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- ItemTunable Circular Dichroism by Photoluminescent Moiré Gratings(Weinheim : Wiley-VCH, 2020) Aftenieva, Olha; Schnepf, Max; Mehlhorn, Börge; König, Tobias A.F.In nanophotonics, there is a current demand for ultrathin, flexible nanostructures that are simultaneously easily tunable, demonstrate a high contrast, and have a strong response in photoluminescent polarization. In this work, the template-assisted self-assembly of water-dispersed colloidal core–shell quantum dots into 1D light-emitting sub-micrometer gratings on a flexible substrate is demonstrated. Combining such structures with a light-absorbing metallic counterpart by simple stacking at various angles results in a tunable Moiré pattern with strong lateral contrast. Furthermore, a combination with an identical emitter-based grating leads to a chiroptical effect with a remarkably high degree of polarization of 0.72. Such a structure demonstrates direct circular polarized photoluminescence, for the first time, without a need for an additional chiral template as an intermediary. The suggested approach allows for reproducible, large-area manufacturing at reasonable costs and is of potential use for chiroptical sensors, photonic circuit applications, or preventing counterfeit. © 2020 The Authors. Advanced Optical Materials published by Wiley-VCH GmbH
- ItemCrystal phase quantum well emission with digital control(Washington D.C. : American Chemical Society, 2017) Assali, S.; Lähnemann, J.; Vu, T.T.T.; Jöns, K.D.; Gagliano, L.; Verheijen, M.A.; Akopian, N.; Bakkers, E.P.A.M.; Haverkort, J.E.M.One of the major challenges in the growth of quantum well and quantum dot heterostructures is the realization of atomically sharp interfaces. Nanowires provide a new opportunity to engineer the band structure as they facilitate the controlled switching of the crystal structure between the zinc-blende (ZB) and wurtzite (WZ) phases. Such a crystal phase switching results in the formation of crystal phase quantum wells (CPQWs) and quantum dots (CPQDs). For GaP CPQWs, the inherent electric fields due to the discontinuity of the spontaneous polarization at the WZ/ZB junctions lead to the confinement of both types of charge carriers at the opposite interfaces of the WZ/ZB/WZ structure. This confinement leads to a novel type of transition across a ZB flat plate barrier. Here, we show digital tuning of the visible emission of WZ/ZB/WZ CPQWs in a GaP nanowire by changing the thickness of the ZB barrier. The energy spacing between the sharp emission lines is uniform and is defined by the addition of single ZB monolayers. The controlled growth of identical quantum wells with atomically flat interfaces at predefined positions featuring digitally tunable discrete emission energies may provide a new route to further advance entangled photons in solid state quantum systems.
- ItemOptimization of the Epitaxial Growth of Undoped GaN Waveguides in GaN-Based Laser Diodes Evaluated by Photoluminescence(Warrendale, Pa : TMS, 2020) Netzel, C.; Hoffmann, V.; Einfeldt, S.; Weyers, M.Non-intentionally doped c-plane GaN layers are generally employed as p-side waveguide layers in violet/blue-emitting laser diodes. The recombination and diffusion of charge carriers in the p-side GaN waveguide influence the injection efficiency of holes into the InGaN quantum wells of these devices. In this study, the non-radiative recombination and the diffusivity in the [000-1] direction for charge carriers in such GaN layers are investigated by the photoluminescence of buried InGaN quantum wells, in addition to the GaN photoluminescence. The vertical charge carrier diffusion length and the diffusion constant in GaN were determined by evaluating the intensity from InGaN quantum wells in different depths below a top GaN layer. Additionally, the intensity from the buried InGaN quantum wells was found to be more sensitive to variations in the non-radiative recombination rate in the GaN layer than the intensity from the GaN itself. The study enables conclusions to be drawn on how the growth of a p-side GaN waveguide layer has to be optimized: (1) The charge carrier diffusivity in the [000-1] direction at device operation temperature is limited by phonon scattering and can be only slightly improved by material quality. (2) The use of TMGa (trimethylgallium) instead of TEGa (triethylgallium) as a precursor for the growth of GaN lowers the background silicon doping level and is advantageous for a large hole diffusion length. (3) Small growth rates below 0.5 μm/h when using TMGa or below 0.12 μm/h when using TEGa enhance non-radiative recombination. (4) A V/III gas ratio of 2200 or more is needed for low non-radiative recombination rates in GaN.
