| 1. |
- Philipps, Jan M., et al.
(author)
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Photoelectrochemical response of GaN, InGaN, and GaNP nanowire ensembles
- 2018
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In: Journal of Applied Physics. - : AMER INST PHYSICS. - 0021-8979 .- 1089-7550. ; 123:17
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Journal article (peer-reviewed)abstract
- The photoelectrochemical responses of GaN, GaNP, and InGaN nanowire ensembles are investigated by the electrical bias dependent photoluminescence, photocurrent, and spin trapping experiments. The results are explained in the frame of the surface band bending model. The model is sufficient for InGaN nanowires, but for GaN nanowires the electrochemical etching processes in the anodic regime have to be considered additionally. These processes lead to oxygen rich surface (GaxOy) conditions as evident from energy dispersive X-ray fluorescence. For the GaNP nanowires, a bias dependence of the carrier transfer to the electrolyte is not reflected in the photoluminescence response, which is tentatively ascribed to a different origin of radiative recombination in this material as compared to (In) GaN. The corresponding consequences for the applications of the materials for water splitting or pH-sensing will be discussed. Published by AIP Publishing.
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| 2. |
- Philipps, Jan M., et al.
(author)
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Recharging behavior of nitrogen-centers in ZnO
- 2014
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In: Journal of Applied Physics. - : AIP Publishing. - 0021-8979 .- 1089-7550. ; 116:063701
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Journal article (peer-reviewed)abstract
- Electron Paramagnetic Resonance was used to study N2-centers in ZnO, which show a 5-line spectrum described by the hyperfine interaction of two nitrogen nuclei (nuclear spin I = 1, 99.6% abundance). The recharging of this center exhibits two steps, a weak onset at about 1.4 eV and a strongly increasing signal for photon energies above 1.9 eV. The latter energy coincides with the recharging energy of NO centers (substitutional nitrogen atoms on oxygen sites). The results indicate that the N2-centers are deep level defects and therefore not suitable to cause significant hole-conductivity at room temperature.
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| 3. |
- Philipps, Jan M., et al.
(author)
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Study of the carrier transfer across the GaNP nanowire electrolyte interface by electron paramagnetic spin trapping
- 2017
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In: Applied Physics Letters. - : AMER INST PHYSICS. - 0003-6951 .- 1077-3118. ; 110:22
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Journal article (peer-reviewed)abstract
- We investigate the transfer of photoexcited charge carriers from GaP and GaNP nanowires to an electrolyte by bias-dependent photocurrent and electron paramagnetic resonance experiments using 5,5-dimethyl-1-pyrroline-N-oxide as a spin trap. The results of the latter show that hydroxyl radicals are created over the entire applied bias range from -1000mV to +1300mV by hole transfer. In contrast, the photocurrent changes from cathodic to anodic at the open circuit potential of the three-electrode setup with the nanowire sample acting as the working electrode. The experiments show that the photoelectrochemical response of GaNP nanowires is significantly stronger compared to that of the GaP nanowires. Published by AIP Publishing.
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| 4. |
- Chen, Shula
(author)
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Excitonic Effects and Energy Upconversion in Bulk and Nanostructured ZnO
- 2014
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Doctoral thesis (other academic/artistic)abstract
- Zinc Oxide (ZnO), a II-VI wurtzite semiconductor, has been drawing enormous research interest for decades as an electronic material for numerous applications. It has a wide and direct band gap of 3.37eV and a large exciton binding energy of 60 meV that leads to intense free exciton (FX) emission at room temperature. As a result, ZnO is currently considered among the key materials for UV light emitting devices with tailored dimensionality and solid state white lighting. Full exploration of ZnO in various applications requires detailed knowledge of its fundamental and materialrelated properties, which remains incomplete. The research work summarized in this thesis addresses a selection of open issues on optical properties of ZnO based on (but not limited to) detailed time-resolved photoluminescence (PL) and magneto-optical studies of various excitonic transitions as specified below.Papers 1 and 2 analyze recombination dynamics of FX and donor bound excitons (DX) in bulk and tetrapod ZnO with the aim to evaluate contributions of radiative and nonradiative carrier recombination processes in the total carrier lifetime. We show that changes in relative contributions of these processes in “bulk” and near-surface areas are responsible for bi-exponential exciton decays typically observed in these materials. The radiative FX lifetime is found to be relatively long, i.e. >1 ns at 77 K and >14 ns at room temperature. In the case of DX, the radiative lifetime depends on exciton localization. Radiative recombination is concluded to dominate the exciton dynamics in “bulk regions” of high-quality materials. It leads to appearance of a slow component in the decays of no-phonon (NP) FX and DX lines, which also determines the dynamics of the longitudinal optical (LO) phonon-assisted and two-electronsatellite DX transitions. On the other hand, the fast component of the exciton decays is argued to be a result of surface recombination.Paper 3 evaluates exciton-phonon coupling in bulk and tetrapod ZnO. It is found that, in contrast to bulk ZnO, the NP FX emission in ZnO tetrapods is weak as compared with the LO phonon assisted transitions. We show that the observed high intensity of the FX-1LO emission does not reflect enhanced exciton-phonon coupling in nanostructured ZnO. Instead, it