Pascal Hille

Germanium doping of self-assembled GaN nanowires grown by plasma-assisted molecular beam epitaxy

Germanium doping of GaN nanowires grown by plasma-assisted molecular beam epitaxy on Si(111) substrates is studied. Time of flight secondary ion mass spectrometry measurements reveal a constant Ge-concentration along the growth axis. A linear relationship between the applied Ge-flux and the resulting ensemble Ge-concentration with a maximum content of 3.3×1020 cm−3 is extracted from energy dispersive X-ray spectroscopy measurements and confirmed by a systematic increase of the conductivity with Ge-concentration in single nanowire measurements. Photoluminescence analysis of nanowire ensembles and single nanowires reveals an exciton localization energy of 9.5 meV at the neutral Ge-donor. A Ge-related emission band at energies above 3.475 eV is found that is assigned to a Burstein-Moss shift of the excitonic emission.

UV Photosensing Characteristics of Nanowire-Based GaN/AlN Superlattices

We have characterized the photodetection capabilities of single GaN nanowires incorporating 20 periods of AlN/GaN:Ge axial heterostructures enveloped in an AlN shell. Transmission electron microscopy confirms the absence of an additional GaN shell around the heterostructures. In the absence of a surface conduction channel, the incorporation of the heterostructure leads to a decrease of the dark current and an increase of the photosensitivity. A significant dispersion in the magnitude of dark currents for different single nanowires is attributed to the coalescence of nanowires with displaced nanodisks, reducing the effective length of the heterostructure. A larger number of active nanodisks and AlN barriers in the current path results in lower dark current and higher photosensitivity and improves the sensitivity of the nanowire to variations in the illumination intensity (improved linearity). Additionally, we observe a persistence of the photocurrent, which is attributed to a change of the resistance of the overall structure, particularly the GaN stem and cap sections. As a consequence, the time response is rather independent of the dark current.

Intraband absorption in self-assembled Ge-doped GaN/AlN nanowire heterostructures.

We report the observation of transverse-magnetic-polarized infrared absorption assigned to the s-p(z) intraband transition in Ge-doped GaN/AlN nanodisks (NDs) in self-assembled GaN nanowires (NWs). The s-p(z) absorption line experiences a blue shift with increasing ND Ge concentration and a red shift with increasing ND thickness. The experimental results in terms of interband and intraband spectroscopy are compared to theoretical calculations of the band diagram and electronic structure of GaN/AlN heterostructured NWs, accounting for their three-dimensional strain distribution and the presence of surface states. From the theoretical analysis, we conclude that the formation of an AlN shell during the heterostructure growth applies a uniaxial compressive strain which blue shifts the interband optical transitions but has little influence on the intraband transitions. The presence of surface states with density levels expected for m-GaN plane charge-deplete the base of the NWs but is insufficient to screen the polarization-induced internal electric field in the heterostructures. Simulations show that the free-carrier screening of the polarization-induced internal electric field in the NDs is critical to predicting the photoluminescence behavior. The intraband transitions, on the other hand, are blue-shifted due to many-body effects, namely, the exchange interaction and depolarization shift, which exceed the red shift induced by carrier screening.

InGaN/GaN nanowires as a new platform for photoelectrochemical sensors – detection of NADH

InGaN/GaN nanowire heterostructures are presented as nanophotonic probes for the light-triggered photoelectrochemical detection of NADH. We demonstrate that photogenerated electron-hole pairs give rise to a stable anodic photocurrent whose potential- and pH-dependences exhibit broad applicability. In addition, the simultaneous measurement of the photoluminescence provides an additional tool for the analysis and evaluation of light-triggered reaction processes at the nanostructured interface. InGaN/GaN nanowire ensembles can be excited over a wide wavelength range, which avoids interferences of the photoelectrochemical response by absorption properties of the compounds to be analyzed by adjusting the excitation wavelength. The photocurrent of the nanostructures shows an NADH-dependent magnitude. The anodic current increases with rising analyte concentration in a range from 5µM to 10mM, at a comparatively low potential of 0mV vs. Ag/AgCl. Here, the InGaN/GaN nanowires reach high sensitivities of up to 91µAmM-1cm-2 (in the linear range) and provide a good reusability for repetitive NADH detection. These results demonstrate the potential of InGaN/GaN nanowire heterostructures for the defined conversion of this analyte paving the way for the realization of light-switchable sensors for the analyte or biosensors by combination with NADH producing enzymes.

