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    A hybrid MBE-based growth method for large-area synthesis of stacked hexagonal boron nitride/graphene heterostructures
    (London : Nature Publishing Group, 2017) Wofford, Joseph M.; Nakhaie, Siamak; Krause, Thilo; Liu, Xianjie; Ramsteiner, Manfred; Hanke, Michael; Riechert, Henning; Lopes, J.; Marcelo, J.
    Van der Waals heterostructures combining hexagonal boron nitride (h-BN) and graphene offer many potential advantages, but remain difficult to produce as continuous films over large areas. In particular, the growth of h-BN on graphene has proven to be challenging due to the inertness of the graphene surface. Here we exploit a scalable molecular beam epitaxy based method to allow both the h-BN and graphene to form in a stacked heterostructure in the favorable growth environment provided by a Ni(111) substrate. This involves first saturating a Ni film on MgO(111) with C, growing h-BN on the exposed metal surface, and precipitating the C back to the h-BN/Ni interface to form graphene. The resulting laterally continuous heterostructure is composed of a top layer of few-layer thick h-BN on an intermediate few-layer thick graphene, lying on top of Ni/MgO(111). Examinations by synchrotron-based grazing incidence diffraction, X-ray photoemission spectroscopy, and UV-Raman spectroscopy reveal that while the h-BN is relaxed, the lattice constant of graphene is significantly reduced, likely due to nitrogen doping. These results illustrate a different pathway for the production of h-BN/graphene heterostructures, and open a new perspective for the large-area preparation of heterosystems combining graphene and other 2D or 3D materials.
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    Indocyanine Green-Loaded Polydopamine-Reduced Graphene Oxide Nanocomposites with Amplifying Photoacoustic and Photothermal Effects for Cancer Theranostics
    (Wyoming, NSW : Ivyspring, 2016) Hu, Dehong; Zhang, Jingnan; Gao, Guanhui; Sheng, Zonghai; Cui, Haodong; Cai, Lintao
    Photoacoustic (PA) imaging and photothermal therapy (PTT) as light-induced theranostic platforms have been attracted much attention in recent years. However, the development of highly efficient and integrated phototheranostic nanoagents for amplifying PA imaging and PTT treatments poses great challenges. Here, we report a novel phototheranostic nanoagent using indocyanine green-loaded polydopamine-reduced graphene oxide nanocomposites (ICG-PDA-rGO) with amplifying PA and PTT effects for cancer theranostics. The results demonstrate that the PDA layer coating on the surface of rGO could effectively absorb a large number of ICG molecules, quench ICG's fluorescence, and enhance the PDA-rGO's optical absorption at 780 nm. The obtained ICG-PDA-rGO exhibits stronger PTT effect and higher PA contrast than that of pure GO and PDA-rGO. After PA imaging-guided PTT treatments, the tumors in 4T1 breast subcutaneous and orthotopic mice models are suppressed completely and no treatment-induced toxicity being observed. It illustrates that the ICG-PDA-rGO nanocomposites constitute a new class of theranostic nanomedicine for amplifying PA imaging and PTT treatments.
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    Phonon anharmonicities and ultrafast dynamics in epitaxial Sb2Te3
    ([London] : Macmillan Publishers Limited, part of Springer Nature, 2020) Bragaglia, V.; Ramsteiner, M.; Schick, D.; Boschker, J.E.; Mitzner, R.; Calarco, R.; Holldack, K.
    In this study we report on the investigation of epitaxially grown Sb2Te3 by employing Fourier-Transform transmission Spectroscopy (FTS) with laser-induced Coherent Synchrotron Radiation (CSR) in the Terahertz (THz) spectral range. Static spectra in the range between 20 and 120 cm−1 highlight a peculiar softening of an in-plane IR-active phonon mode upon temperature decrease, as opposed to all Raman active modes which instead show a hardening upon temperature decrease in the same energy range. The phonon mode softening is found to be accompanied by an increase of free carrier concentration. A strong coupling of the two systems (free carriers and phonons) is observed and further evidenced by exciting the same phonon mode at 62 cm−1 within an ultrafast pump-probe scheme employing a femtosecond laser as pump and a CSR single cycle THz pulse as probe. Separation of the free carrier contribution and the phonon resonance in the investigated THz range reveals that, both damping of the phonon mode and relaxation of hot carriers in the time domain happen on the same time scale of 5 ps. This relaxation is about a factor of 10 slower than expected from the Lorentz time-bandwidth limit. The results are discussed in the framework of phonon scattering at thermal and laser induced transient free carriers.
