Optical absorption of composition-tunable InGaAs nanowire arrays.

InGaAs nanowire (NW) arrays have emerged as important active materials in future photovoltaic and photodetector applications, due to their excellent electronic properties and tunable band gap. Here, we report a systematic investigation of the optical absorption characteristics of composition-tunable vertical InGaAs NW arrays. Using finite-difference time-domain simulations we first study the effect of variable composition (Ga-molar fraction) and NW array geometry (NW diameter, period, fill factor) on the optical generation rate. NWs with typical diameters in the range of ∼100-250 nm lead to generation rates higher than the equivalent bulk case for moderate fill factors (NW period of ∼0.3-0.8 µm), while slightly smaller fill factors and increased diameters are required to maintain high generation rates at increased Ga-molar fraction. The optical absorption was further measured using spectrally resolved ultraviolet-visible-near-infrared (UV-vis-NIR) spectroscopy on NW arrays transferred to transparent substrates. Interestingly, large variations in Ga-molar fraction (0 < x(Ga) < 0.5) have a negligible influence, while minute changes in NW diameter of less than ±20 nm affect the absorption spectra very strongly, leading to pronounced shifts in the peak absorption energies by more than ∼700 meV. These results clearly highlight the much larger sensitivity of the optical absorption behavior to geometric parameters rather than to variations in the electronic band gap of the underlying NW array.

Monolithically Integrated High-ß Nanowire Lasers on Silicon.

Reliable technologies for the monolithic integration of lasers onto silicon represent the holy grail for chip-level optical interconnects. In this context, nanowires (NWs) fabricated using III-V semiconductors are of strong interest since they can be grown site-selectively on silicon using conventional epitaxial approaches. Their unique one-dimensional structure and high refractive index naturally facilitate low loss optical waveguiding and optical recirculation in the active NW-core region. However, lasing from NWs on silicon has not been achieved to date, due to the poor modal reflectivity at the NW-silicon interface. We demonstrate how, by inserting a tailored dielectric interlayer at the NW-Si interface, low-threshold single mode lasing can be achieved in vertical-cavity GaAs-AlGaAs core-shell NW lasers on silicon as measured at low temperature. By exploring the output characteristics along a detection direction parallel to the NW-axis, we measure very high spontaneous emission factors comparable to nanocavity lasers (ß = 0.2) and achieve ultralow threshold pump energies ≤11 pJ/pulse. Analysis of the input-output characteristics of the NW lasers and the power dependence of the lasing emission line width demonstrate the potential for high pulsation rates ≥250 GHz. Such highly efficient nanolasers grown monolithically on silicon are highly promising for the realization of chip-level optical interconnects.

Ultrafast Photodetection in the Quantum Wells of Single AlGaAs/GaAs-Based Nanowires.

We investigate the ultrafast optoelectronic properties of single Al0.3Ga0.7As/GaAs core-shell nanowires. The nanowires contain GaAs-based quantum wells. For a resonant excitation of the quantum wells, we find a picosecond photocurrent which is consistent with an ultrafast lateral expansion of the photogenerated charge carriers. This Dember-effect does not occur for an excitation of the GaAs-based core of the nanowires. Instead, the core exhibits an ultrafast displacement current and a photothermoelectric current at the metal Schottky contacts. Our results uncover the optoelectronic dynamics in semiconductor core-shell nanowires comprising quantum wells, and they demonstrate the possibility to use the low-dimensional quantum well states therein for ultrafast photoswitches and photodetectors.

Demonstration of Confined Electron Gas and Steep-Slope Behavior in Delta-Doped GaAs-AlGaAs Core-Shell Nanowire Transistors.

