Exciton localization mechanisms in wurtzite/zinc-blende GaAs nanowires

We investigate the emission properties of excitons in GaAs nanowires containing quantum disks formed by structural alternation between the zinc-blende and wurtzite phases, by means of temperature-dependent photoluminescence. At 10 K the emission from an ensemble of disks is distributed in a band of full width at half maximum ∼30 meV, whereas the emission linewidth for a single disk is 700 μeV. While the disk ensemble emission exhibits an S-shaped temperature dependence, the emission from single quantum disks follows the temperature dependence of the band gap over the whole temperature range. This indicates that intradisk exciton localization on impurities is negligible and that increasing the temperature induces a transfer of excitons from narrow to thick disks along the length of the wires. Our observations of the emission linewidth for single crystal-phase quantum disks show a scattering rate of excitons with acoustic phonons eight times larger than the values usually reported for (Al,Ga)As/GaAs quantum wells. This large scattering rate demonstrates that the electron effective mass in wurtzite GaAs is much heavier than in zinc-blende GaAs and is evidence of coupling between the Γ7 and Γ8 conduction bands of wurtzite GaAs.We acknowledge financial support from the Poynton Cambridge Australia Scholarship and from the European Union Seventh Framework Program under grant agreement No. 265073. A.F.iM. and E.U. acknowledge funding through the Marie Curie Excellence grant SENFED. S.C.B. thanks S.N.F. for funding through the Marie-Heim Vögtlin scheme

Growth study of indium-catalyzed silicon nanowires by plasma enhanced chemical vapor deposition

Indium was used as a catalyst for the synthesis of silicon nanowires in a plasma enhanced chemical vapor deposition reactor. In order to foster the catalytic activity of indium, the indium droplets had to be exposed to a hydrogen plasma prior to nanowire growth in a silane plasma. The structure of the nanowires was investigated as a function of the growth conditions by electron microscopy and Raman spectroscopy. The nanowires were found to crystallize along the , or growth direction. When growing on the and directions, they revealed a similar crystal quality and the presence of a high density of twins along the {111} planes. The high density and periodicity of these twins lead to the formation of hexagonal domains inside the cubic structure. The corresponding Raman signature was found to be a peak at 495 cm−1, in agreement with previous studies. Finally, electron energy loss spectroscopy indicates an occasional migration of indium during growt

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

A novel 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

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 E1(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 E1(TO). The transversal optical mode related to the wurtzite structure, E2H, is measured between 254 and 256 cm-1, depending on the wurtzite content. The azymutal dependence of E2H 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 E1(TO) and E2H modes. Finally, the influence of the surface roughness in the intensity of the longitudinal optical mode on {110} facets is presented.Comment: 28 pages, 12 figures. to be published in Phys. Rev.

Structural and optical properties of high quality zinc-blende/wurtzite GaAs hetero-nanowires

The structural and optical properties of 3 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.Comment: 24 page

Three-dimensional nanoscale study of Al segregation and quantum dot formation in GaAs/AlGaAs core-shell nanowires

GaAs/Al-GaAs core-shell nanowires fabricated by molecular beam epitaxy contain quantum confining structures susceptible of producing narrow photoluminescence (PL) and single photons. The nanoscale chemical mapping of these structures is analyzed in 3D by atom probe tomography (APT). The study allows us to confirm that Al atoms tend to segregate within the AlGaAs shells towards the vertices of the hexagons defining the nanowire cross section. We also find strong alloy fluctuations remaining AlGaAs shell, leading occasionally to the formation of quantum dots (QDs). The PL emission energies predicted in the framework of a 3D effective mass model for a QD analyzed by APT and the PL spectra measured on other nanowires from the same growth batch are consistent within the experimental uncertainties. (C) 2014 AIP Publishing LLC

III-V nanowire arrays: growth and light interaction

Semiconductor nanowire arrays are reproducible and rational platforms for the realization of high performing designs of light emitting diodes and photovoltaic devices. In this paper we present an overview of the growth challenges of III-V nanowire arrays obtained by molecular beam epitaxy and the design of III-V nanowire arrays on silicon for solar cells. While InAs tends to grow in a relatively straightforward manner on patterned (111) Si substrates, GaAs nanowires remain more challenging; success depends on the cleaning steps, annealing procedure, pattern design and mask thickness. Nanowire arrays might also be used for next generation solar cells. We discuss the photonic effects derived from the vertical configuration of nanowires standing on a substrate and how these are beneficial for photovoltaics. Finally, due to the special interaction of light with standing nanowires we also show that the Raman scattering properties of standing nanowires are modified. This result is important for fundamental studies on the structural and functional properties of nanowires

Growth mechanisms and process window for InAs V-shaped nanoscale membranes on Si[001]

Organized growth of high aspect-ratio nanostructures such as membranes is interesting for opto-electronic and energy harvesting applications. Recently, we reported a new form of InAs nano-membranes grown on Si substrates with enhanced light scattering properties. In this paper we study how to tune the morphology of the membranes by changing the growth conditions. We examine the role of the V/III ratio, substrate temperature, mask opening size and inter-hole distances in determining the size and shape of the structures. Our results show that the nano-membranes form by a combination of the growth mechanisms of nanowires and the Stranski-Krastanov type of quantum dots: in analogy with nanowires, the length of the membranes strongly depends on the growth temperature and the V/III ratio; the inter-hole distance of the sample determines two different growth regimes: competitive growth for small distances and an independent regime for larger distances. Conversely, and similarly to quantum dots, the width of the nano-membranes increases with the growth temperature and does not exhibit dependence on the V/III ratio. These results constitute an important step towards achieving rational design of high aspect-ratio nanostructures