Dries Smeets

Size-Dependent Optical Properties of Colloidal PbS Quantum Dots

We quantitatively investigate the size-dependent optical properties of colloidal PbS nanocrystals or quantum dots (Qdots), by combining the Qdot absorbance spectra with detailed elemental analysis of the Qdot suspensions. At high energies, the molar extinction coefficient epsilon increases with the Qdot volume d(3) and agrees with theoretical calculations using the Maxwell-Garnett effective medium theory and bulk values for the Qdot dielectric function. This demonstrates that quantum confinement has no influence on epsilon in this spectral range, and it provides an accurate method to calculate the Qdot concentration. Around the band gap, epsilon only increases with d(1.3), and values are comparable to the epsilon of PbSe Qdots. The data are related to the oscillator strength f(if) of the band gap transition and results agree well with theoretical tight-binding calculations, predicting a linear dependence of f(if) on d. For both PbS and PbSe Qdots, the exciton lifetime tau is calculated from f(if). We find values ranging between 1 and 3 mus, in agreement with experimental literature data from time-resolved luminescence spectroscopy. Our results provide a thorough general framework to calculate and understand the optical properties of suspended colloidal quantum dots. Most importantly, it highlights the significance of the local field factor in these systems.

Pt redistribution during Ni(Pt) silicide formation

We report on a real-time Rutherford backscattering spectrometry study of the erratic redistribution of Pt during Ni silicide formation in a solid phase reaction. The inhomogeneous Pt redistribution in Ni(Pt)Si films is a consequence of the low solubility of Pt in Ni2Si compared to NiSi and the limited mobility of Pt in NiSi. Pt further acts as a diffusion barrier and resides in the Ni2Si grain boundaries, significantly slowing down the Ni2Si and NiSi growth kinetics. Moreover, the observed incorporation of a large amount of Pt in the NiSi seeds indicates that Pt plays a major role in selecting the crystallographic orientation of these seeds and thus in the texture of the resulting Ni1−xPtxSi film.

The influence of Pt redistribution on Ni1−xPtxSi growth properties

We have studied the influence of Pt on the growth of Ni silicide thin films by examining the Pt redistribution during silicide growth. Three different initial Pt configurations were investigated, i.e., a Pt alloy (Ni+Pt/⟨Si⟩), a Pt capping layer (Pt/Ni/⟨Si⟩) and a Pt interlayer (Ni/Pt/⟨Si⟩), all containing 7 at. % Pt relative to the Ni content. The Pt redistribution was probed using in situ real-time Rutherford backscattering spectrometry (RBS) whereas the phase sequence was monitored during the solid phase reaction (SPR) using in situ real-time x-ray diffraction. We found that the capping layer and alloy exhibit a SPR comparable to the pure Ni/⟨Si⟩ system, whereas Pt added as an interlayer has a much more drastic influence on the Ni silicide phase sequence. Nevertheless, for all initial sample configurations, Pt redistributes in an erratic way. This phenomenon can be assigned to the low solubility of Pt in Ni2Si compared to NiSi and the high mobility of Pt in Ni2Si compared to pure Ni. Real-time RBS furt...

Dependence of the sticking coefficient of sputtered atoms on the target-substrate distance

A Ti target was mounted on a planar magnetron and sputtered in a mixture of Ar and N2, resulting in a flux of metallic Ti particles forming a TiN film on a substrate. The sticking coefficient of Ti was determined by comparing the Ti flux towards the substrate with the actual amount of deposited Ti particles, as determined by Rutherford backscattering spectrometry. It was observed that the sticking coefficient of Ti increases significantly with increasing target–substrate distance, but is to a lesser extent influenced by the N2 partial pressure.

The role of lattice mismatch and kinetics in texture development: Co1-xNixSi2 thin films on Si(100)

Mixed Co1−xNixSi2 films (0≤x≤1) were grown by solid phase reaction of homogeneous Co1−xNix metal films, codeposited on Si(100). The texture of these films was contemplated using complementary experimental techniques: Rutherford backscattering and channeling spectrometry, x-ray pole figure measurements, and orientation imaging with electron backscattering diffraction. Based on the increasing Co1−xNixSi2 lattice parameter with increasing Ni concentration, a gradual, continuous improvement of the epitaxial quality of the film would be expected. The observed trend is significantly different. The epitaxial quality of the disilicide film indeed improves with increasing Ni concentration, but only up to 15% Ni. Moreover, the increasing epitaxial quality is due to a large volume fraction of (110)-oriented grains, instead of the anticipated (100) orientation. The most abundant texture component is not necessarily the one with the best in-plane match with the substrate, i.e., epitaxy, nor the one which assures the c...

