Photoluminescence of silicon nano-clusters functionalized microtoroids

We report on the first realization of on-chip toroid microcavities embedding size-controlled silicon nanoclusters (Si-nc), produced by reactive magnetron co-sputtering. We demonstrate functionalized whispering gallery microresonators with low volume and high quality factor. Emission properties are optimized by tailoring the size and the shape of the toroids and the Si-nc distribution. Coalescence of Si-nc during the melting of the toroid is minimized by the design of the microdisk preforms. Photolumines- cence in the whispering gallery modes of 13:5 m diameter microtoroids, is observed in both near-field and far-field

Silicon Nanoscale Materials : From Theoretical Simulations to Photonic Applications

Peer reviewe

Luminescence efficiency at 1.5 μm of Er-doped thick SiO layers and Er-doped SiO∕SiO2 multilayers

International audienceThe luminescence from Er-doped thin films is studied in two different systems. The first one is a SiO single layer. The second one is a SiO / SiO 2 multilayer allowing us to obtain size-controlled silicon nanocrystals. In both systems, the annealing-temperature dependence of the luminescence is investigated. It is shown that the optimal annealing temperatures are equal to 700 and 1050°C for the single layer and the multilayer, respectively. Moreover the luminescence efficiency at 1.5 m is one order of magnitude higher in the single Er-doped SiO layer. These results are discussed in relation to the formation of silicon nanoparticles with annealing treatments

Atomic characterization of Si nanoclusters embedded in SiO2 by atom probe tomography

Silicon nanoclusters are of prime interest for new generation of optoelectronic and microelectronics components. Physical properties (light emission, carrier storage...) of systems using such nanoclusters are strongly dependent on nanostructural characteristics. These characteristics (size, composition, distribution, and interface nature) are until now obtained using conventional high-resolution analytic methods, such as high-resolution transmission electron microscopy, EFTEM, or EELS. In this article, a complementary technique, the atom probe tomography, was used for studying a multilayer (ML) system containing silicon clusters. Such a technique and its analysis give information on the structure at the atomic level and allow obtaining complementary information with respect to other techniques. A description of the different steps for such analysis: sample preparation, atom probe analysis, and data treatment are detailed. An atomic scale description of the Si nanoclusters/SiO2 ML will be fully described. This system is composed of 3.8-nm-thick SiO layers and 4-nm-thick SiO2 layers annealed 1 h at 900°C

Influence of the annealing treatments on the luminescence properties of SiO∕SiO2 multilayers

International audienceThe formation of silicon nanocrystals ͑Si-ncs͒ and their room temperature photoluminescence ͑PL͒ properties were investigated in samples elaborated by the evaporation method. Silicon oxide ͑SiO͒ single layer and SiO / SiO 2 multilayers with different SiO layer thicknesses from 1 to 5 nm were prepared and annealed at different temperatures up to 1050°C. The structure and the formation of Si-nc were studied by transmission electron microscopy ͑TEM͒ and by Fourier transform infrared ͑FTIR͒ absorption spectroscopy. It is demonstrated that the Si-ncs appear by the phase separation process from SiO due to the annealing treatments. Contrary to the SiO single layer, the multilayers are a powerful system to obtain highly luminescent Si-nc and to control the Si-nc size for SiO layer thicknesses lower than or equal to 4 nm. It is clearly shown that, in agreement with the quantum confinement theory, the PL energy is a decreasing function of the Si-nc size. However, thanks to the correlation between FTIR, TEM, and PL results, it is demonstrated that the PL energy is also strongly dependent on the quality of the matrix in which the Si-nc are embedded. A model based on the existence of a SiO x shell surrounding the Si-nc is proposed to explain the PL results

