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- ItemOptical Anisotropy and Momentum-Dependent Excitons in Dibenzopentacene Single Crystals(Washington, DC : ACS Publications, 2022) Graf, Lukas; Liu, Fupin; Naumann, Marco; Roth, Friedrich; Debnath, Bipasha; Büchner, Bernd; Krupskaya, Yulia; Popov, Alexey A.; Knupfer, MartinHigh-quality single crystals of the organic semiconductor (1,2;8,9)-dibenzopentacene were grown via physical vapor transport. The crystal structure─unknown before─was determined by single-crystal X-ray diffraction; polarization-dependent optical absorption measurements display a large anisotropy in the ac plane of the crystals. The overall Davydov splitting is ∼110 meV, which is slightly lower than that in the close relative pentacene (120 meV). Momentum-dependent electron energy-loss spectroscopy measurements show a clear exciton dispersion of the Davydov components. An analysis of the dispersion using a simple 1D model indicates smaller electron- and hole-transfer integrals in dibenzopentacene as compared to pentacene. The spectral weight distribution of the excitation spectra is strongly momentum-dependent and demonstrates a strong momentum-dependent admixture of Frenkel excitons, charge-transfer excitons, and vibrational modes.
- ItemThree-Dimensional Composition and Electric Potential Mapping of III–V Core–Multishell Nanowires by Correlative STEM and Holographic Tomography(Washington, DC : ACS Publ., 2018-7-13) Wolf, Daniel; Hübner, René; Niermann, Tore; Sturm, Sebastian; Prete, Paola; Lovergine, Nico; Büchner, Bernd; Lubk, AxelThe nondestructive characterization of nanoscale devices, such as those based on semiconductor nanowires, in terms of functional potentials is crucial for correlating device properties with their morphological/materials features, as well as for precisely tuning and optimizing their growth process. Electron holographic tomography (EHT) has been used in the past to reconstruct the total potential distribution in three-dimension but hitherto lacked a quantitative approach to separate potential variations due to chemical composition changes (mean inner potential, MIP) and space charges. In this Letter, we combine and correlate EHT and high-angle annular dark-field scanning transmission electron microscopy (HAADF-STEM) tomography on an individual ⟨111⟩ oriented GaAs–AlGaAs core–multishell nanowire (NW). We obtain excellent agreement between both methods in terms of the determined Al concentration within the AlGaAs shell, as well as thickness variations of the few nanometer thin GaAs shell acting as quantum well tube. Subtracting the MIP determined from the STEM tomogram, enables us to observe functional potentials at the NW surfaces and at the Au–NW interface, both ascribed to surface/interface pinning of the semiconductor Fermi level.
- ItemTheoretical Prediction of a Giant Anisotropic Magnetoresistance in Carbon Nanoscrolls(Washington, DC : ACS Publ., 2017-4-12) Chang, Ching-Hao; Ortix, CarmineSnake orbits are trajectories of charge carriers curving back and forth that form at an interface where either the magnetic field direction or the charge carrier type are inverted. In ballistic samples, their presence is manifested in the appearance of magnetoconductance oscillations at small magnetic fields. Here we show that signatures of snake orbits can also be found in the opposite diffusive transport regime. We illustrate this by studying the classical magnetotransport properties of carbon tubular structures subject to relatively weak transversal magnetic fields where snake trajectories appear in close proximity to the zero radial field projections. In carbon nanoscrolls, the formation of snake orbits leads to a strongly directional dependent positive magnetoresistance with an anisotropy up to 80%.
- ItemGraphene transfer methods: A review(New York, NY [u.a.] : Springer, 2021) Ullah, Sami; Yang, Xiaoqin; Ta, Huy Q.; Hasan, Maria; Bachmatiuk, Alicja; Tokarska, Klaudia; Trzebicka, Barbara; Fu, Lei; Rummeli, Mark H.Graphene is a material with unique properties that can be exploited in electronics, catalysis, energy, and bio-related fields. Although, for maximal utilization of this material, high-quality graphene is required at both the growth process and after transfer of the graphene film to the application-compatible substrate. Chemical vapor deposition (CVD) is an important method for growing high-quality graphene on non-technological substrates (as, metal substrates, e.g., copper foil). Thus, there are also considerable efforts toward the efficient and non-damaging transfer of quality of graphene on to technologically relevant materials and systems. In this review article, a range of graphene current transfer techniques are reviewed from the standpoint of their impact on contamination control and structural integrity preservation of the as-produced graphene. In addition, their scalability, cost- and time-effectiveness are discussed. We summarize with a perspective on the transfer challenges, alternative options and future developments toward graphene technology.