Long-lived excitons in GaN/AlN nanowire heterostructures

GaN/AlN nanowire heterostructures can display photoluminescence (PL) decay times on the order of microseconds that persist up to room temperature. Doping the GaN nanodisk insertions with Ge can reduce these PL decay times by two orders of magnitude. These phenomena are explained by the three-dimensional electric field distribution within the GaN nanodisks, which has an axial component in the range of a few MV/cm associated to the spontaneous and piezoelectric polarization, and a radial piezoelectric contribution associated to the shear components of the lattice strain. At low dopant concentrations, a large electron-hole separation in both the axial and radial directions is present. The relatively weak radial electric fields, which are about one order of magnitude smaller than the axial fields, are rapidly screened by doping. This bidirectional screening leads to a radial and axial centralization of the hole underneath the electron, and consequently, to large decreases in PL decay times, in addition to luminescence blue shifts.

Probing the Internal Electric Field in GaN/AlGaN Nanowire Heterostructures

We demonstrate the direct analysis of polarization-induced internal electric fields in single GaN/Al0.3Ga0.7N nanodiscs embedded in GaN/AlN nanowire heterostructures. Superposition of an external electric field with different polarity results in compensation or enhancement of the quantum-confined Stark effect in the nanodiscs. By field-dependent analysis of the low temperature photoluminescence energy and intensity, we prove the [0001̅]-polarity of the nanowires and determine the internal electric field strength to 1.5 MV/cm.

Screening of the quantum-confined Stark effect in AlN/GaN nanowire superlattices by germanium doping

We report on electrostatic screening of polarization-induced internal electric fields in AlN/GaN nanowire heterostructures with germanium-doped GaN nanodiscs embedded between AlN barriers. The incorporation of germanium at concentrations above 1020 cm–3 shifts the photoluminescence emission energy of GaN nanodiscs to higher energies accompanied by a decrease of the photoluminescence decay time. At the same time, the thickness-dependent shift in emission energy is significantly reduced. In spite of the high donor concentration, a degradation of the photoluminescence properties is not observed.

Effect of Water Vapor and Surface Morphology on the Low Temperature Response of Metal Oxide Semiconductor Gas Sensors

In this work the low temperature response of metal oxide semiconductor gas sensors is analyzed. Important characteristics of this low-temperature response are a pronounced selectivity to acid- and base-forming gases and a large disparity of response and recovery time constants which often leads to an integrator-type of gas response. We show that this kind of sensor performance is related to the trend of semiconductor gas sensors to adsorb water vapor in multi-layer form and that this ability is sensitively influenced by the surface morphology. In particular we show that surface roughness in the nanometer range enhances desorption of water from multi-layer adsorbates, enabling them to respond more swiftly to changes in the ambient humidity. Further experiments reveal that reactive gases, such as NO2 and NH3, which are easily absorbed in the water adsorbate layers, are more easily exchanged across the liquid/air interface when the humidity in the ambient air is high.

Bias-Controlled Spectral Response in GaN/AlN Single-Nanowire Ultraviolet Photodetectors

We present a study of GaN single-nanowire ultraviolet photodetectors with an embedded GaN/AlN superlattice. The heterostructure dimensions and doping profile were designed in such a way that the application of positive or negative bias leads to an enhancement of the collection of photogenerated carriers from the GaN/AlN superlattice or from the GaN base, respectively, as confirmed by electron beam-induced current measurements. The devices display enhanced response in the ultraviolet A (≈ 330-360 nm)/B (≈ 280-330 nm) spectral windows under positive/negative bias. The result is explained by correlation of the photocurrent measurements with scanning transmission electron microscopy observations of the same single nanowire and semiclassical simulations of the strain and band structure in one and three dimensions.

Photoluminescence Probing of Complex H2O Adsorption on InGaN/GaN Nanowires

We demonstrate that the complex adsorption behavior of H2O on InGaN/GaN nanowire arrays is directly revealed by their ambient-dependent photoluminescence properties. Under low-humidity, ambient-temperature, and low-excitation-light conditions, H2O adsorbates cause a quenching of the photoluminescence. In contrast, for high humidity levels, elevated temperature, and high excitation intensity, H2O adsorbates act as efficient photoluminescence enhancers. We show that this behavior, which can only be detected due to the low operation temperature of the InGaN/GaN nanowires, can be explained on the basis of single H2O adsorbates forming surface recombination centers and multiple H2O adsorbates forming surface passivation layers. Reversible creation of such passivation layers is induced by the photoelectrochemical splitting of adsorbed water molecules and by the interaction of reactive H3O+ and OH- ions with photoactivated InGaN surfaces. Due to electronic coupling of adsorbing molecules with photoactivated surfaces, InGaN/GaN nanowires act as sensitive nanooptical probes for the analysis of photoelectrochemical surface processes.