- ItemPhotoluminescence investigation of strictly ordered Ge dots grown on pit-patterned Si substrates(Bristol : IOP Publ., 2015) Brehm, Moritz; Grydlik, Martyna; Tayagaki, Takeshi; Langer, Gregor; Schäffler, Friedrich; Schmidt, Oliver G.We investigate the optical properties of ordered Ge quantum dots (QDs) by means of micro-photoluminescence spectroscopy (PL). These were grown on pit-patterned Si(001) substrates with a wide range of pit-periods and thus inter QD-distances (425–3400 nm). By exploiting almost arbitrary inter-QD distances achievable in this way we are able to choose the number of QDs that contribute to the PL emission in a range between 70 and less than three QDs. This well-defined system allows us to clarify, by PL-investigation, several points which are important for the understanding of the formation and optical properties of ordered QDs. We directly trace and quantify the amount of Ge transferred from the surrounding wetting layer (WL) to the QDs in the pits. Moreover, by exploiting different pit-shapes, we reveal the role of strain-induced activation energy barriers that have to be overcome for charge carriers generated outside the dots. These need to diffuse between the energy minimum of the WL in and between the pits, and the one in the QDs. In addition, we demonstrate that the WL in the pits is already severely intermixed with Si before upright QDs nucleate, which further enhances intermixing of ordered QDs as compared to QDs grown on planar substrates. Furthermore, we quantitatively determine the amount of Ge transferred by surface diffusion through the border region between planar and patterned substrate. This is important for the growth of ordered islands on patterned fields of finite size. We highlight that the Ge WL-facets in the pits act as PL emission centres, similar to upright QDs.
- ItemA diuranium carbide cluster stabilized inside a C80 fullerene cage(London : Nature Publishing Group, 2018) Zhang, X.; Li, W.; Feng, L.; Chen, X.; Hansen, A.; Grimme, S.; Fortier, S.; Sergentu, D.-C.; Duignan, T.J.; Autschbach, J.; Wang, S.; Wang, Y.; Velkos, G.; Popov, A.A.; Aghdassi, N.; Duhm, S.; Li, X.; Li, J.; Echegoyen, L.; Schwarz, W.H.E.; Chen, N.Unsupported non-bridged uranium-carbon double bonds have long been sought after in actinide chemistry as fundamental synthetic targets in the study of actinide-ligand multiple bonding. Here we report that, utilizing I h(7)-C80 fullerenes as nanocontainers, a diuranium carbide cluster, U=C=U, has been encapsulated and stabilized in the form of UCU@I h(7)-C80. This endohedral fullerene was prepared utilizing the Krätschmer-Huffman arc discharge method, and was then co-crystallized with nickel(II) octaethylporphyrin (NiII-OEP) to produce UCU@I h(7)-C80·[NiII-OEP] as single crystals. X-ray diffraction analysis reveals a cage-stabilized, carbide-bridged, bent UCU cluster with unexpectedly short uranium-carbon distances (2.03 Å) indicative of covalent U=C double-bond character. The quantum-chemical results suggest that both U atoms in the UCU unit have formal oxidation state of +5. The structural features of UCU@I h(7)-C80 and the covalent nature of the U(f1)=C double bonds were further affirmed through various spectroscopic and theoretical analyses.