Strong surface and impurity scattering in III-V semiconductor-based nanowires (NW) degrade the performance of electronic devices, requiring refined concepts for controlling charge carrier conductivity. Here, we demonstrate remote Si delta (δ)-doping of radial GaAs-AlGaAs core-shell NWs that unambiguously exhibit a strongly confined electron gas with enhanced low-temperature field-effect mobilities up to 5 × 10(3) cm(2) V(-1) s(-1). The spatial separation between the high-mobility free electron gas at the NW core-shell interface and the Si dopants in the shell is directly verified by atom probe tomographic (APT) analysis, band-profile calculations, and transport characterization in advanced field-effect transistor (FET) geometries, demonstrating powerful control over the free electron gas density and conductivity. Multigated NW-FETs allow us to spatially resolve channel width- and crystal phase-dependent variations in electron gas density and mobility along single NW-FETs. Notably, dc output and transfer characteristics of these n-type depletion mode NW-FETs reveal excellent drain current saturation and record low subthreshold slopes of 70 mV/dec at on/off ratios >10(4)-10(5) at room temperature.

All optical quantum control of a spin-quantum state and ultrafast transduction into an electric current.

The ability to control and exploit quantum coherence and entanglement drives research across many fields ranging from ultra-cold quantum gases to spin systems in condensed matter. Transcending different physical systems, optical approaches have proven themselves to be particularly powerful, since they profit from the established toolbox of quantum optical techniques, are state-selective, contact-less and can be extremely fast. Here, we demonstrate how a precisely timed sequence of monochromatic ultrafast (~ 2-5 ps) optical pulses, with a well defined polarisation can be used to prepare arbitrary superpositions of exciton spin states in a semiconductor quantum dot, achieve ultrafast control of the spin-wavefunction without an applied magnetic field and make high fidelity read-out the quantum state in an arbitrary basis simply by detecting a strong (~ 2-10 pA) electric current flowing in an external circuit. The results obtained show that the combined quantum state preparation, control and read-out can be performed with a near-unity (≥97%) fidelity.

Electrical control of interdot electron tunneling in a double InGaAs quantum-dot nanostructure.

We employ ultrafast pump-probe spectroscopy to directly monitor electron tunneling between discrete orbital states in a pair of spatially separated quantum dots. Immediately after excitation, several peaks are observed in the pump-probe spectrum due to Coulomb interactions between the photogenerated charge carriers. By tuning the relative energy of the orbital states in the two dots and monitoring the temporal evolution of the pump-probe spectra the electron and hole tunneling times are separately measured and resonant tunneling between the two dots is shown to be mediated both by elastic and inelastic processes. Ultrafast (<5 ps) interdot tunneling is shown to occur over a surprisingly wide bandwidth, up to ∼8 meV, reflecting the spectrum of exciton-acoustic phonon coupling in the system.

Rate-limiting mechanisms in high-temperature growth of catalyst-free InAs nanowires with large thermal stability.

We identify the entire growth parameter space and rate-limiting mechanisms in non-catalytic InAs nanowires (NWs) grown by molecular beam epitaxy. Surprisingly huge growth temperature ranges are found with maximum temperatures close to ~600°C upon dramatic increase of V/III ratio, exceeding by far the typical growth temperature range for catalyst-assisted InAs NWs. Based on quantitative in situ line-of-sight quadrupole mass spectrometry, we determine the rate-limiting factors in high-temperature InAs NW growth by directly monitoring the critical desorption and thermal decomposition processes of InAs NWs. Both under dynamic (growth) and static (no growth, ultra-high vacuum) conditions the (111)-oriented InAs NWs evidence excellent thermal stability at elevated temperatures even under negligible supersaturation. The rate-limiting factor for InAs NW growth is hence dominated by In desorption from the substrate surface. Closer investigation of the group-III and group-V flux dependences on growth rate reveals two apparent growth regimes, an As-rich and an In-rich regime defined by the effective As/In flux ratio, and maximum achievable growth rates of > 6 µm h(-1). The unique features of high-T growth and excellent thermal stability provide the opportunity for operation of InAs-based NW materials under caustic environment and further allow access to temperature regimes suitable for alloying non-catalytic InAs NWs with GaAs.