is a result of stronger suppression of the NP FX emission in faceted regions of the tetrapods as revealed from spatially resolved cathodoluminescence (CL) studies. This is attributed to enhanced re-absorption due to multiple internal reflections, which become especially pronounced in the vicinity of the FX resonance.Effects of exciton-photon coupling on light propagation through the ZnO media are studied in Papers 4 and 5. By employing the time-of-flight spectroscopy, in Paper 4 we demonstrate that the group velocity of laser pulses propagating through bulk ZnO can be slowed down to as low as 2044 km/s when photon energies approach the optical absorption edge of the material. The magnitude of this decrease can be manipulated by changing light polarization. In Paper 5 we show that the observed slow-down is caused by the formation of free exciton-polaritons and is determined by their dispersion. On the other hand, contributions of DX polaritons become important only in the proximity to their corresponding resonances.Excitonic effects can also be utilized to investigate fundamental properties and defect formation in ZnO. In Paper 6, we employ DX to study magneto-optical properties of the B valence band (B-VB) states as well as dynamics of inter-VB energy relaxation. We show that PL decays of the emissions involving the B-VB holes are faster than that of their counterparts involving the A-VB holes, which is interpreted as being due to energy relaxation of the holes assisted by acoustic phonons. Values of effective Landé g factors for the B-VB holes are also accurately determined. In paper 7, we uncover the origin of a new class of bound exciton lines detected within the nearband-edge region. Based on their magnetic behavior we show that these lines do not stem from DXs bound to either ionized or neutral donors but instead arise from an exciton bound to an isoelectronic center with a hole-attractive local potential.In Paper 8, DX emissions are used to monitor energy upconversion in bulk and nanorod ZnO. Based on excitation power dependent PL measurements performed with different energies of excitation photons, the physical processes responsible for the upconversion are assigned to two-photon-absorption (TPA) via virtual states and twostep TPA (TS-TPA) via real states. In the former case the observed threshold energy for the TPA process is larger than half of that for one-photon absorption across the bandgap, which can be explained by the different selection rules between the involved optical transitions. It is also concluded that the TS-TPA process occurs via a defect/impurity with an energy level lying within 1.14-1.56 eV from one of the band edges, likely a zinc vacancy.
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| 5. |
- Nakamura, Hisao, et al.
(author)
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Probing embedded topological modes in bulk-like GeTe-Sb2Te3 heterostructures
- 2020
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In: Scientific Reports. - : Springer Science and Business Media LLC. - 2045-2322. ; 10
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Journal article (peer-reviewed)abstract
- The interface between topological and normal insulators hosts metallic states that appear due to the change in band topology. While topological states at a surface, i.e., a topological insulator-air/vacuum interface, have been studied intensely, topological states at a solid-solid interface have been less explored. Here we combine experiment and theory to study such embedded topological states (ETSs) in heterostructures of GeTe (normal insulator) and Sb 2Te 3 (topological insulator). We analyse their dependence on the interface and their confinement characteristics. First, to characterise the heterostructures, we evaluate the GeTe-Sb2Te3 band offset using X-ray photoemission spectroscopy, and chart the elemental composition using atom probe tomography. We then use first-principles to independently calculate the band offset and also parametrise the band structure within a four-band continuum model. Our analysis reveals, strikingly, that under realistic conditions, the interfacial topological modes are delocalised over many lattice spacings. In addition, the first-principles calculations indicate that the ETSs are relatively robust to disorder and this may have practical ramifications. Our study provides insights into how to manipulate topological modes in heterostructures and also provides a basis for recent experimental findings [Nguyen et al. Sci. Rep. 6, 27716 (2016)] where ETSs were seen to couple over thick layers.
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| 6. |
- Stehr, Jan Eric, et al.
(author)
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Magneto-optical properties of Cr3+ in beta-Ga2O3
- 2021
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In: Applied Physics Letters. - : AIP Publishing. - 0003-6951 .- 1077-3118. ; 119:5
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Journal article (peer-reviewed)abstract
- beta-Ga2O3 is a wide bandgap semiconductor that is attractive for various applications, including power electronics and transparent conductive electrodes. Its properties can be strongly affected by transition metal impurities commonly present during the growth such as Cr. In this Letter, we determine the electronic structure of Cr3+ by performing a correlative study of magneto-photoluminescence (magneto-PL) and electron paramagnetic resonance. We unambiguously prove that the so-called R-1 and R-2 PL lines at around 1.79eV originate from an internal transition between the first excited state (E-2) and the (4)A(2) ground state of Cr3+. The center is concluded to have monoclinic local symmetry and exhibits a large zero-field splitting (similar to 147 mu eV) of the ground state, which can be directly measured from the fine structure of the R1 transition. Furthermore, g-values of the first excited state are accurately determined as g(a) = 1.7, g(b) = 1.5, and g(c*) = 2.1. Our results advance our understanding of the electronic structure of Cr in beta-Ga2O3 and provide a spectroscopic signature of this common residual impurity. (C) 2021 Author(s).
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