- ItemSolar spectral conversion for improving the photosynthetic activity in algae reactors(London : Nature Publishing Group, 2013) Wondraczek, L.; Batentschuk, M.; Schmidt, M.A.; Borchardt, R.; Scheiner, S.; Seemann, B.; Schweizer, P.; Brabec, C.J.Sustainable biomass production is expected to be one of the major supporting pillars for future energy supply, as well as for renewable material provision. Algal beds represent an exciting resource for biomass/biofuel, fine chemicals and CO2 storage. Similar to other solar energy harvesting techniques, the efficiency of algal photosynthesis depends on the spectral overlap between solar irradiation and chloroplast absorption. Here we demonstrate that spectral conversion can be employed to significantly improve biomass growth and oxygen production rate in closed-cycle algae reactors. For this purpose, we adapt a photoluminescent phosphor of the type Ca 0.59Sr0.40Eu0.01S, which enables efficient conversion of the green part of the incoming spectrum into red light to better match the Qy peak of chlorophyll b. Integration of a Ca 0.59Sr0.40Eu0.01S backlight converter into a flat panel algae reactor filled with Haematococcus pluvialis as a model species results in significantly increased photosynthetic activity and algae reproduction rate.
- ItemHierarchical Corannulene‐Based Materials: Energy Transfer and Solid‐State Photophysics(Weinheim : Wiley-VCH, 2017-3-23) Rice, Allison M.; Fellows, W. Brett; Dolgopolova, Ekaterina A.; Greytak, Andrew B.; Vannucci, Aaron K.; Smith, Mark D.; Karakalos, Stavros G.; Krause, Jeanette A.; Avdoshenko, Stanislav M.; Popov, Alexey A.; Shustova, Natalia B.We report the first example of a donor–acceptor corannulene-containing hybrid material with rapid ligand-to-ligand energy transfer (ET). Additionally, we provide the first time-resolved photoluminescence (PL) data for any corannulene-based compounds in the solid state. Comprehensive analysis of PL data in combination with theoretical calculations of donor–acceptor exciton coupling was employed to estimate ET rate and efficiency in the prepared material. The ligand-to-ligand ET rate calculated using two models is comparable with that observed in fullerene-containing materials, which are generally considered for molecular electronics development. Thus, the presented studies not only demonstrate the possibility of merging the intrinsic properties of π-bowls, specifically corannulene derivatives, with the versatility of crystalline hybrid scaffolds, but could also foreshadow the engineering of a novel class of hierarchical corannulene-based hybrid materials for optoelectronic devices.
- ItemImportance of the dielectric contrast for the polarization of excitonic transitions in single GaN nanowires(Milton Park : Taylor & Francis, 2015) Corfdir, Pierre; Feix, Felix; Zettler, Johannes K.; Fernández-Garrido, Sergio; Brandt, OliverWe investigate the polarization of excitonic transitions of single dispersed GaN nanowires with a diameter of about 50 nm. We observe donor-bound exciton transitions with a linewidth narrower than 250 μeV at 10 K, whereas the luminescence from free excitons exhibits a width of up to 5 meV. This broadening is larger than that observed for free excitons in the as-grown nanowire ensemble and is the result of inhomogeneous strain introduced by the nanowire dispersion. This strain lowers the symmetry of the lattice structure and allows A excitons to emit light polarized parallel to the nanowire axis. The polarization anisotropy of A excitons, however, is found to largely vary from one nanowire to another. In addition, the various bound-exciton lines in a given nanowire do not show the same polarization anisotropies. These findings can be explained by the dielectric contrast between the nanowire and its environment, but only when taking into account the strong variations of the dielectric function of GaN at the near band-edge.
