Ultrafast collinear scattering and carrier multiplication in graphene.

Graphene is emerging as a viable alternative to conventional optoelectronic, plasmonic and nanophotonic materials. The interaction of light with charge carriers creates an out-of-equilibrium distribution, which relaxes on an ultrafast timescale to a hot Fermi-Dirac distribution, that subsequently cools emitting phonons. Although the slower relaxation mechanisms have been extensively investigated, the initial stages still pose a challenge. Experimentally, they defy the resolution of most pump-probe setups, due to the extremely fast sub-100 fs carrier dynamics. Theoretically, massless Dirac fermions represent a novel many-body problem, fundamentally different from Schrödinger fermions. Here we combine pump-probe spectroscopy with a microscopic theory to investigate electron-electron interactions during the early stages of relaxation. We identify the mechanisms controlling the ultrafast dynamics, in particular the role of collinear scattering. This gives rise to Auger processes, including charge multiplication, which is key in photovoltage generation and photodetectors.

Imaging and optical properties of single core-shell GaAs-AlGaAs nanowires

We study the optical properties of a single core-shell GaAs-AlGaAs nanowire (grown by VLS method) using the technique of micro-photoluminescence and spatially-resolved photoluminescence imaging. We observe large linear polarization anisotropy in emission and excitation of nanowires.

Phase separation induced by Au catalysts in ternary InGaAs nanowires.

We report a novel phase separation phenomenon observed in the growth of ternary In(x)Ga(1-x)As nanowires by metalorganic chemical vapor deposition. A spontaneous formation of core-shell nanowires is investigated by cross-sectional transmission electron microscopy, revealing the compositional complexity within the ternary nanowires. It has been found that for In(x)Ga(1-x)As nanowires high precursor flow rates generate ternary In(x)Ga(1-x)As cores with In-rich shells, while low precursor flow rates produce binary GaAs cores with ternary In(x)Ga(1-x)As shells. First-principle calculations combined with thermodynamic considerations suggest that this phenomenon is due to competitive alloying of different group-III elements with Au catalysts, and variations in elemental concentrations of group-III materials in the catalyst under different precursor flow rates. This study shows that precursor flow rates are critical factors for manipulating Au catalysts to produce nanowires of desired composition.

Vertically oriented epitaxial germanium nanowires on silicon substrates using thin germanium buffer layers.

We demonstrate a method to realize vertically oriented Ge nanowires on Si(111) substrates. Ge nanowires were grown by chemical vapor deposition using Au nanoparticles to seed nanowire growth via a vapor-liquid-solid growth mechanism. Rapid oxidation of Si during Au nanoparticle application inhibits the growth of vertically oriented Ge nanowires directly on Si. The present method employs thin Ge buffer layers grown at low temperature less than 600 degrees C to circumvent the oxidation problem. By using a thin Ge buffer layer with root-mean-square roughness of approximately 2 nm, the yield of vertically oriented Ge nanowires is as high as 96.3%. This yield is comparable to that of homoepitaxial Ge nanowires. Furthermore, branched Ge nanowires could be successfully grown on these vertically oriented Ge nanowires by a secondary seeding technique. Since the buffer layers are grown under moderate conditions without any high temperature processing steps, this method has a wide process window highly suitable for Si-based microelectronics.

CdS/CdSe lateral heterostructure nanobelts by a two-step physical vapor transport method.

The two-dimensional heterostructure nanobelts with a central CdSe region and lateral CdS structures are synthesized by a two-step physical vapor transport method. The large growth rate difference between lateral CdS structures on both +/- (0001) sides of the CdSe region is found. The growth anisotropy is discussed in terms of the polar nature of the side +/- (0001) surfaces of CdSe. High-resolution transmission electron microscopy reveals the CdSe central region covered with non-uniform CdS layer/islands. From micro-photoluminescence measurements, a systematic blueshift of emission energy from the central CdSe region in accordance with the increase of lateral CdS growth temperature is observed. This result indicates that the intermixing rate in the CdSe region with CdS increases with the increase of lateral CdS growth temperature. In conventional CdSSe ternary nanostructures, morphology and emission wavelength were correlated parameters. However, the morphology and emission wavelength are independently controllable in the CdS/CdSe lateral heterostructure nanobelts. This structure is attractive for applications in visible optoelectronic devices.

Novel growth and properties of GaAs nanowires on Si substrates.

