Thermal transport in epitaxial Si1-x Ge x alloy nanowires with varying composition and morphology.

We report on structural, compositional, and thermal characterization of self-assembled in-plane epitaxial Si1-x Ge x alloy nanowires grown by molecular beam epitaxy on Si (001) substrates. The thermal properties were studied by means of scanning thermal microscopy (SThM), while the microstructural characteristics, the spatial distribution of the elemental composition of the alloy nanowires and the sample surface were investigated by transmission electron microscopy and energy dispersive x-ray microanalysis. We provide new insights regarding the morphology of the in-plane nanostructures, their size-dependent gradient chemical composition, and the formation of a 5 nm thick wetting layer on the Si substrate surface. In addition, we directly probe heat transfer between a heated scanning probe sensor and Si1-x Ge x alloy nanowires of different morphological characteristics and we quantify their thermal resistance variations. We correlate the variations of the thermal signal to the dependence of the heat spreading with the cross-sectional geometry of the nanowires using finite element method simulations. With this method we determine the thermal conductivity of the nanowires with values in the range of 2-3 W m-1 K-1. These results provide valuable information in growth processes and show the great capability of the SThM technique in ambient environment for nanoscale thermal studies, otherwise not possible using conventional techniques.

Effects of magnetic field gradients on the aggregation dynamics of colloidal magnetic nanoparticles.

We have used low-field (1)H nuclear-magnetic resonance (NMR) spectroscopy and molecular dynamics (MD) to investigate the aggregation dynamics of magnetic particles in ionic ferrofluids (IFFs) in the presence of magnetic field gradients. At the beginning of the experiments, the measured NMR spectra were broad and asymmetric, exhibiting two features attributed to different dynamical environments of water protons, depending on the local strength of the field gradients. Hence, the spatial redistribution of the magnetic particles in the ferrofluid caused by the presence of an external magnetic field in a time scale of minutes can be monitored in real time, following the changes in the features of the NMR spectra during a period of about an hour. As previously reported [Heinrich et al., Phys. Rev. Lett., 2011, 106, 208301], in the homogeneous magnetic field of a NMR spectrometer, the aggregation of the particles of the IFF proceeds in two stages. The first stage corresponds to the gradual aggregation of monomers prior to and during the formation of chain-like structures. The second stage proceeds after the chains have reached a critical average length, favoring lateral association of the strings into hexagonal zipped-chain superstructures or bundles. In this work, we focus on the influence of a strongly inhomogeneous magnetic field on the aforementioned aggregation dynamics. The main observation is that, as the sample is immersed in a certain magnetic field gradient and kept there for a time τinh, magnetophoresis rapidly converts the ferrofluid into an aggregation state which finds its correspondence to a state on the evolution curve of the pristine sample in a homogeneous field. From the degree of aggregation reached at the time τinh, the IFF sample just evolves thereafter in the homogeneous field of the NMR spectrometer in exactly the same way as the pristine sample. The final equilibrium state always consists of a colloidal suspension of zipped-chain bundles with the chain axes aligned along the magnetic field direction.

In-plane thermal conductivity of sub-20 nm thick suspended mono-crystalline Si layers.

We measure the thermal conductivity of a 17.5-nm-thick single crystalline Si layer by using a suspended structure developed from a silicon-on-insulator wafer, in which the Si layer bridges the suspended platforms. The obtained value of 19 Wm(-1) K(-1) at room temperature represents a tenfold reduction with respect to bulk Si. This design paves the way for subsequent lateral nanostructuration of the layer with lithographic techniques, to define different geometries such as Si nanowires, nanostrips or phononic grids. As a proof of concept, nanostrips of 0.5 × 10 µm have been defined by focused ion beam (FIB) in the ultrathin Si layer. After the FIB cutting process with Ga ions at 30 kV and 100 pA, the measured thermal conductivity dramatically decreased to 1.7 Wm(-1) K(-1), indicating that the structure became severely damaged (amorphous). Re-crystallization of the structure was promoted by laser annealing while monitoring the Raman spectra. The thermal conductivity of the layer increased again to a value of 9.5 Wm(-1) K(-1) at room temperature, below that of the single crystalline material due to phonon scattering at the grain boundaries.

Probing local strain and composition in Ge nanowires by means of tip-enhanced Raman scattering.

Local strain and Ge content distribution in self-assembled, in-plane Ge/Si nanowires grown by combining molecular beam epitaxy and the metal-catalyst assisted-growth method were investigated by tip-enhanced Raman scattering. We show that this technique is essential to study variations of physical properties of single wires at the nanoscale, a task which cannot be achieved with conventional micro-Raman scattering. As two major findings, we report that (i) the Ge distribution in the (001) crystallographic direction is inhomogeneous, displaying a gradient with a higher Ge content close to the top surface, and (ii) in contrast, the (uncapped) wires exhibit essentially the same small residual compressive strain everywhere along the wire.

Magneto-optical enhancement by plasmon excitations in nanoparticle/metal structures.

Coupling magnetic materials to plasmonic structures provides a pathway to dramatically increase the magneto-optical response of the resulting composite architecture. Although such optical enhancement has been demonstrated in a variety of systems, some basic aspects are scarcely known. In particular, reflectance/transmission modulations and electromagnetic field intensification, both triggered by plasmon excitations, can contribute to the magneto-optical enhancement. However, a quantitative evaluation of the impact of both factors on the magneto-optical response is lacking. To address this issue, we have measured magneto-optical Kerr spectra on corrugated gold/dielectric interfaces with magnetic (nickel and iron oxide) nanoparticles. We find that the magneto-optical activity is enhanced by up to an order of magnitude for wavelengths that are correlated to the excitation of propagating or localized surface plasmons. Our work sheds light on the fundamental principles for the observed optical response and demonstrates that the outstanding magneto-optical performance is originated by the increase of the polarization conversion efficiency, whereas the contribution of reflectance modulations is negligible.