Local modification of GaAs nanowires induced by laser heating.

GaAs nanowires were heated locally under ambient air conditions by a focused laser beam which led to oxidation and formation of crystalline arsenic on the nanowire surface. Atomic force microscopy, photoluminescence and Raman spectroscopy experiments were performed on the same single GaAs nanowires in order to correlate their structural and optical properties. We show that the local changes of the nanowires act as a barrier for thermal transport which is of interest for thermoelectric applications.

Self-induced growth of vertical free-standing InAs nanowires on Si(111) by molecular beam epitaxy.

We report self-induced growth of vertically aligned (i.e. along the [111] direction), free-standing InAs nanowires on Si(111) substrates by solid-source molecular beam epitaxy. Implementation of an ultrathin amorphous SiO(x) mask on Si(111) facilitated epitaxial InAs nanowire growth, as confirmed by high-resolution x-ray diffraction 2theta-omega scans and transmission electron microscopy. Depending on growth temperature (in the range of 400-520 degrees C) substantial size variation of both nanowire length and diameter was found under preservation of uniform, non-tapered hexagon-shaped geometries. The majority of InAs nanowires exhibited phase-pure zinc blende crystal structure with few defective regions consisting of stacking faults. Photoluminescence spectroscopy at 20 K revealed peak emission of the InAs nanowires at 0.445 eV, which is approximately 30 meV blueshifted with respect to the emission of the bulk InAs reference due to radial quantum confinement effects. These results show a promising route towards integration of well-aligned, high structural quality InAs-based nanowires with the desired aspect ratio and tailored emission wavelengths on an Si platform.

An atomically resolved study of InGaAs quantum dot layers grown with an indium flush step.

In this cross-sectional scanning tunnelling microscopy study we investigate the indium flush method as a means to control the height of self-assembled InGaAs quantum dots and wetting layers. The results show that application of an indium flush step during growth results in flattened dots and a reduced wetting layer of which the height can be precisely controlled by varying the height of the first capping layer.

Quantum interference control of femtosecond, microA current bursts in single GaAs nanowires.

A phase-stable superposition of femtosecond pulses from a compact erbium-doped fiber source and their second harmonic is shown to induce ultrashort approximately microA current bursts in single unbiased GaAs nanowires. Current injection relies on a quantum interference of one- and two-photon absorption pathways. The vector direction of the current is solely dictated by the polarization and relative phase of the harmonically related light components while its power dependence is consistent with a third order optical nonlinearity.

Ge(1-x) Mn(x) clusters: central structural and magnetic building blocks of nanoscale wire-like self-assembly in a magnetic semiconductor.

Controlled nanoscale self-assembly of magnetic entities in semiconductors opens novel perspectives for the tailoring of magnetic semiconductor films and nanostructures with room temperature functionality. We report that a strongly directional self-assembly in growth direction in Mn-alloyed Ge is due to a stacking of individual Ge(1-x)Mn(x) clusters. The clusters represent the relevant entities for the magnetization of the material. They are formed of a core-shell structure displaying a Mn concentration gradient. While the magnetic moments seem to be carried by the shells of the clusters, their core is magnetically inactive.

Photonic crystal nanostructures for optical biosensing applications.

We present the design, fabrication and optical investigation of photonic crystal (PhC) nanocavity drop filters for use as optical biosensors. The resonant cavity mode wavelength and Q-factor are studied as a function of the ambient refractive index and as a function of adsorbed proteins (bovine serum albumin) on the sensor surface. Experiments were performed by evanescent excitation of the cavity mode via a PhC waveguide. This in turn is coupled to a ridge waveguide that allows the introduction of a fluid flow cell on a chip. A response of partial delta lambda/delta c=(4.54+/-0.66)x10(5)nm/M is measured leading to a measured detection limit as good as Delta m=4.0+/-0.6 fg or Delta m/Delta A=(4.9+/-0.7)x10(2)pg/mm(2)in the sensitive area.

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.