- ItemElectronic properties of wurtzite GaAs: A correlated structural, optical, and theoretical analysis of the same polytypic GaAs nanowire(Heidelberg : Springer, 2018) Senichev, Alexander; Corfdir, Pierre; Brandt, Oliver; Ramsteiner, Manfred; Breuer, Steffen; Schilling, Jörg; Geelhaar, Lutz; Werner, PeterIII-V compound semiconductor nanowires are generally characterized by the coexistence of zincblende and wurtzite structures. So far, this polytypism has impeded the determination of the electronic properties of the metastable wurtzite phase of GaAs, which thus remain highly controversial. In an effort to obtain new insights into this topic, we cross-correlate nanoscale spectral imaging by near-field scanning optical microscopy with a transmission electron microscopy analysis of the very same polytypic GaAs nanowire dispersed onto a Si wafer. Thus, spatially resolved photoluminescence spectra could be unambiguously assigned to nanowire segments whose structure is known with lattice-resolved accuracy. An emission energy of 1.528 eV was observed from extended zincblende segments, revealing that the dispersed nanowire was under uniaxial strain presumably due to interaction with its supporting substrate. These crucial information and the emission energy obtained for extended pure wurtzite segments were used to perform envelope function calculations of zincblende quantum disks in a wurtzite matrix as well as the inverse structure. In these calculations, we varied the fundamental bandgap, the electron mass, and the band offset between zincblende and wurtzite GaAs. From this multi-parameter comparison with the experimental data, we deduced that the bandgap between the Γ8 conduction and A valence band ranges from 1.532 to 1.539 eV in strain-free wurtzite GaAs, and estimated values of 1.507 to 1.514 eV for the Γ7–A bandgap. Address correspondence
- ItemGrowth of GaN nanowire ensembles in molecular beam epitaxy: Overcoming the limitations of their spontaneous formation(Berlin : Humboldt-Universität zu Berlin, 2018) Zettler, Johannes KristianDichte Ensembles aus GaN-Nanodrähten können in der Molekularstrahlepitaxie mithilfe eines selbstinduzierten Prozesses sowohl auf kristallinen als auch amorphen Substraten gezüchtet werden. Aufgrund der Natur selbstgesteuerter Prozesse ist dabei die Kontrolle über viele wichtige Ensembleparameter jedoch eingeschränkt. Die Arbeit adressiert genau diese Einschränkungen bei der Kristallzucht selbstinduzierter GaN-Nanodrähte. Konkret sind das Limitierungen bezüglich der Nanodraht-Durchmesser, die Nanodraht-Anzahl-/Flächendichte, der Koaleszenzgrad sowie die maximal realisierbare Wachstumstemperatur. Für jede dieser Einschränkungen werden Lösungen präsentiert, um die jeweilige Limitierung zu umgehen oder zu verschieben. Als Resultat wurde eine neue Klasse von GaN Nanodrähten mit bisher unerreichten strukturellen und optischen Eigenschaften geschaffen. Mithilfe eines Zwei-Schritt-Ansatzes, bei dem die Wachstumstemperatur während der Nukleationsphase erhöht wurde, konnte eine verbesserte Kontrolle über die Flächendichte, den Durchmesser und den Koaleszenzgrad der GaN-Nanodraht-Ensembles erreicht werden. Darüber hinaus werden Ansätze präsentiert, um die außerordentlich lange Inkubationszeit bei hohen Wachstumstemperaturen zu minimieren und damit wesentlich höhere Wachstumstemperaturen zu ermöglichen (bis zu 905°C). Die resulierenden GaN-Nanodraht-Ensembles weisen schmale exzitonische Übergänge mit sub-meV Linienbreiten auf, vergleichbar zu denen freistehender GaN-Schichten. Abschließend wurden Nanodrähte mit Durchmessern deutlich unterhalb von 10 nm fabriziert. Mithilfe eines Zersetzungsschrittes im Ultrahochvakuum direkt im Anschluss an die Wachstumsphase wurden reguläre Nanodraht-Ensembles verdünnt. Die resultierenden ultradünnen Nanodrähte weisen dielektrisches Confinement auf. Wir zeigen eine ausgeprägte exzitonische Emission von puren GaN-Nanodrähten mit Durchmessern bis hinab zu 6 nm.