Martin Heiss

Single-nanowire solar cells beyond the Shockley-Queisser limit

Light management is of great importance in photovoltaic cells, as it determines the fraction of incident light entering the device. An optimal p–n junction combined with optimal light absorption can lead to a solar cell efficiency above the Shockley–Queisser limit. Here, we show how this is possible by studying photocurrent generation for a single core–shell p–i–n junction GaAs nanowire solar cell grown on a silicon substrate. At 1 sun illumination, a short-circuit current of 180 mA cm –2 is obtained, which is more than one order of magnitude higher than that predicted from the Lambert–Beer law. The enhanced light absorption is shown to be due to a light-concentrating property of the standing nanowire, as shown by photocurrent maps of the device. The results imply new limits for the maximum efficiency obtainable with III–V based nanowire solar cells under 1 sun illumination.

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.

Impact of surfaces on the optical properties of GaAs nanowires

The effect of surfaces on the optical properties of GaAs nanowires is evidenced by comparing nanowires with or without an AlGaAs capping shell as a function of the diameter. We find that the optical properties of unpassivated nanowires are governed by Fermi-level pinning, whereas, the optical properties of passivated nanowires are mainly governed by surface recombinations. Finally, we measure a surface recombination velocity of 3 x 10(3) cm s(-1) one order of magnitude lower than values previously reported for (110) GaAs surfaces. These results will serve as guidance for the application of nanowires in solar cell and light emitting devices.

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.

Polarity Assignment in ZnTe, GaAs, ZnO, and GaN-AlN Nanowires from Direct Dumbbell Analysis

Aberration corrected scanning transmission electron microscopy (STEM) with high angle annular dark field (HAADF) imaging and the newly developed annular bright field (ABF) imaging are used to define a new guideline for the polarity determination of semiconductor nanowires (NWs) from binary compounds in two extreme cases: (i) when the dumbbell is formed with atoms of similar mass (GaAs) and (ii) in the case where one of the atoms is extremely light (N or O: ZnO and GaN/AlN). The theoretical fundaments of these procedures allow us to overcome the main challenge in the identification of dumbbell polarity. It resides in the separation and identification of the constituent atoms in the dumbbells. The proposed experimental via opens new routes for the fine characterization of nanostructures, e.g., in electronic and optoelectronic fields, where the polarity is crucial for the understanding of their physical properties (optical and electronic) as well as their growth mechanisms.

Three-Dimensional Multiple-Order Twinning of Self-Catalyzed GaAs Nanowires on Si Substrates

In this paper we introduce a new paradigm for nanowire growth that explains the unwanted appearance of parasitic nonvertical nanowires. With a crystal structure polarization analysis of the initial stages of GaAs nanowire growth on Si substrates, we demonstrate that secondary seeds form due to a three-dimensional twinning phenomenon. We derive the geometrical rules that underlie the multiple growth directions observed experimentally. These rules help optimizing nanowire array devices such as solar or water splitting cells or of more complex hierarchical branched nanowire devices.

Untangling the Electronic Band Structure of Wurtzite GaAs Nanowires by Resonant Raman Spectroscopy

In semiconductor nanowires, the coexistence of wurtzite and zinc-blende phases enables the engineering of the electronic structure within a single material. This presupposes an exact knowledge of the band structure in the wurtzite phase. We demonstrate that resonant Raman scattering is a important tool to probe the electronic structure of novel materials. Exemplarily, we use this technique to elucidate the band structure of wurtzite GaAs at the Γ point. Within the experimental uncertainty we find that the free excitons at the edge of the wurtzite and the zinc-blende band gap exhibit equal energies. For the first time we show that the conduction band minimum in wurtzite GaAs is of Γ(7) symmetry, meaning a small effective mass. We further find evidence for a light-hole-heavy-hole splitting of 103 meV at 10 K.

Suppression of three dimensional twinning for a 100% yield of vertical GaAs nanowires on silicon

Multiple seed formation by three-dimensional twinning at the initial stages of growth explains the manifold of orientations found when self-catalyzed GaAs nanowires grow on silicon. This mechanism can be tuned as a function of the growth conditions by changing the relative size between the GaAs seed and the Ga droplet. We demonstrate how growing under high V/III ratio results in a 100% yield of vertical nanowires on silicon(111). These results open up the avenue towards the efficient integration of III-V nanowire arrays on the silicon platform.

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.

Photonic–Plasmonic Coupling of GaAs Single Nanowires to Optical Nanoantennas

We successfully demonstrate the plasmonic coupling between metal nanoantennas and individual GaAs nanowires (NWs). In particular, by using dark-field scattering and second harmonic excitation spectroscopy in partnership with analytical and full-vector FDTD modeling, we demonstrate controlled electromagnetic coupling between individual NWs and plasmonic nanoantennas with gap sizes varied between 90 and 500 nm. The significant electric field enhancement values (up to 20×) achieved inside the NW-nanoantennas gap regions allowed us to tailor the nonlinear optical response of NWs by engineering the plasmonic near-field coupling regime. These findings represent an initial step toward the development of coupled metal-semiconductor resonant nanostructures for the realization of next generation solar cells, detectors, and nonlinear optical devices with reduced footprints and energy consumption.