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- ItemRevealing all states of dewetting of a thin gold layer on a silicon surface by nanosecond laser conditioning(Amsterdam : Elsevier, 2021) Ernst, Owen C.; Uebel, David; Kayser, Stefan; Lange, Felix; Teubner, Thomas; Boeck, TorstenDewetting is a ubiquitous phenomenon which can be applied to the laser synthesis of nanoparticles. A classical spinodal dewetting process takes place in four successive states, which differ from each other in their morphology. In this study all states are revealed by interaction of pulsed nanosecond UV laser light with thin gold layers with thicknesses between 1 nm and 10 nm on (100) silicon wafers. The specific morphologies of the dewetting states are discussed with particular emphasis on the state boundaries. The main parameter determining which state is formed is not the duration for which the gold remains liquid, but rather the input energy provided by the laser. This shows that each state transition has a separate measurable activation energy. The temperature during the nanosecond pulses and the duration during which the gold remains liquid was determined by simulation using the COMSOL Multiphysics® software package. Using these calculations, an accurate local temperature profile and its development over time was simulated. An analytical study of the morphologies and formed structures was performed using Minkowski measures. With aid of this tool, the laser induced structures were compared with thermally annealed samples, with perfectly ordered structures and with perfectly random structures. The results show that both, structures of the laser induced and the annealed samples, strongly resemble the perfectly ordered structures. This reveals a close relationship between these structures and suggests that the phenomenon under investigation is indeed a spinodal dewetting generated by an internal material wave function. The purposeful generation of these structures and the elucidation of the underlying mechanism of dewetting by short pulse lasers may assist the realisation of various technical elements such as nanowires in science and industry. © 2020
- ItemInvestigating the electrochemical stability of Li7La3Zr2O12 solid electrolytes using field stress experiments(London [u.a.] : RSC, 2021) Smetaczek, Stefan; Pycha, Eva; Ring, Joseph; Siebenhofer, Matthäus; Ganschow, Steffen; Berendts, Stefan; Nenning, Andreas; Kubicek, Markus; Rettenwander, Daniel; Limbeck, Andreas; Fleig, JürgenCubic Li7La3Zr2O12 (LLZO) garnets are among the most promising solid electrolytes for solid-state batteries with the potential to exceed conventional battery concepts in terms of energy density and safety. The electrochemical stability of LLZO is crucial for its application, however, controversial reports in the literature show that it is still an unsettled matter. Here, we investigate the electrochemical stability of LLZO single crystals by applying electric field stress via macro- and microscopic ionically blocking Au electrodes in ambient air. Induced material changes are subsequently probed using various locally resolved analysis techniques, including microelectrode electrochemical impedance spectroscopy (EIS), laser induced breakdown spectroscopy (LIBS), laser ablation-inductively coupled plasma-mass spectrometry (LA-ICP-MS), and microfocus X-ray diffraction (XRD). Our experiments indicate that LLZO decomposes at 4.1–4.3 V vs. Li+/Li, leading to the formation of Li-poor phases like La2Zr2O7 beneath the positively polarized electrode. The reaction is still on-going even after several days of polarization, indicating that no blocking interfacial layer is formed. The decomposition can be observed at elevated as well as room temperature and suggests that LLZO is truly not compatible with high voltage cathode materials.
- ItemEpitaxial growth of the first two members of the Ban +1InnO2.5 n +1Ruddlesden-Popper homologous series(New York, NY : American Institute of Physics, 2022) Hensling, Felix V. E.; Smeaton, Michelle A.; Show, Veronica; Azizie, Kathy; Barone, Matthew R.; Kourkoutis, Lena F.; Schlom, Darrell G.We demonstrate the epitaxial growth of the first two members, and the n = ∞ member of the homologous Ruddlesden-Popper series of Ba n + 1 In n O 2.5 n + 1 of which the n = 1 member was previously unknown. The films were grown by suboxide molecular-beam epitaxy where the indium is provided by a molecular beam of indium-suboxide [In 2O (g)]. To facilitate ex situ characterization of the highly hygroscopic barium indate films, a capping layer of amorphous SiO 2 was deposited prior to air exposure. The structural quality of the films was assessed by x-ray diffraction, reflective high-energy electron diffraction, and scanning transmission electron microscopy.