Straight, vertically aligned GaAs nanowires were grown on Si(111) substrates coated with thin GaAs buffer layers. We find that the V/III precursor ratio and growth temperature are crucial factors influencing the morphology and quality of buffer layers. A double layer structure, consisting of a thin initial layer grown at low V/III ratio and low temperature followed by a layer grown at high V/III ratio and high temperature, is crucial for achieving straight, vertically aligned GaAs nanowires on Si(111) substrates. An in situ annealing step at high temperature after buffer layer growth improves the surface and structural properties of the buffer layer, which further improves the morphology of the GaAs nanowire growth. Through such optimizations we show that vertically aligned GaAs nanowires can be fabricated on Si(111) substrates and achieve the same structural and optical properties as GaAs nanowires grown directly on GaAs(111)B substrates.

Unexpected benefits of rapid growth rate for III-V nanowires.

In conventional planar growth of bulk III-V materials, a slow growth rate favors high crystallographic quality, optical quality, and purity of the resulting material. Surprisingly, we observe exactly the opposite effect for Au-assisted GaAs nanowire growth. By employing a rapid growth rate, the resulting nanowires are markedly less tapered, are free of planar crystallographic defects, and have very high purity with minimal intrinsic dopant incorporation. Importantly, carrier lifetimes are not adversely affected. These results reveal intriguing behavior in the growth of nanoscale materials, and represent a significant advance toward the rational growth of nanowires for device applications.

Evolution of Wurtzite Structured GaAs Shells Around InAs Nanowire Cores.

GaAs was radially deposited on InAs nanowires by metal-organic chemical vapor deposition and resultant nanowire heterostructures were characterized by detailed electron microscopy investigations. The GaAs shells have been grown in wurtzite structure, epitaxially on the wurtzite structured InAs nanowire cores. The fundamental reason of structural evolution in terms of material nucleation and interfacial structure is given.

Vertically standing Ge nanowires on GaAs(110) substrates.

The growth of epitaxial Ge nanowires is investigated on (100), (111) B and (110) GaAs substrates in the growth temperature range from 300 to 380 °C. Unlike epitaxial Ge nanowires on Ge or Si substrates, Ge nanowires on GaAs substrates grow predominantly along the [Formula: see text] direction. Using this unique property, vertical [Formula: see text] Ge nanowires epitaxially grown on GaAs(110) surface are realized. In addition, these Ge nanowires exhibit minimal tapering and uniform diameters, regardless of growth temperatures, which is an advantageous property for device applications. Ge nanowires growing along the [Formula: see text] directions are particularly attractive candidates for forming nanobridge devices on conventional (100) surfaces.

Twin-free uniform epitaxial GaAs nanowires grown by a two-temperature process.

We demonstrate vertically aligned epitaxial GaAs nanowires of excellent crystallographic quality and optimal shape, grown by Au nanoparticle-catalyzed metalorganic chemical vapor deposition. This is achieved by a two-temperature growth procedure, consisting of a brief initial high-temperature growth step followed by prolonged growth at a lower temperature. The initial high-temperature step is essential for obtaining straight, vertically aligned epitaxial nanowires on the (111)B GaAs substrate. The lower temperature employed for subsequent growth imparts superior nanowire morphology and crystallographic quality by minimizing radial growth and eliminating twinning defects. Photoluminescence measurements confirm the excellent optical quality of these two-temperature grown nanowires. Two mechanisms are proposed to explain the success of this two-temperature growth process, one involving Au nanoparticle-GaAs interface conditions and the other involving melting-solidification temperature hysteresis of the Au-Ga nanoparticle alloy.

Dynamics of strongly degenerate electron-hole plasmas and excitons in single InP nanowires.

Low-temperature time-resolved photoluminescence spectroscopy is used to probe the dynamics of photoexcited carriers in single InP nanowires. At early times after pulsed excitation, the photoluminescence line shape displays a characteristic broadening, consistent with emission from a degenerate, high-density electron-hole plasma. As the electron-hole plasma cools and the carrier density decreases, the emission rapidly converges toward a relatively narrow band consistent with free exciton emission from the InP nanowire. The free excitons in these single InP nanowires exhibit recombination lifetimes closely approaching that measured in a high-quality epilayer, suggesting that in these InP nanowires, electrons and holes are relatively insensitive to surface states. This results in higher quantum efficiencies than other single-nanowire systems as well as significant state-filling and band gap renormalization, which is observed at high electron-hole carrier densities.

Resonant excitation and imaging of nonequilibrium exciton spins in single core-shell GaAs-AlGaAs nanowires.

Nonequilibrium spin distributions in single GaAs/AlGaAs core-shell nanowires are excited using resonant polarized excitation at 10 K. At all excitation energies, we observe strong photoluminescence polarization due to suppressed radiative recombination of excitons with dipoles aligned perpendicular to the nanowire. Excitation resonances are observed at 1- or 2-LO phonon energies above the exciton ground states. Using rate equation modeling, we show that, at the lowest energies, strongly nonequilibrium spin distributions are present and we estimate their spin relaxation rate.