- ItemPhonon-Assisted Two-Photon Interference from Remote Quantum Emitters(Washington, DC : ACS Publ., 2017-6-7) Reindl, Marcus; Jöns, Klaus D.; Huber, Daniel; Schimpf, Christian; Huo, Yongheng; Zwiller, Val; Rastelli, Armando; Trotta, RinaldoPhotonic quantum technologies are on the verge of finding applications in everyday life with quantum cryptography and quantum simulators on the horizon. Extensive research has been carried out to identify suitable quantum emitters and single epitaxial quantum dots have emerged as near-optimal sources of bright, on-demand, highly indistinguishable single photons and entangled photon-pairs. In order to build up quantum networks, it is essential to interface remote quantum emitters. However, this is still an outstanding challenge, as the quantum states of dissimilar “artificial atoms” have to be prepared on-demand with high fidelity and the generated photons have to be made indistinguishable in all possible degrees of freedom. Here, we overcome this major obstacle and show an unprecedented two-photon interference (visibility of 51 ± 5%) from remote strain-tunable GaAs quantum dots emitting on-demand photon-pairs. We achieve this result by exploiting for the first time the full potential of a novel phonon-assisted two-photon excitation scheme, which allows for the generation of highly indistinguishable (visibility of 71 ± 9%) entangled photon-pairs (fidelity of 90 ± 2%), enables push-button biexciton state preparation (fidelity of 80 ± 2%) and outperforms conventional resonant two-photon excitation schemes in terms of robustness against environmental decoherence. Our results mark an important milestone for the practical realization of quantum repeaters and complex multiphoton entanglement experiments involving dissimilar artificial atoms.
- ItemProgress and challenges in using sustainable carbon anodes in rechargeable metal-ion batteries(Amsterdam [u.a.] : Elsevier, 2021) Soltani, Niloofar; Bahrami, Amin; Giebeler, Lars; Gemming, Thomas; Mikhailova, DariaRechargeable lithium-ion batteries (LIBs) are one of the most promising alternatives to effectively bypass fossil fuels. However, long-term energy application of LIBs could be restricted in the future due to the increased production cost of LIB arising from the shortage and inaccessibility of Li in the Earth's crust. Na or K have been considered as substitutes for Li but in spite of their natural abundance, they suffer from low gravimetric/volumetric energy density. An alternative to increase the efficiency of sodium-ion battery (SIBs) and potassium-ion battery (KIBs) is to focus on finding the high‐performing negative electrode, the anode. The large volume changes of alloying and conversion type anodes for KIBs and SIBs make hard carbons to a better option on this regard than usual graphitic carbons, but a key obstacle is the reliance on unsustainable sources. Thus, biomass-derived carbon could offer a promising alternative, and it has indeed been in the focus of much recent work. This review highlights the recent advances in using carbon extracted from various biomass sources in rechargeable Li-, Na-, and K-ion batteries. Maximizing the energy and power densities as well as the lifetime of carbon anodes require an exploration of the right balance between carbon structures, pore morphology, chemical composition and alkali metal-ion storage. Thus, in this review, first, we take stock of key challenges and opportunities to extract carbon from various plants structural components and identify the extracted carbon structure compared to graphite-like structure. Then, we provide an overview on morphological and structural modification of the extracted carbons. Finally, we show how the physicochemical properties, structural alignment and morphological variation of the biomass-derived carbon can affect the storage mechanism and electrochemical performance. The extensive overview of this topic provided here is expected to stimulate further work on environmentally friendly battery design and towards the optimization of the battery performance. Electrode materials in alkali-metal-ion batteries that are based on biomass-derived carbon may allow not only a technical breakthrough, but also an ethically and socially acceptable product.
