Jörg Teubert

Bias-enhanced optical pH response of group III-nitride nanowires.

We show that the photoluminescence intensity of GaN and InGaN nanowires in electrolytes sensitively responds to variations of the pH value and the applied bias. The realization of an electrochemical working point allows pH detection with a resolution better than 0.05 pH. The observed effects are attributed to bias-dependent nonradiative recombination processes competing with interband transitions. The results show that group III-nitride nanowires are excellently suited as nanophotonic pH sensor elements.

GaN nanodiscs embedded in nanowires as optochemical transducers

The photoluminescence (PL) response of GaN/AlGaN nanowire heterostructures (NWHs) to hydrogen and oxygen between room temperature and 300 °C is reported. Exposure of Pt-coated NWHs to H2 leads to an increase of the PL intensity attributed to the suppression of surface recombination by local dipole fields of adsorbed atomic hydrogen. When exposed to O2, uncoated NWHs show a decrease in PL intensity that is assigned to enhanced non-radiative recombination. The detection limits are below 5 ppm at 150 °C.

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.

Carrier confinement in GaN/AlxGa1−xN nanowire heterostructures (0<x≤1)

The three dimensional carrier confinement in GaN nanodiscs embedded in GaN/AlGaN nanowires and its effect on their photoluminescence properties is analyzed for Al concentrations between x = 0.08 and 1. Structural analysis by high resolution transmission electron microscopy reveals the presence of a lateral AlGaN shell due to a composition dependent lateral growth rate of the barrier material. The structural properties are used as input parameters for three dimensional numerical simulations of the confinement which show that the presence of the AlGaN shell has to be considered to explain the observed dependence of the emission energy on the Al concentration in the barrier. The simulations reveal that the maximum in the emission energy for x ~ 30% is assigned to the smallest lateral strain gradient and consequently the lowest radial internal electric fields in the nanodiscs. Higher Al-concentrations in the barrier cause high radial electric fields that can overcome the exciton binding energy and result in substantially reduced emission intensities. Effects of polarization-induced axial internal electric fields on the photoluminescence characteristics have been investigated using nanowire samples with nanodisc heights ranging between 1.2 nm and 3.5 nm at different Al concentrations. The influence of the quantum confined Stark effect is significantly reduced compared to GaN/AlGaN quantum well structures which is attributed to the formation of misfit dislocations at the heterointerfaces which weakens the internal electric polarization fields.

Electrochemical properties of GaN nanowire electrodes—influence of doping and control by external bias

We report on the electrochemical characteristics of GaN nanowire (NW) ensembles grown by plasma-assisted molecular beam epitaxy on Si111 substrates and on the influence of Si and Mg doping. The NW electrochemical properties in terms of surface capacitance (C(S)), surface resistance (R(S)) are extracted from electrochemical impedance spectra. While Mg doping of GaN NWs does not cause a significant variation of these quantities, an increase of the Si concentration leads to an increase of C(S) and a simultaneous decrease of R(S), indicating the presence of charge carriers in the NWs. According to the extracted values for R(S) and C(S) the NWs are classified into resistive and conductive. For conductive NWs charge transfer to a ferricyanide redox couple in the electrolyte is demonstrated and the ensemble average of the flatband voltage was determined. Variation of the lateral surface potential due to application of an external bias via the electrolyte is demonstrated.

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.

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.

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.

Radical formation at the gallium nitride nanowire–electrolyte interface by photoactivated charge transfer

We investigated the transfer of photogenerated charge carriers from GaN nanowires into a surrounding electrolyte by electron paramagnetic resonance (EPR) and fluorescence spectroscopy. Using 5,5-dimethyl-1-pyrroline-N-oxide (DMPO) as a spin trap we find that the formation of hydroxyl radicals dominates in acidic, neutral and moderately basic environments, while in an electrolyte with a pH of 13.5 the superoxide formation becomes detectable. We explain the two processes considering the redox potentials for radical formation in the electrolyte as well as the positions of the conduction and valence bands. The role of surface band bending and surface states in the semiconductor is discussed.