- ItemHigh‐Temperature Annealing and Patterned AlN/Sapphire Interfaces(Weinheim : Wiley-VCH, 2021) Hagedorn, Sylvia; Mogilatenko, Anna; Walde, Sebastian; Pacak, Daniel; Weinrich, Jonas; Hartmann, Carsten; Weyers, MarkusUsing the example of epitaxial lateral overgrowth of AlN on trench-patterned AlN/sapphire templates, the impact of introducing a high-temperature annealing step into the process chain is investigated. Covering the open surfaces of sapphire trench sidewalls with a thin layer of AlN is found to be necessary to preserve the trench shape during annealing. Both the influence of annealing temperature and annealing duration are investigated. To avoid the deformation of the AlN/sapphire interface during annealing, the annealing duration or annealing temperature must be low enough. Annealing for 1 h at 1730 °C is found to allow for the lowest threading dislocation density of 3.5 × 108 cm−2 in the subsequently grown AlN, while maintaining an uncracked smooth surface over the entire 2 in. wafer. Transmission electron microscopy study confirms the defect reduction by high-temperature annealing and reveals an additional strain relaxation mechanism by accumulation of horizontal dislocation lines at the interface between annealed and nonannealed AlN. By applying a second annealing step, the dislocation density can be further reduced to 2.5 × 108 cm−2.
- ItemCurrent Status of Carbon‐Related Defect Luminescence in GaN(Weinheim : Wiley-VCH, 2021) Zimmermann, Friederike; Beyer, Jan; Röder, Christian; Beyer, Franziska C.; Richter, Eberhard; Irmscher, Klaus; Heitmann, JohannesHighly insulating layers are a prerequisite for gallium nitride (GaN)-based power electronic devices. For this purpose, carbon doping is one of the currently pursued approaches. However, its impact on the optical and electrical properties of GaN has been widely debated in the scientific community. For further improvement of device performance, a better understanding of the role of related defects is essential. To study optically active point defects, photoluminescence is one of the most frequently used experimental characterization techniques. Herein, the main recent advances in the attribution of carbon-related photoluminescence bands are reviewed, which were enabled by the interplay of a refinement of growth and characterization techniques and state-of-the-art first-principles calculations developed during the last decade. The predicted electronic structures of isolated carbon defects and selected carbon-impurity complexes are compared to experimental results. Taking into account both of these, a comprehensive overview on the present state of interpretation of carbon-related broad luminescence bands in bulk GaN is presented.
- ItemMelt Growth and Physical Properties of Bulk LaInO3 Single Crystals(Weinheim : Wiley-VCH, 2021) Galazka, Zbigniew; Irmscher, Klaus; Ganschow, Steffen; Zupancic, Martina; Aggoune, Wahib; Draxl, Claudia; Albrecht, Martin; Klimm, Detlef; Kwasniewski, Albert; Schulz, Tobias; Pietsch, Mike; Dittmar, Andrea; Grueneberg, Raimund; Juda, Uta; Schewski, Robert; Bergmann, Sabine; Cho, Hyeongmin; Char, Kookrin; Schroeder, Thomas; Bickermann, MatthiasLarge bulk LaInO3 single crystals are grown from the melt contained within iridium crucibles by the vertical gradient freeze (VGF) method. The obtained crystals are undoped or intentionally doped with Ba or Ce, and enabled wafer fabrication of size 10 × 10 mm2. High melting point of LaInO3 (≈1880 °C) and thermal instability at high temperatures require specific conditions for bulk crystal growth. The crystals do not undergo any phase transition up to 1300 °C, above which a noticeable thermal decomposition takes place. The good structural quality of the crystals makes them suitable for epitaxy. The onset of strong optical absorption shows orientation-dependent behavior due to the orthorhombic symmetry of the LaInO3 crystals. Assuming direct transitions, optical bandgaps of 4.35 and 4.39 eV are obtained for polarizations along the [010] and the [100], [001] crystallographic directions, respectively. There is an additional weak absorption in the range between 2.8 and 4 eV due to oxygen vacancies. Density-functional-theory calculations support the interpretation of the optical absorption data. Cathodoluminescence spectra show a broad, structured emission band peaking at ≈2.2 eV. All bulk crystals are electrically insulating. The relative static dielectric constant is determined at a value of 24.6 along the [001] direction.
- ItemSub-6 optical-cycle Kerr-lens mode-locked Tm:Lu2O3 and Tm:Sc2O3 combined gain media laser at 2.1 μm(Washington, DC : Soc., 2021) Suzuki, Anna; Kränkel, Christian; Tokurakawa, MasakiWe present a combined gain media Kerr-lens mode-locked laser based on a Tm:Lu2O3 ceramic and a Tm:Sc2O3 single crystal. Pulses as short as 41 fs, corresponding to less than 6 optical cycles, were obtained with an average output power of 42 mW at a wavelength of 2.1 μm and a repetition rate of 93.3 MHz. Furthermore, a maximum average power of 316 mW with a pulse duration of 73 fs was achieved.
