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.
The complete Raman spectrum of SnO 2 nanoparticles in presented and analyzed. In addition to the ''classical'' modes observed in the rutile structure, two other regions shown Raman activity for nanoparticles. The Raman bands in the low-frequency region are attributed to acoustic modes associated with the vibration of the individual nanoparticle as a whole. The high-frequency region is activated by surface disorder. A detailed analysis of these regions and the changes in the normal modes of SnO 2 are presented as a function nanoparticle size.
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-innanowire 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. S emiconductor quantum dots have been shown to be excellent building blocks for quantum photonics applications, such as single-photon sources and nano-sensing. Desirable properties of a single-photon emitter include high-fidelity anti-bunching (very small g 2 (t = 0)), narrow emission lines (ideally transform limited to a few microelectronvolt) and high brightness (>1 MHz count rate on standard detector). For simplicity, these properties should be achieved either with electrical injection or non-resonant optical excitation. Desirable properties of a nano-sensor include a high sensitivity to local electric and magnetic fields, with the quantum dot located as close as possible to the target region. A popular realization involves Stranski-Krastanow InGaAs quantum dots embedded in a three-dimensional matrix, which are excellent building blocks for the realization of practical singlephoton sources 1 . However, the photon extraction out of the bulk semiconductor is highly inefficient on account of the large mismatch in refractive indices of GaAs and vacuum. An attractive way forward is to embed the quantum dots in a nanowire 2 . To solve the extraction problem, the nanowire is designed to operate as a single-mode waveguide, a so-called photonic nanowire, with a taper as photon out-coupler 3 . Also, for nano-sensing applications, a quantum dot in a nanowire can be located much closer to the active medium. Top-down fabrication of the photonic waveguide is technologically complex, however. Bottom-up fabrication of the photonic waveguide is very attractive 4-6 , but it is at present challenging to self-assemble quantum dots in the nanowires with narrow linewidths and high yields 7,8 . Nano-sensing applications are at present not highly developed. Other degrees of freedom of the quantum-dot-in-nanowire system that can be usefully exploited are the mechanical modes ...
Molecular beam epitaxy Ga-assisted synthesis of GaAs nanowires is demonstrated. The nucleation and growth are seen to be related to the presence of a SiO 2 layer previously deposited on the GaAs wafer. The interaction of the reactive gallium with the SiO 2 pinholes induces the formation of nanocraters, found to be the key for the nucleation of the nanowires. With SiO 2 thicknesses up to 30 nm, nanocraters reach the underlying substrate, resulting into a preferential growth orientation of the nanowires. Possibly related to the formation of nanocraters, we observe an incubation period of 258 s before the nanowires growth is initiated. © 2008 American Institute of Physics. ͓DOI: 10.1063/1.2837191͔Semiconductor nanowires are believed to play a decisive role in the electronic and optoelectronic devices of the 21st century. Up to now, the synthesis of nanowires is mainly based on the vapor-liquid-solid and vapor-solid-solid mechanisms. 1,2 Common in both mechanisms is that a metal nanoparticle gathers and decomposes catalytically the precursor molecules. Supersaturation of the metal droplet follows and leads to the precipitation of a solid phase underneath the droplet in the form of a nanowire. Typically, gold is used as a catalyst. The use of such an extrinsic catalytic metal is in general not desired and some effort has been directed into finding alternatives. 3,4 Recently, catalyst-free growth has been achieved both with metal-organic chemical vapor deposition and molecular beam epitaxy ͑MBE͒. 5,6 This type of growth has always been linked to the existence of a plain or patterned SiO 2 surface, whose role has still to be clarified. To our knowledge, a detailed study on the nucleation stage of the nanowires and an analysis of the role of the SiO 2 are still missing.Nanowires were grown in a Gen-II MBE system. 2 in. GaAs wafers were sputtered with silicon dioxide; the thickness was varied between 20 and 100 nm. In order to ensure a contamination-free surface, the substrates were dipped for 2 s in a 12% HF aqueous solution, nitrogen blow dried, and were immediately after transferred in the load lock of the growth chamber. In order to desorb any remnant adsorbed molecules at the surface, the wafers were heated to 650°C for 30 min prior to growth. The synthesis was carried out at a temperature of 630°C, an arsenic As 4 partial pressure of 8 ϫ 10 −7 mbar, a Ga rate of 0.25 Å / s and under rotation of 4 rpm.We first discuss nanowires which were grown simultaneously on two different halves of GaAs substrates with the ͑001͒ and ͑111͒B orientations. After cleaning of the surface and HF dip, the two halves were still coated with a 6 nm SiO 2 thin film. Cross-sectional scanning electron microscopy ͑SEM͒ measurements of the grown nanowires are shown in Fig. 1. The micrographs clearly reveal that the nanowires mainly grow perpendicular to the substrate in the case of the ͑111͒B GaAs, and with an angle of ϳ35°in the case of the ͑001͒ GaAs. This result clearly proves the existence of a relation between the nanowire orientation and...
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 ͑TO͒ 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 ͑TO͒. 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 ͑TO͒ and E 2 H modes. Finally, the influence of the surface roughness in the intensity of the longitudinal optical mode on ͕110͖ facets is presented.
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.
We study the influence of Nb doping on the TiO 2 anatase-to-rutile phase transition, using combined transmission electron microscopy, Raman spectroscopy, x-ray diffraction and selected area electron diffraction analysis. This approach enabled anatase-to-rutile phase transition hindering to be clearly observed for low Nb-doped TiO 2 samples. Moreover, there was clear grain growth inhibition in the samples containing Nb. The use of high resolution transmission electron microscopy with our samples provides an innovative perspective compared with previous research on this issue. Our analysis shows that niobium is segregated from the anatase structure before and during the phase transformation, leading to the formation of NbO nanoclusters on the surface of the TiO 2 rutile nanoparticles.
This work reports the in-depth resolved Raman scattering analysis with different excitation wavelengths of Cu2ZnSnS4 layers. Secondary phases constitute a central problem in this material, particularly since they cannot be distinguished by x-ray diffraction. Raman spectra measured with 325 nm excitation light after sputtering the layers to different depths show peaks that are not detectable by excitation in the visible. These are identified with Cu3SnS4 modes at the surface region while spectra measured close to the back region show peaks from ZnS and MoS2. Observation of ZnS is enhanced by resonant excitation conditions achieved when working with UV excitation.
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