Self organized formation of Ge nanocrystals in multilayers

The aim of this work is to create a process which allows the tailored growth of Ge nanocrystals for use in photovoltic applications. The multilayer systems used here provide a reliable method to control the Ge nanocrystal size after phase separation. In this thesis, the deposition of GeOx/SiO2 and Ge:SiOx~ 2/SiO2 multilayers via reactive dc magnetron sputtering and the self-ordered Ge nanocrystal formation within the GeOx and Ge:SiOx~ 2 sublayers during subsequent annealing is investigated. Mostly the focus of this work is on the determination of the proper deposition conditions for tuning the composition of the systems investigated. For the GeOx/SiO2 multilayers this involves changing the GeOx composition between elemental Ge (x = 0) and GeO2 (x = 2), whereas for the Ge:SiOx~ 2/SiO2 multilayers this involves changing the stoichiometry of the Ge:SiOx~ 2 sublayers in the vicinity of stochiometric silica (x = 2). The deposition conditions are controlled by the variation of the deposition rate, the deposition temperature and the oxygen partial pressure. A convenient process window has been found which allows the sequential deposition of GeOx/SiO2 or Ge:SiOx ~2/SiO2 without changing the oxygen partial pressure during deposition. For stoichiometry determination Rutherford back-scattering spectrometry has been applied extensively. The phase separation in the spatially confined GeOx and Ge:SiOx ~2 sublayers was investigated by X-ray absorption spectroscopy at the Ge K-edge. The Ge sub-oxides content of the as-deposited multilayers diminishes with increasing annealing temperature, showing complete phase separation at approximately 450° C for both systems (using inert N2 at ambient pressure). With the use of chemical reducing H2 in the annealing atmosphere, the temperature regime where the GeOx phase separation occurs is lowered by approximately 100 °C. At temperatures above 400° C the sublayer composition, and thus the density of the Ge nanocrystals, can be altered by making use of the reduction of GeO2 by H2. The Ge nanocrystal formation after subsequent annealing was investigated with X-ray scattering, Raman spectroscopy and electron microscopy. By these methods the existence of 2 - 5 nm Ge nanocrystals at annealing temperatures of 550 (GeOx) - 700° C (Ge:SiOx ~2) has been confirmed which is within the multilayer stability range. The technique used allows the production of extended multilayer stacks (50 periods ~ 300 nm) with very smooth interfaces (roughness ~ 0.5 nm). Thus it was possible to produce Ge nanocrystal layers with ultra-thin SiO2 separation layers (thickness ~ 1 nm) which offers interesting possibilities for charge transport via direct tunneling.:Contents 1 Introduction and motivation 1 2 Basic aspects 6 2.1 Microstructure of sub-stoichiometric oxides (SiOx, GeOx) 6 2.2 Phase transformations 9 2.3 Quantum confinement effect in nanocrystals 12 2.4 Applications of nanostructures in 3rd generation photovoltaics 17 3 Experimental setup 21 3.1 The magnetron deposition chamber 21 3.2 (Reactive) dc sputtering 22 3.3 Annealing processing 26 3.4 X-ray facilities 26 4 Analytical methods 30 4.1 Rutherford backscattering spectrometry (RBS) 30 4.2 Raman scattering 33 4.3 (Grazing incidence) X-ray diffraction (GIXRD) 35 4.4 X-ray reflectivity (XRR) 39 4.5 X-ray absorption near edge structure (XANES) 41 4.6 Transmission electron microscopy (TEM) 42 5 Properties of reactive dc magnetron sputtered Si-Ge-O (multi)layers 44 5.1 Deposition rate and film stoichiometry investigations 44 5.2 Stoichiometry dependent properties of GeOx/SiO2 multilayers 47 5.3 Lateral intercluster distance of the Ge nanocrystals in multilayers 51 6 Confined Ge nanocrystal growth in GeOx/SiO2 multilayers 54 6.1 Phase separation in GeOx single layers and GeOx/SiO2 multilayers 54 6.2 Crystallization in GeOx single layers and GeOx/SiO2 multilayers 58 6.3 Multilayer stability and smallest possible Ge nanocrystal size 60 6.4 Stacked Ge NC films with ultra thin SiO2 separation layers 66 7 Confined Ge nanocrystal growth in Ge:SiOx/SiO2 multilayers 71 7.1 Phase separation in Ge:SiOx/SiO2 multilayers 72 7.2 Crystallisation in Ge:SiOx/SiO2 multilayers 76 8 Summary and conclusions 79 List of Figures 83 List of Tables 85 Bibliography 8

Untersuchungen von fotoaktiven Materialien und Strukturen auf Basis von In-S-Verbindungen und siliziumreichen Oxiden

The thesis consists of two parts: 1. The preparation of new materials based on thioindates and indium sulfides with possible photoactive properties. The synthesized materials were tested in the areas of photovoltaics, photocatalysis and/or photoluminescence. 2. The second part of the work deals with the fabrication of multilayers of SRO (Silicon Rich Oxide) with high Si contents and SiO2 prepared by LPCVD (Low Pressure Chemical Vapor Deposition) as well as with studies on their structural, morphologic, optical and luminescent properties.Die Dissertation umfasst zwei Teile: 1. Die Darstellung neuer Materialien auf Basis von Thioindaten und Indiumsulfiden, die photoaktive Eigenschaften aufweisen können. Die hergestellten Materialien wurden auf den Gebieten der Photoelektronik, Photokatalyse und/oder Photolumineszenz getestet. 2. Der zweite Teil der Arbeit beschäftigt sich mit der Darstellung von Multi-Schichten aus SRO (Silicon Rich Oxide) mit hohem Si-Gehalt und SiO2 durch die LPCVD-Methode (Low Pressure Chemical Vapor Deposition) sowie den Untersuchungen ihrer strukturellen, morphologischen, optischen und lumineszierenden Eigenschaften

Doped and codoped silicon nanocrystals: The role of surfaces and interfaces

Si nanocrystals have been extensively studied because of their novel properties and their potential applications in electronic, optoelectronic, photovoltaic, thermoelectric and biological devices. These new properties are achieved through the combination of the quantum confinement of carriers and the strong influence of surface chemistry. As in the case of bulk Si the tuning of the electronic, optical and transport properties is related to the possibility of doping, in a controlled way, the nanocrystals. This is a big challenge since several studies have revealed that doping in Si nanocrystals differs from the one of the bulk. Theory and experiments have underlined that doping and codoping are influenced by a large number of parameters such as size, shape, passivation and chemical environment of the silicon nanocrystals. However, the connection between these parameters and dopant localization as well as the occurrence of self-purification effects are still not clear. In this review we summarize the latest progress in this fascinating research field considering free-standing and matrix-embedded Si nanocrystals both from the theoretical and experimental point of view, with special attention given to the results obtained by ab-initio calculations and to size-, surface- and interface-induced effects

Silicon-Rich Oxide Obtained by Low-Pressure Chemical Vapor Deposition to Develop Silicon Light Sources

Abstract Off stoichiometric silicon oxide, also known as silicon-rich oxide (SRO), is a lightemitting material that is compatible with silicon technology; therefore, it is a good candidate to be used as a light source in all-silicon optoelectronic circuits. The SRO obtained by low-pressure chemical vapor deposition (LPCVD) has shown the best luminescent properties compared to other techniques. In spite of LPCVD being a simple technique, it is not a simple task to obtain SRO with exact silicon excess in a reliable and repetitive way. In this work, the expertise obtained in our group to obtain SRO by LPCVD with precise variation is presented. Also, the characteristics of this SRO obtained in our group are revised and discussed. It is demonstrated that LPCVD is an excellent technique to obtain single layers and multilayers of nanometric single layers with good characteristics