- ItemStrain-stabilized superconductivity([London] : Nature Publishing Group UK, 2021) Ruf, J.P.; Paik, H.; Schreiber, N.J.; Nair, H.P.; Miao, L.; Kawasaki, J.K.; Nelson, J.N.; Faeth, B.D.; Lee, Y.; Goodge, B.H.; Pamuk, B.; Fennie, C.J.; Kourkoutis, L.F.; Schlom, D.G.; Shen, K.M.Superconductivity is among the most fascinating and well-studied quantum states of matter. Despite over 100 years of research, a detailed understanding of how features of the normal-state electronic structure determine superconducting properties has remained elusive. For instance, the ability to deterministically enhance the superconducting transition temperature by design, rather than by serendipity, has been a long sought-after goal in condensed matter physics and materials science, but achieving this objective may require new tools, techniques and approaches. Here, we report the transmutation of a normal metal into a superconductor through the application of epitaxial strain. We demonstrate that synthesizing RuO2 thin films on (110)-oriented TiO2 substrates enhances the density of states near the Fermi level, which stabilizes superconductivity under strain, and suggests that a promising strategy to create new transition-metal superconductors is to apply judiciously chosen anisotropic strains that redistribute carriers within the low-energy manifold of d orbitals.
- ItemThe multi-photon induced Fano effect([London] : Nature Publishing Group UK, 2021) Litvinenko, K.L.; Le, Nguyen H.; Redlich, B.; Pidgeon, C.R.; Abrosimov, N.V.; Andreev, Y.; Huang, Zhiming; Murdin, B.N.The ordinary Fano effect occurs in many-electron atoms and requires an autoionizing state. With such a state, photo-ionization may proceed via pathways that interfere, and the characteristic asymmetric resonance structures appear in the continuum. Here we demonstrate that Fano structure may also be induced without need of auto-ionization, by dressing the continuum with an ordinary bound state in any atom by a coupling laser. Using multi-photon processes gives complete, ultra-fast control over the interference. We show that a line-shape index q near unity (maximum asymmetry) may be produced in hydrogenic silicon donors with a relatively weak beam. Since the Fano lineshape has both constructive and destructive interference, the laser control opens the possibility of state-selective detection with enhancement on one side of resonance and invisibility on the other. We discuss a variety of atomic and molecular spectroscopies, and in the case of silicon donors we provide a calculation for a qubit readout application.
- ItemEngineering new limits to magnetostriction through metastability in iron-gallium alloys([London] : Nature Publishing Group UK, 2021) Meisenheimer, P.B.; Steinhardt, R.A.; Sung, S.H.; Williams, L.D.; Zhuang, S.; Nowakowski, M.E.; Novakov, S.; Torunbalci, M.M.; Prasad, B.; Zollner, C. J.; Wang, Z.; Dawley, N.M.; Schubert, J.; Hunter, A.H.; Manipatruni, S.; Nikonov, D.E.; Young, I.A.; Chen, L.Q.; Bokor, J.; Bhave, S.A.; Ramesh, R.; Hu, J.-M.; Kioupakis, E.; Hovden, R.; Schlom, D.G.; Heron, J.T.Magnetostrictive materials transduce magnetic and mechanical energies and when combined with piezoelectric elements, evoke magnetoelectric transduction for high-sensitivity magnetic field sensors and energy-efficient beyond-CMOS technologies. The dearth of ductile, rare-earth-free materials with high magnetostrictive coefficients motivates the discovery of superior materials. Fe1−xGax alloys are amongst the highest performing rare-earth-free magnetostrictive materials; however, magnetostriction becomes sharply suppressed beyond x = 19% due to the formation of a parasitic ordered intermetallic phase. Here, we harness epitaxy to extend the stability of the BCC Fe1−xGax alloy to gallium compositions as high as x = 30% and in so doing dramatically boost the magnetostriction by as much as 10x relative to the bulk and 2x larger than canonical rare-earth based magnetostrictors. A Fe1−xGax − [Pb(Mg1/3Nb2/3)O3]0.7−[PbTiO3]0.3 (PMN-PT) composite magnetoelectric shows robust 90° electrical switching of magnetic anisotropy and a converse magnetoelectric coefficient of 2.0 × 10−5 s m−1. When optimally scaled, this high coefficient implies stable switching at ~80 aJ per bit.
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