminescence (PL) spectra and atomic force microscopy. We find that the strain reduces in the growth direction of InAs islands covered by InGaAs instead of GaAs layer. Significant redshift of PL peak energy and narrowing of PL linewidth are observed for the InAs QDs covered by 3 nm thick InGaAs layer. In addition, atomic force microscopy measurements indicate that the InGaAs islands will nucleate on top of InAs quantum dots, when 3 nm In0.3Ga0.7As overgrowth layer is deposited. This result can well explain the PL intensify degradation and linewidth increment of quantum dots with a higher In-mole-fraction InGaAs layer. The energy gap change of InAs QDs covered by InGaAs may be explained in terms of reducing strain, suppressing compositional mixing and increasing island height. (C) 2000 Elsevier Science B.V. All rights reserved.

Surface-enhanced Raman scattering of 4-aminothiophenol self-assembled monolayers in sandwich structure with nanoparticle shape dependence: Off-surface plasmon resonance condition

A universal metal-molecule-metal sandwich architecture by the self-assembly of Ag nanoparticles (NPs) and Au NPs of various shapes interconnected with 4-aminothiophenol (4-ATP) molecules was presented. These Ag NPs/4-ATP/Au NPs sandwich structures were characterized by surface enhanced Raman scattering (SERS) using an off-surface plasmon resonance condition. Enhancement factors (EF) on the order of 10(8) for 9b(b(2)) vibration mode were observed for the 4-ATP self-assembled monolayers (SAMs) in such sandwich structures. The factors are 2 orders of magnitude larger than that on the monolayer of Au NPs of various shapes under similar condition. More importantly, remarkable increase in the intensity of b(2) vibrational modes, which is characteristic of the charge transfer (CT) behavior between metal NPs and 4-ATP molecules, was observed in these sandwich structures under 1064 nm excitation. The obtained EF on these sandwich structure for 9b(b(2)) is larger than that for 7a vibration mode by a factor of similar to 10(2), demonstrating the importance of the contribution of the CT mechanism and the CT behavior of metal contacts, which play a significant role in metal-molecule-metal nanosystems.

Microelectrode array in mixed alkanethiol self-assembled monolayers: Electrochemical studies

We report an efficient alternative to obtain recessed microelectrodes device on gold electrode surface, in which mixed self-assembled monolayer of long and short carbon alkanethiol chains was used for this purpose. Development of the modified electrodes included the chemical adsorption of 11-mercaptoundecanoic acid and 2-mercaptoethanol solution, as well as their mixtures, on gold surface, resulting in the final mixed self-assembled monolayer configuration. For comparison, the electrochemical performance of self-assembled monolayer of 11-mercaptoundecanoic acid. 3-mercaptopropionic acid, 4-mercapto-1-butanol and 6-mercapto-1-hexanol modified electrodes was also investigated. It was verified that, in the mixed self-assembled monolayer, the 11-mercaptoundecanoic acid acts as a barrier for electron transfer while the short alkanethiol chair is deposited in an island-like shape through which electrons can be freely transferred to ions in solution, allowing electrochemical reactions to occur. The performance of the modified electrodes toward microelectrode behavior was investigated via cyclic voltammetry and electrochemical impedance spectroscopy measurements using [Fe(CN)(6)](3-/4-) redox couple as a probe. In this case, sigmoidal voltammetric responses were obtained, very similar to those observed for microelectrodes. Such behavior reinforces the proposition of electron transfer through the short alkanethiol chain layer and surface blockage by the long chain one. Electrochemical impedance results allowed calculated the mean radius value of each microelectrode disks of 3.8 mu m with about 22 mu m interval between them. The microelectrode environment provided by the mixed self-assembled monolayer can be conveniently used to provide an efficient catalytic conversion in biosensing applications. (C) 2012 Elsevier Ltd. All rights reserved.

Towards a controlled growth of self-assembled nanostructures: shaping, ordering and localization in Ge/Si heteroepitaxy.