Size and environment dependence of surface phonon modes of gallium arsenide nanowires as measured by Raman spectroscopy.

Gallium arsenide nanowires were synthesized by gallium-assisted molecular beam epitaxy. By varying the growth time, nanowires with diameters ranging from 30 to 160 nm were obtained. Raman spectra of the nanowire ensembles were measured. The small linewidth of the optical phonon modes agree with an excellent crystalline quality. A surface phonon mode was also revealed, as a shoulder at lower frequencies of the longitudinal optical mode. In agreement with the theory, the surface mode shifts to lower wavenumbers when the diameter of the nanowires is decreased or the environment dielectric constant increased.

Silicon-on-insulator based nanopore cavity arrays for lipid membrane investigation.

We present the fabrication and characterization of nanopore microcavities for the investigation of transport processes in suspended lipid membranes. The cavities are situated below the surface of silicon-on-insulator (SOI) substrates. Single cavities and large area arrays were prepared using high resolution electron-beam lithography in combination with reactive ion etching (RIE) and wet chemical sacrificial underetching. The locally separated compartments have a circular shape and allow the enclosure of picoliter volume aqueous solutions. They are sealed at their top by a 250 nm thin Si membrane featuring pores with diameters from 2 µm down to 220 nm. The Si surface exhibits excellent smoothness and homogeneity as verified by AFM analysis. As biophysical test system we deposited lipid membranes by vesicle fusion, and demonstrated their fluid-like properties by fluorescence recovery after photobleaching. As clearly indicated by AFM measurements in aqueous buffer solution, intact lipid membranes successfully spanned the pores. The nanopore cavity arrays have potential applications in diagnostics and pharmaceutical research on transmembrane proteins.

Optically probing spin and charge interactions in a tunable artificial molecule.

We optically probe and electrically control a single artificial molecule containing a well defined number of electrons. Charge and spin dependent interdot quantum couplings are probed optically by adding a single electron-hole pair and detecting the emission from negatively charged exciton states. Coulomb- and Pauli-blockade effects are directly observed, and tunnel coupling and electrostatic charging energies are independently measured. The interdot quantum coupling is shown to be mediated by electron tunneling. Our results are in excellent accord with calculations that provide a complete picture of negative excitons and few-electron states in quantum dot molecules.

The role of surface charging during the coadsorption of mercaptohexanol to DNA layers on gold: direct observation of desorption and layer reorientation.

We study the coadsorption of mercaptohexanol onto preimmobilized oligonucleotide layers on gold. Monitoring the position of the DNA relative to the surface by optical means directly shows the mercaptohexanol-induced desorption of DNA and the reorientation of surface-tethered strands in situ and in real time. By simultaneously recording the electrochemical electrode potential, we are able to demonstrate that changes in the layer conformation are predominantly of electrostatic origin and can be reversed by applying external bias to the substrate.

Clustering in a precipitate-free GeMn magnetic semiconductor.

We present the first study relating structural parameters of precipitate-free Ge0.95Mn0.05 films to magnetization data. Nanometer-sized clusters--areas with increased Mn content on substitutional lattice sites compared to the host matrix--are detected in transmission electron microscopy analysis. The films show no overall spontaneous magnetization at all down to 2 K. The TEM and magnetization results are interpreted in terms of an assembly of superparamagnetic moments developing in the dense distribution of clusters. Each cluster individually turns ferromagnetic below an ordering temperature which depends on its volume and Mn content.

Direct observation of controlled coupling in an individual quantum dot molecule.

We report the direct observation of quantum coupling in individual quantum dot molecules and its manipulation using static electric fields. A pronounced anticrossing of different excitonic transitions is observed as the electric field is tuned. A comparison of our experimental results with theory shows that the observed anticrossing occurs between excitons with predominant spatially direct and indirect character and reveals a field driven transition of the nature of the molecular ground state exciton wave function. Finally, the interdot quantum coupling strength is deduced optically and its dependence on the interdot separation is calculated.