Dynamics of the field-induced formation of hexagonal zipped-chain superstructures in magnetic colloids.

Combining nuclear magnetic resonance and molecular dynamics simulations, we unravel the long-time dynamics of a paradigmatic colloid with strong dipole-dipole interactions. In a homogeneous magnetic field, ionic ferrofluids exhibit a stepwise association process from ensembles of monomers over stringlike chains to bundles of hexagonal zipped-chain patches. We demonstrate that attractive van der Waals interactions due to charge-density fluctuations in the magnetic particles play the key role for the dynamical stabilization of the hexagonal superstructures against thermal dissociation. Our results give insight into the dynamics of self-organization in systems dominated by dipolar interactions.

On the assessment of hydroxyapatite fluoridation by means of Raman scattering.

Hydroxyapatite is the main mineral component of bones and teeth. Fluorapatite, a bioceramic that can be obtained from hydroxyapatite by chemical substitution of the hydroxide ions with fluoride, exhibits lower mineral solubility and larger mechanical strength. Despite the widespread use of fluoride against caries, a reliable technique for unambiguous assessment of fluoridation in in vitro tests is still lacking. Here we present a method to probe fluorapatite formation in fluoridated hydroxyapatite by combining Raman scattering with thermal annealing. In synthetic minerals, we found that effectively fluoride substituted hydroxyapatite transforms into fluorapatite only after heat treatment, due to the high activation energy for this first order phase transition.

Direct imaging of the visible emission bands from individual ZnO nanowires by near-field optical spectroscopy.

Room-temperature photoluminescence (PL) measurements have been performed on single-crystal ZnO nanowires grown on SiO2/Si and quartz substrates by the vapor transport method using Au as a catalyst. Two emission bands are apparent, one in the UV spectral region around 380 nm (3.26 eV) associated with exciton recombination processes and a much broader structure in the visible range from 420 to 700 nm, which exhibits two distinct peak-like features around 520 and 590 nm (2.38 and 2.10 eV). Spectrally resolved scanning near-field optical microscopy (SNOM) of single ZnO nanowires have been performed for a direct imaging of the PL emission with spatial resolution below 100 nm. SNOM results provide evidence that the yellow emission band observed at 590 nm is a unique property of the ZnO nanowires, being most likely related to radiative recombination processes associated with Au impurities introduced during the catalytic growth.

Crystallisation of amorphous germanium thin films.

By combining cross-sectional transmission and scanning electron microscopy with Raman scattering we have investigated the mechanism of nanocrystal formation in ultrathin amorphous SiO2/Ge/SiO2 trilayers grown by e-beam evaporation as a function of annealing temperature and a-Ge layer thickness. We observe that with decreasing a-Ge thickness the amorphous-to-crystalline (a-to-c) transition occurs at considerably higher temperatures, even avoiding crystallisation for very thin films below 2 nm thickness. Furthermore, we demonstrate that the formation of Ge nanocrystals by annealing at around 900 degrees C takes place driven by a liquid-mediated mechanism. As indicated by the observed microstructure, the metallic liquid film dewets from the surface forming droplets that upon cooling and under the influence of the SiO2 capping layer, solidify into barrel-type nanocrystals.

Dynamics of magnetic-field-induced clustering in ionic ferrofluids from Raman scattering.

Using Raman spectroscopy, the authors have investigated the aggregation/disgregation of magnetic nanoparticles in dense ionic ferrofluids (IFF) into clusters due to the action of an inhomogeneous external magnetic field. Evidence for changes in particle density and/or effective cluster size were obtained from the variation of the Raman intensity in a time window from 10 s to 10 min for magnetic fields up to 350 mT and at a temperature of 28 degrees C. Clustering sets in already at very low fields (>15 mT) and the IFF samples exhibit a clear hysteresis in the Raman spectra after releasing the magnetic field, which lasts for many hours at room temperature. The authors determined the characteristic times of the two competing processes, that of field-induced cluster formation and, at room temperature, that of thermal-activated dissociation, to range from 100 to 150 s.

Influence of Si interdiffusion on carbon-induced growth of Ge quantum dots: a strategy for tuning island density.

We have studied the epitaxial growth of self-assembled Ge quantum dots when a submonolayer of carbon is deposited on a Ge wetting layer (WL) prior to the growth of the dots. Using atomic-force microscopy combined with optical techniques like Raman and ellipsometry, we performed a systematic study of the role played by thermally activated Si interdiffusion on dot density, composition and morphology, by changing only the growth temperature T(WL) of the WL. Strikingly, we observe that higher dot densities and a narrower size distribution are achieved by increasing the deposition temperature T(WL), i.e. by enhancing Si interdiffusion from the substrate. We suggest a two-stage growth procedure for fine tuning of dot topography (density, shape and size) useful for possible optoelectronic applications.

Raman spectroscopy on surfacted ferrofluids in a magnetic field.

We investigated the effect of an external magnetic field up to 0.25 T on the Raman spectra of surfacted ferrofluids with various magnetic-particle concentrations. With increasing magnetic field the Raman spectra, which display the characteristic broad bands associated with vibrations of surfactant and water molecules, show a pronounced decrease in intensity in the range up to 50 mT. We interpret this behavior as due to an increase of the local particle concentration in the magnetic fluid. At larger fields a magnetic excitation with an intensity growing in proportion to the magnetization of the ferrofluid becomes apparent at around 4400 cm(-1). We consider both effects as evidence for the formation of a solid structure by the magnetic nanoparticles in the presence of a magnetic field.