Sonia Conesa-Boj

Structural and optical properties of high quality zinc-blende/wurtzite GaAs nanowire heterostructures

The structural and optical properties of three different kinds of GaAs nanowires with 100% zinc-blende structure and with an average of 30% and 70% wurtzite are presented. A variety of shorter and longer segments of zinc-blende or wurtzite crystal phases are observed by transmission electron microscopy in the nanowires. Sharp photoluminescence lines are observed with emission energies tuned from 1.515 eV down to 1.43 eV when the percentage of wurtzite is increased. The downward shift of the emission peaks can be understood by carrier confinement at the interfaces, in quantum wells and in random short period superlattices existent in these nanowires, assuming a staggered band offset between wurtzite and zinc-blende GaAs. The latter is confirmed also by time-resolved measurements. The extremely local nature of these optical transitions is evidenced also by cathodoluminescence measurements. Raman spectroscopy on single wires shows different strain conditions, depending on the wurtzite content which affects also the band alignments. Finally, the occurrence of the two crystallographic phases is discussed in thermodynamic terms.

Self-assembled quantum dots in a nanowire system for quantum photonics

Quantum dots embedded within nanowires represent one of the most promising technologies for applications in quantum photonics. Whereas the top-down fabrication of such structures remains a technological challenge, their bottom-up fabrication through self-assembly is a potentially more powerful strategy. However, present approaches often yield quantum dots with large optical linewidths, making reproducibility of their physical properties difficult. We present a versatile quantum-dot-in-nanowire system that reproducibly self-assembles in core-shell GaAs/AlGaAs nanowires. The quantum dots form at the apex of a GaAs/AlGaAs interface, are highly stable, and can be positioned with nanometre precision relative to the nanowire centre. Unusually, their emission is blue-shifted relative to the lowest energy continuum states of the GaAs core. Large-scale electronic structure calculations show that the origin of the optical transitions lies in quantum confinement due to Al-rich barriers. By emitting in the red and self-assembling on silicon substrates, these quantum dots could therefore become building blocks for solid-state lighting devices and third-generation solar cells.

Raman spectroscopy of wurtzite and zinc-blende GaAs nanowires: Polarization dependence, selection rules, and strain effects

Polarization-dependent Raman scattering experiments realized on single GaAs nanowires with different percentages of zinc-blende and wurtzite structure are presented. The selection rules for the special case of nanowires are found and discussed. In the case of zinc-blende, the transversal optical mode E-1 (TO) at 267 cm(-1) exhibits the highest intensity when the incident and analyzed polarization are parallel to the nanowire axis. This is a consequence of the nanowire geometry and dielectric mismatch with the environment, and in quite good agreement with the Raman selection rules. We also find a consistent splitting of 1 cm(-1) of the E-1 (TO). The transversal optical mode related to the wurtzite structure, E-2(H), is measured between 254 and 256 cm(-1), depending on the wurtzite content. The azimuthal dependence of E-2(H) indicates that the mode is excited with the highest efficiency when the incident and analyzed polarization are perpendicular to the nanowire axis, in agreement with the selection rules. The presence of strain between wurtzite and zinc-blende is analyzed by the relative shift of the E-1 (TO) and E-2(H) modes. Finally, the influence of the surface roughness in the intensity of the longitudinal optical mode on {110} facets is presented.

Direct correlation of crystal structure and optical properties in wurtzite/zinc-blende GaAs nanowire heterostructures

A method for the direct correlation at the nanoscale of structural and optical properties of single GaAs nanowires is reported. Nanowires consisting of 100% wurtzite and nanowires presenting zinc-blende/wurtzite polytypism are investigated by photoluminescence spectroscopy and transmission electron microscopy. The photoluminescence of wurtzite GaAs is consistent with a band gap of 1.5 eV. In the polytypic nanowires, it is shown that the regions that are predominantly composed of either zinc-blende or wurtzite phase show photoluminescence emission close to the bulk GaAs band gap, while regions composed of a nonperiodic superlattice of wurtzite and zinc-blende phases exhibit a redshift of the photoluminescence spectra as low as 1.455 eV. The dimensions of the quantum heterostructures are correlated with the light emission, allowing us to determine the band alignment between these two crystalline phases. Our first-principles electronic structure calculations within density functional theory, employing a hybrid-exchange functional, predict band offsets and effective masses in good agreement with experimental results.