- ItemSerrated flow of CuZr-based bulk metallic glasses probed by nanoindentation: Role of the activation barrier, size and distribution of shear transformation zones(Amsterdam [u.a.] : Elsevier Science, 2017) Limbach, R.; Kosiba, K.; Pauly, S.; Kühn, U.; Wondraczek, L.We report on the effect of Al and Co alloying in vitreous Cu50Zr50 on local deformation and serrated flow as a model for relating the size and localization of shear transformation zones (STZ) to Poisson ratio and strain-rate sensitivity of metallic glasses. Alloying with Al results in significant variations in mechanical performance, in particular, in Young's modulus, hardness and strain-rate sensitivity. Increasing strain-rate sensitivity with increasing degree of alloying indicates a reduced tendency for shear localization. In parallel, a gradual transition from inhomogeneous to homogeneous plastic flow is observed. Using a statistical analysis of the shear stress associated with the initiation of the first pop-in in the load-displacement curve during spherical indentation, the activation volume for plastic flow at the onset of yielding is reported. This analysis is employed for experimental evaluation of the compositional dependence of activation barrier, size and distribution of STZs. It is demonstrated that the STZ size does not change significantly upon Al alloying and encompasses a local volume of around 22–24 atoms. However, the barrier energy density for the initiation of a single STZ progressively increases. The broader distribution of STZs impedes their accumulation into larger-size flow units, leading to a lower number and reduced size of serrations in the load-displacement curve. On the contrary, lower barrier energy densities enable a larger quantity of STZs to be activated simultaneously. These STZs can easily percolate into large flow units, promoting plastic flow through their interaction. We employ Poisson's ratio as an indicator for plasticity to shown that this interpretation can be transferred to other types of metallic glasses. That is, larger flow units were found for metallic glasses with higher Poisson ratio and more pronounced plasticity, while the flow units in alloys with very low Poisson ratio and high brittleness are significantly reduced in size and more homogeneously distributed throughout the material.
- ItemFreestanding Nanolayers of a Wide-Gap Topological Insulator through Liquid-Phase Exfoliation(Weinheim : Wiley-VCH, 2021) Lê Anh, Mai; Potapov, Pavel; Wolf, Daniel; Lubk, Axel; Glatz, Bernhard; Fery, Andreas; Doert, Thomas; Ruck, MichaelThe layered salt Bi14Rh3I9 is a weak three-dimensional (3D) topological insulator (TI), that is, a stack of two-dimensional (2D) TIs. It has a wide non-trivial band gap of 210 meV, which is generated by strong spin-orbit coupling, and possesses protected electronic edge-states. In the structure, charged layers of (Formula presented.) (Bi4Rh)3I]2+ honeycombs and (Formula presented.) Bi2I8]2− chains alternate. The non-trivial topology of Bi14Rh3I9 is an inherent property of the 2D intermetallic fragment. Here, the exfoliation of Bi14Rh3I9 was performed using two different chemical approaches: (a) through a reaction with n-butyllithium and poly(vinylpyrrolidone), (b) through a reaction with betaine in dimethylformamide at 55 °C. The former yielded few-layer sheets of the new compound Bi12Rh3I, while the latter led to crystalline sheets of Bi14Rh3I9 with a thickness down to 5 nm and edge-lengths up to several ten microns. X-ray diffraction and electron microscopy proved that the structure of Bi14Rh3I9 remained intact. Thus, it was assumed that the particles are still TIs. Dispersions of these flakes now allow for next steps towards the envisioned applications in nanoelectronics, such as the study of quantum coherence in deposited films, the combination with superconducting particles or films for the generation of Majorana fermions, or studies on their behavior under the influence of magnetic or electric fields or in contact with various materials occurring in devices. The method presented generally allows to exfoliate layers with high specific charges and thus the use of layered starting materials beyond van der Waals crystals. © 2020 The Authors. Chemistry - A European Journal published by Wiley-VCH GmbH
- ItemSingle-atom catalytic growth of crystals using graphene as a case study(London : Nature Publishing Group, 2021) Yang, Xiaoqin; Liu, Yu; Ta, Huy Q.; Rezvani, Ehsan; Zhang, Yue; Zeng, Mengqi; Fu, Lei; Bachmatiuk, Alicja; Luo, Jinping; Liu, Lijun; Rümmeli, Mark H.Anchored Single-atom catalysts have emerged as a cutting-edge research field holding tremendous appeal for applications in the fields of chemicals, energy and the environment. However, single-atom-catalysts for crystal growth is a nascent field. Of the few studies available, all of them are based on state-of-the-art in situ microscopy investigations and computational studies, and they all look at the growth of monolayer graphene from a single-atom catalyst. Despite the limited number of studies, they do, collectively, represent a new sub-field of single-atom catalysis, namely single-atom catalytic growth of crystalline solids. In this review, we examine them on substrate-supported and as freestanding graphene fabrication, as well as rolled-up graphene, viz., single-walled carbon nanotubes (SWCNT), grown from a single atom. We also briefly discuss the catalytic etching of graphene and SWCNT’s and conclude by outlining the future directions we envision this nascent field to take.