Nucleation and diffusion during growth of ternary Co1−xNixSi2 thin films studied by complementary techniques in real time

The growth kinetics of ternary Co1−xNixSi2 thin films was studied in real time. The “Kissinger” method was applied to the results of ramped sheet resistance measurements to extract the apparent activation energy for the growth process. By simultaneously acquiring sheet resistance, x-ray diffraction and laser light scattering data on one hand and combining resistance measurements and Rutherford backscattering spectrometry on the other hand, we could distinguish between the initial, nucleation controlled thin film growth, and the subsequent diffusion controlled growth. The apparent activation energy for the initial growth decreases with increasing Ni concentration as a result of a lower nucleation barrier for the ternary disilicide. The markedly different microstructure of the ternary Co1−xNixSi2 films with respect to pure CoSi2 layers lies at the origin of a lower activation energy for the diffusion controlled growth of the ternary films. Despite the low activation energy, these films grow at a much slower...

Simultaneous real-time x-ray diffraction spectroscopy, Rutherford backscattering spectrometry, and sheet resistance measurements to study thin film growth kinetics by Kissinger plots

When the Kissinger method is used to investigate thin film growth kinetics, activation energies obtained are often significantly higher than those of Arrhenius plots based on isothermal studies. The reason for the higher activation energies is related to the sensitivity of the Kissinger analysis to nucleation effects. In fact, this often undesirable effect opens the possibility of studying nucleation barriers in a semiquantitative way. Furthermore, we show that these nucleation effects can be filtered out by a more careful application of the Kissinger method, and activation energies that are consistent with Arrhenius plots are then obtained.

On the growth kinetics of Ni(Pt) silicide thin films

We report on the effect of Pt on the growth kinetics of δ-Ni2Si and Ni1−xPtxSi thin films formed by solid phase reaction of a Ni(Pt) alloyed thin film on Si(100). The study was performed by real-time Rutherford backscattering spectrometry examining the silicide growth rates for initial Pt concentrations of 0, 1, 3, 7, and 10 at. % relative to the Ni content. Pt was found to exert a drastic effect on the growth kinetics of both phases. δ-Ni2Si growth is slowed down tremendously, which results in the simultaneous growth of this phase with Ni1−xPtxSi. Activation energies extracted for the Ni1−xPtxSi growth process exhibit an increase from Ea = 1.35 ± 0.06 eV for binary NiSi to Ea = 2.7 ± 0.2 eV for Ni1−xPtxSi with an initial Pt concentration of 3 at. %. Further increasing the Pt content to 10 at. % merely increases the activation energy for Ni1−xPtxSi growth to Ea = 3.1 ± 0.5 eV.

High-temperature AlN interlayer for crack-free AlGaN growth on GaN

This paper presents a study of the transformation of high-temperature AlN (HT-AlN) interlayer (IL) and its effect on the strain relaxation of Al0.25Ga0.75N/HT-AlN/GaN. The HT-AlN IL capped with Al0.25Ga0.75N transforms into AlGaN IL in which the Al composition increases with the HT-AlN IL thickness while the total Ga content keeps nearly constant. During the HT-AlN IL growth on GaN, the tensile stress is relieved through the formation of V trenches. The filling up of the V trenches by the subsequent Al0.25Ga0.75N growth is identified as the Ga source for the IL transformation, whose effect is very different from a direct growth of HT-AlGaN IL. The a-type dislocations generated during the advancement of V trenches and their filling up propagate into the Al0.25Ga0.75N overlayer. The a-type dislocation density increases dramatically with the IL thickness, which greatly enhances the strain relaxation of Al0.25Ga0.75N. (c) 2008 American Institute of Physics.

In situ study of the growth properties of Ni-rare earth silicides for interlayer and alloy systems on Si(100)

We report on the solid-phase reaction of thin Ni-rare earth films on a Si(100) substrate, for a variety of rare earth (RE) elements (Y, Gd, Dy, and Er). Both interlayer (Ni/RE/〈Si〉) and alloy (Ni-RE/〈Si〉) configurations were studied. The phase sequence during reaction was revealed using real-time x-ray diffraction whereas the elemental diffusion and growth kinetics were examined by real-time Rutherford backscattering spectrometry. All RE elements studied exert a similar influence on the solid phase reaction. Independent of the RE element or its initial distribution a ternary Ni2Si2RE phase forms, which ends up at the surface after NiSi growth. With respect to growth kinetics, the RE metal addition hampers the Ni diffusion process even for low concentrations of 2.5 at. %, resulting in the simultaneous growth of Ni-rich silicide and NiSi. Moreover, the formation of Ni2Si2RE during NiSi growth alters the Ni diffusion mechanism in the interlayer causing a sudden acceleration of the Ni silicide growth. Besides...