Plasma-enhanced low temperature growth of silicon nanowires and hierarchical structures by using tin and indium catalysts

Plasma-enhanced low temperature growth (<300 degrees C) of silicon nanowires (SiNWs) and hierarchical structures via a vapor-liquid-solid (VLS) mechanism are investigated. The SiNWs were grown using tin and indium as catalysts prepared by in situ H(2) plasma reduction of SnO(2) and ITO substrates, respectively. Effective growth of SiNWs at temperatures as low as 240 degrees C have been achieved, while tin is found to be more ideal than indium in achieving a better size and density control of the SiNWs. Ultra-thin (4-8 nm) silica nanowires, sprouting from the dendritic nucleation patterns on the catalysts surface, were also observed to form during the cooling process. A kinetic growth model has been proposed to account for their formation mechanism. This hierarchical structure combines the advantages of the size and position controllability from the catalyst-on-top VLS-SiNWs and the ultra-thin size from the catalyst-on-bottom VLS-ScNWs.

Catalyst-free nanowires with axial InxGa1-xAs/GaAs heterostructures

Self-catalyzed growth of axial In(x)Ga(1-x)As/GaAs heterostructures has been realized by molecular beam epitaxy. The growth of the wires is achieved from gallium/indium alloy droplets that are nucleated in situ. By variation of the In/Ga beam flux during the growth it was possible to vary the effective indium content up to x = 5%, as deduced from photoluminescence measurements. We have analyzed the dependence of the alloy concentration on the growth conditions and present a simple model for the growth. The heterostructures grown with the method presented were spatially mapped along the wires with confocal microphotoluminescence and cathodoluminescence. It was found as expected that the emission of GaAs/In(x)Ga(1-x)As/GaAs heterostructures is localized. This work is important for the use of an external catalyst-free growth of complex axial heterostructures and related opto-electronic devices that facilitates its possible integration in the device or system fabrication processes.

Long range epitaxial growth of prismatic heterostructures on the facets of catalyst-free GaAs nanowires

Molecular beam epitaxy is used for the synthesis of catalyst-free GaAs nanowires and related quantum heterostructures. After growth of the nanowire GaAs core, the conditions are changed in situ towards standard MBE planar growth in order to obtain quantum heterostructures on the facets of the nanowires. Depending on the nanowire orientation, different geometries of the quantum heterostructures are obtained. This growth method is fully characterized by high resolution and scanning transmission electron microscopy and Z-contrast electron tomography. The growth conditions are also tuned for the optimization and homogeneity of the optical properties. The feedback of these analyses allows the tuning of the growth conditions according to the required optical properties. This work is the basis for obtaining a new generation of devices based on the heterostructures existing on the nanowire facets.

Hexagonal silicon realized

Silicon, arguably the most important technological semiconductor, is predicted to exhibit a range of new and interesting properties when grown in the hexagonal crystal structure. To obtain pure hexagonal silicon is a great challenge because it naturally crystallizes in the cubic structure. Here, we demonstrate the fabrication of pure and stable hexagonal silicon evidenced by structural characterization. In our approach, we transfer the hexagonal crystal structure from a template hexagonal gallium phosphide nanowire to an epitaxially grown silicon shell, such that hexagonal silicon is formed. The typical ABABAB... stacking of the hexagonal structure is shown by aberration-corrected imaging in transmission electron microscopy. In addition, X-ray diffraction measurements show the high crystalline purity of the material. We show that this material is stable up to 9 GPa pressure. With this development, we open the way for exploring its optical, electrical, superconducting, and mechanical properties.

Gold-Free Ternary III-V Antimonide Nanowire Arrays on Silicon: Twin-Free down to the First Bilayer

With the continued maturation of III–V nanowire research, expectations of material quality should be concomitantly raised. Ideally, III–V nanowires integrated on silicon should be entirely free of extended planar defects such as twins, stacking faults, or polytypism, position-controlled for convenient device processing, and gold-free for compatibility with standard complementary metal–oxide–semiconductor (CMOS) processing tools. Here we demonstrate large area vertical GaAsxSb1–x nanowire arrays grown on silicon (111) by molecular beam epitaxy. The nanowires’ complex faceting, pure zinc blende crystal structure, and composition are mapped using characterization techniques both at the nanoscale and in large-area ensembles. We prove unambiguously that these gold-free nanowires are entirely twin-free down to the first bilayer and reveal their three-dimensional composition evolution, paving the way for novel infrared devices integrated directly on the cost-effective Si platform.

Gallium assisted plasma enhanced chemical vapor deposition of silicon nanowires

Silicon nanowires have been grown with gallium as catalyst by plasma enhanced chemical vapor deposition. The morphology and crystalline structure has been studied by electron microscopy and Raman spectroscopy as a function of growth temperature and catalyst thickness. We observe that the crystalline quality of the wires increases with the temperature at which they have been synthesized. The crystalline growth direction has been found to vary between <111> and <112>, depending on both the growth temperature and catalyst thickness. Gallium has been found at the end of the nanowires, as expected from the vapor-liquid-solid growth mechanism. These results represent good progress towards finding alternative catalysts to gold for the synthesis of nanowires.