The strain-induced self-assembly of suitable semiconductor pairs is an attractive natural route to nanofabrication. To bring to fruition their full potential for actual applications, individual nanostructures need to be combined into ordered patterns in which the location of each single unit is coupled with others and the surrounding environment. Within the Ge/Si model system, we analyze a number of examples of bottom-up strategies in which the shape, positioning, and actual growth mode of epitaxial nanostructures are tailored by manipulating the intrinsic physical processes of heteroepitaxy. The possibility of controlling elastic interactions and, hence, the configuration of self-assembled quantum dots by modulating surface orientation with the miscut angle is discussed. We focus on the use of atomic steps and step bunching as natural templates for nanodot clustering. Then, we consider several different patterning techniques which allow one to harness the natural self-organization dynamics of the system, such as: scanning tunneling nanolithography, focused ion beam and nanoindentation patterning. By analyzing the evolution of the dot assembly by scanning probe microscopy, we follow the pathway which leads to lateral ordering, discussing the thermodynamic and kinetic effects involved in selective nucleation on patterned substrates.

Self-assembled hyperbranched polymer - gold nanoparticle hybrids : understanding the effect of polymer coverage on assembly size and SERS performance

In the past few years, remarkable progress has been made in unveiling novel and unique optical properties of strongly coupled plasmonic nanostructures. However, application of such plasmonic nanostructures in biomedicine remains challenging due to the lack of facile and robust assembly methods for producing stable nanostructures. Previous attempts to achieve plasmonic nano-assemblies using molecular ligands were limited due to the lack of flexibility that could be exercised in forming them. Here, we report the utilization of tailor-made hyperbranched polymers (HBP) as linkers to assemble gold nanoparticles (NPs) into nano-assemblies. The ease and flexibility in tuning the particle size and number of branch ends of a HBP makes it an ideal candidate as a linker, as opposed to DNA, small organic molecules and linear or dendrimeric polymers. We report a strong correlation of polymer (HBP) concentration with the size of the hybrid nano-assemblies and “hot-spot” density. We have shown that such solutions of stable HBP-gold nano-assemblies can be barcoded with various Raman tags to provide improved surface-enhanced Raman scattering (SERS) compared with non-aggregated NP systems. These Raman barcoded hybrid nano-assemblies, with further optimization of NP shape, size and “hot-spot” density, may find application as diagnostic tools in nanomedicine.

Mussel-inspired bioceramics with self-assembled Ca-P/polydopamine composite nanolayer : preparation, formation mechanism, improved cellular bioactivity and osteogenic differentiation of bone marrow stromal cells

The nanostructured surface of biomaterials plays an important role in improving their in vitro cellular bioactivity as well as stimulating in vivo tissue regeneration. Inspired by the mussel’s adhesive versatility, which is thought to be due to the plaque–substrate interface being rich in 3,4-dihydroxy-L-phenylalamine (DOPA) and lysine amino acids, in this study we developed a self-assembly method to prepare a uniform calcium phosphate (Ca-P)/polydopamine composite nanolayer on the surface of b-tricalcium phosphate (b-TCP) bioceramics by soaking b-TCP bioceramics in Tris–dopamine solution. It was found that the addition of dopamine, reaction temperature and reaction time are three key factors inducing the formation of a uniform Ca-P/polydopamine composite nanolayer. The formation mechanism of a Ca-P/polydopamine composite nanolayer involved two important steps: (i) the addition of dopamine to Tris–HCl solution decreases the pH value and accelerates Ca and P ionic dissolution from the crystal boundaries of b-TCP ceramics; (ii) dopamine is polymerized to form self-assembled polydopamine film and, at the same time, nanosized Ca-P particles are mineralized with the assistance of polydopamine, in which the formation of polydopamine occurs simultaneously with Ca-P mineralization (formation of nanosized microparticles composed of calcium phosphate-based materials), and finally a self-assembled Ca-P/polydopamine composite nanolayer forms on the surface of the b-TCP ceramics. Furthermore, the formed self-assembled Ca-P/polydopamine composite nanolayer significantly enhances the surface roughness and hydrophilicity of b-TCP ceramics, and stimulates the attachment, proliferation, alkaline phosphate (ALP) activity and bone-related gene expression (ALP, OCN, COL1 and Runx2) of human bone marrow stromal cells. Our results suggest that the preparation of self-assembled Ca-P/polydopamine composite nanolayers is a viable method to modify the surface of biomaterials by significantly improving their surface physicochemical properties and cellular bioactivity for bone regeneration application.

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.

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.

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.