Physical characterization of complex semiconductor nanomaterials : from hetero-structures to 2D super-lattices

Le développement de nanomatériaux semi-conducteurs s'accompagne d'une complexification de leur structure cristalline et de leur composition chimique. Les interfaces y constituent un élément essentiel, qu'il est nécessaire d'étudier. Pour cela, il faut disposer d'outils de caractérisation adaptés, qui sont décrits dans le premier chapitre de ce mémoire. Ces instruments ont tout d'abord servi à explorer des nano-fils semi-conducteurs à hétéro-structures (chapitre 2), dans lesquels des inclusions poly-types présentent un piégeage du niveau de Fermi en surface, conduisant ainsi à la formation de jonctions surfaciques i-p. Dans un second temps, des nano-cristaux à hétéro-structures ont été analysés (chapitre 3). Les mesures ont révélé une transformation de phase des nano-cristaux sous excitation lumineuse, qui a pour origine une différence de structure cristalline des deux matériaux de base. En parallèle, des études ont été menées sur de nouveaux matériaux à deux dimensions constitués de pores : le Silicène (chapitre 4), l'équivalent du graphène à base d'atomes de silicium uniquement, et des super-réseaux de nano-cristaux semi-conducteurs fusionnés, possédant une structure poreuse (chapitre 5). Dans les deux cas, après avoir étudié la structure cristalline des matériaux, des mesures de transport ont été effectuées grâce à la technique de mesure par microscopie à effet tunnel à pointe multiple. De par la faible résistivité mesurée, ces matériaux servent de système modèle unique pour comprendre le transport dans des réseaux poreux à deux dimensions.The development of semi-conductor nanomaterials takes along with an increase of the complexity regarding their crystalline structure and chemical composition. Interfaces are essential in accounting for the physical properties of the materials and require a thorough investigation. It relies on the use of specific instruments, that are described in the first section of this work. These instruments are then used to explore hetero-structure nanowires, that contain poly-types segments with different Fermi level pinnings at the surface, leading to i-p junctions (section 2). Hetero-structure nanocrystals have also been characterized (section 3). Their study has revealed a phase transformation under light irradiation, that is attributed to the different crystalline structures between their core and their shell. Along with these investigations, novel two-dimensional semi-conductor crystals have been explored due to the exotic electronic structures that they could exhibit. Silicene, the Graphene analog, and porous networks of semi-conductor nanocrystals have been studied (section 4 and 5 respectively). The transport properties have been characterized with multiple probes Scanning Tunneling Microscopy and have revealed the uniqueness of these systems to improve our understanding of the electrical transport in two-dimensional crystals

Electronic properties of atomically coherent square PbSe nanocrystal superlattice resolved by Scanning Tunneling Spectroscopy

Rock-salt lead selenide nanocrystals can be used as building blocks for large scale square superlattices via two-dimensional assembly of nanocrystals at a liquid-air interface followed by oriented attachment. Here we report Scanning Tunneling Spectroscopy measurements of the local density of states of an atomically coherent superlattice with square geometry made from PbSe nanocrystals. Controlled annealing of the sample permits the imaging of a clean structure and to reproducibly probe the band gap and the valence hole and conduction electron states. The measured band gap and peak positions are compared to the results of optical spectroscopy and atomistic tight-binding calculations of the square superlattice band structure. In spite of the crystalline connections between nanocrystals that induce significant electronic couplings, the electronic structure of the superlattices remains very strongly influenced by the effects of disorder and variability

Sheet resistance of multi-layer stacking of silicene

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Electrical characterization of semiconductor nanowires by scanning tunneling microscopy

In order to understand the structural and electronic properties of semiconductor nanowires, scanning tunneling microscopy is an appealing technique that can supplement transmission electron microscopies and conventional electrical characterization techniques. It is able to probe the surface of semiconductor materials at the atomic scale and can be successfully applied to study the nanofaceting morphology, the atomic structure and the surface composition of oxide-free nanowire sidewalls. Based on the advantages provided by the unique geometry of semiconductor nanowires for a low-cost and efficient integration into nanoscale devices, additional characterization schemes performed with multiple probe scanning tunneling microscopy are also presented to get a deeper understanding of their transport properties

Synthesis and electrical conductivity of multilayer silicene

The epitaxial growth and the electrical resistance of multilayer silicene on the Ag(111) surface has been investigated. We show that the atomic structure of the first silicene layer differs from the next layers and that the adsorption of Si induces the formation of extended silicene terraces surrounded by step bunching. Thanks to the controlled contact formation between the tips of a multiple probe scanning tunneling microscope and these extended terraces, a low sheet resistance, albeit much higher than the electrical resistance of the underlying silver substrate, has been measured, advocating for the electrical viability of multilayer silicene

Organization and magnetic properties of FePt nanoparticles deposited on graphene/Ir moiré pattern

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Nanoscale carrier multiplication mapping in a Si diode

International audienceCarrier multiplication (CM), the creation of electron-hole pairs from an excited electron, has been investigated in a silicon p-n junction by multiple probe scanning tunneling microscopy. The technique enables an unambiguous determination of the quantum yield based on the direct measurement of both electron and hole currents, that are generated by hot tunneling electrons. The combined effect of impact ionization, carrier diffusion and recombination is directly visualized from the spatial mapping of the CM efficiency. Atomically well-ordered areas of the p-n junction surface sustain the highest CM rate, demonstrating the key role of the surface in reaching high yield

Elaboration of nanomagnet arrays: organization and magnetic properties of mass-selected FePt nanoparticles deposited on epitaxially grown graphene on Ir(111)

International audienceThe moiré pattern created by the epitaxy of a graphene sheet on an iridium substrate can be used as a template for the growth of 2D atomic or cluster arrays. We observed for the first time a coherent organization of hard magnetic preformed FePt nanoparticles on the 2D lattice of graphene/Ir(111). Nanoparticles of 2 nm diameter have been mass-selected in gas phase and deposited with a low energy on the hexagonal moiré pattern. Their morphology and organization have been investigated using Grazing Incidence Small Angle X-ray Scattering, while their magnetic properties have been studied by X-ray Magnetic Circular Dichroism, both pointing to a FePt cluster/graphene surface specific interaction. The spatial coherence of the nanoparticles is preserved upon annealing up to 700°C where the hard magnetic phase of FePt is obtained

Electronic properties of atomically coherent square PbSe nanocrystal superlattice resolved by Scanning Tunneling Spectroscopy

Rock-salt lead selenide nanocrystals can be used as building blocks for large scale square superlattices via two-dimensional assembly of nanocrystals at a liquid-air interface followed by oriented attachment. Here we report Scanning Tunneling Spectroscopy measurements of the local density of states of an atomically coherent superlattice with square geometry made from PbSe nanocrystals. Controlled annealing of the sample permits the imaging of a clean structure and to reproducibly probe the band gap and the valence hole and conduction electron states. The measured band gap and peak positions are compared to the results of optical spectroscopy and atomistic tight-binding calculations of the square superlattice band structure. In spite of the crystalline connections between nanocrystals that induce significant electronic couplings, the electronic structure of the superlattices remains very strongly influenced by the effects of disorder and variability