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    Application of electron tomography for comprehensive determination of III-V interface properties
    (Amsterdam : Elsevier Science, 2021) Nicolai, Lars; Biermann, Klaus; Trampert, Achim
    We present an electron tomography method for the comprehensive characterization of buried III-V semiconductor interfaces that is based on chemical-sensitive high-angle annular dark-field scanning transmission electron microscopy. For this purpose, an (Al,Ga)As/GaAs multi-layer system grown by molecular beam epitaxy is used as a case study. Isoconcentration surfaces are exploited to obtain topographic height maps of 120 nm × 120 nm area, revealing the interface morphology. By applying the height-height correlation function, we are able to determine important interface properties like root mean square roughness and lateral correlation length of various interfaces of the (Al,Ga)As/GaAs system characterized by different Al concentrations. Height-difference maps based on isosurfaces corresponding to 30% and 70% of the total compositional difference at the interfaces are used to create topographic maps of the interface width and to calculate an average interface width. This methodology proves differences in the properties of direct and inverted interfaces and allows the observation of interfacial anisotropies. © 2021
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    Terahertz quantum-cascade lasers for high-resolution absorption spectroscopy of atoms and ions in plasmas
    (Bristol : IOP Publ., 2023) Lü, X.; Röben, B.; Biermann, K.; Wubs, J.R.; Macherius, U.; Weltmann, K.-D.; van Helden, J.H.; Schrottke, L.; Grahn, H.T.
    We report on terahertz (THz) quantum-cascade lasers (QCLs) based on GaAs/AlAs heterostructures, which exhibit single-mode emission at 3.360, 3.921, and 4.745 THz. These frequencies are in close correspondence to fine-structure transitions of Al atoms, N+ ions, and O atoms, respectively. Due to the low electrical pump power of these THz QCLs, they can be operated in a mechanical cryocooler in continuous-wave mode, while a sufficient intrinsic tuning range of more than 5 GHz is maintained. The single-mode operation and the intrinsic tuning range of these THz QCLs allow for the application of these lasers as radiation sources for high-resolution absorption spectroscopy to determine the absolute densities of Al atoms, N+ ions, and O atoms in plasmas.
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    Mirror-symmetric Magneto-optical Kerr Rotation using Visible Light in [(GeTe)2(Sb2Te3)1]n Topological Superlattices
    (London : Nature Publishing, 2014) Bang, Do; Awano, Hiroyuki; Tominaga, Junji; Kolobov, Alexander V.; Fons, Paul; Saito, Yuta; Makino, Kotaro; Nakano, Takashi; Hase, Muneaki; Takagaki, Yukihiko; Giussani, Alessandro; Calarco, Raffaella; Murakami, Shuichi
    Interfacial phase change memory (iPCM), that has a structure of a superlattice made of alternating atomically thin GeTe and Sb2Te3 layers, has recently attracted attention not only due to its superior performance compared to the alloy of the same average composition in terms of energy consumption but also due to its strong response to an external magnetic field (giant magnetoresistance) that has been speculated to arise from switching between topological insulator (RESET) and normal insulator (SET) phases. Here we report magneto-optical Kerr rotation loops in the visible range, that have mirror symmetric resonances with respect to the magnetic field polarity at temperatures above 380 K when the material is in the SET phase that has Kramers-pairs in spin-split bands. We further found that this threshold temperature may be controlled if the sample was cooled in a magnetic field. The observed results open new possibilities for use of iPCM beyond phase-change memory applications.
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    Sub-nanometre resolution of atomic motion during electronic excitation in phase-change materials
    (London : Nature Publishing, 2016) Mitrofanov, Kirill V.; Fons, Paul; Makino, Kotaro; Terashima, Ryo; Shimada, Toru; Kolobov, Alexander, V.; Tominaga, Junji; Bragaglia, Valeria; Giussani, Alessandro; Calarco, Raffaella; Riechert, Henning; Sato, Takahiro; Katayama, Tetsuo; Ogawa, Kanade; Togashi, Tadashi; Yabashi, Makina; Wall, Simon; Brewe, Dale; Hase, Muneaki
    Phase-change materials based on Ge-Sb-Te alloys are widely used in industrial applications such as nonvolatile memories, but reaction pathways for crystalline-to-amorphous phase-change on picosecond timescales remain unknown. Femtosecond laser excitation and an ultrashort x-ray probe is used to show the temporal separation of electronic and thermal effects in a long-lived (>100 ps) transient metastable state of Ge2Sb2Te5 with muted interatomic interaction induced by a weakening of resonant bonding. Due to a specific electronic state, the lattice undergoes a reversible nondestructive modification over a nanoscale region, remaining cold for 4 ps. An independent time-resolved x-ray absorption fine structure experiment confirms the existence of an intermediate state with disordered bonds. This newly unveiled effect allows the utilization of non-thermal ultra-fast pathways enabling artificial manipulation of the switching process, ultimately leading to a redefined speed limit and improved energy efficiency and reliability of phase-change memory technologies.
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    Far-infrared and Raman spectroscopy investigation of phonon modes in amorphous and crystalline epitaxial GeTe-Sb2Te3 alloys
    (London : Nature Publishing Group, 2016) Bragaglia, V.; Holldack, K.; Boschker, J.E.; Arciprete, F.; Zallo, E.; Flissikowski, T.; Calarco, R.
    A combination of far-infrared and Raman spectroscopy is employed to investigate vibrational modes and the carrier behavior in amorphous and crystalline ordered GeTe-Sb2Te3 alloys (GST) epitaxially grown on Si(111). The infrared active GST mode is not observed in the Raman spectra and vice versa, indication of the fact that inversion symmetry is preserved in the metastable cubic phase in accordance with the Fm3 space group. For the trigonal phase, instead, a partial symmetry break due to Ge/Sb mixed anion layers is observed. By studying the crystallization process upon annealing with both the techniques, we identify temperature regions corresponding to the occurrence of different phases as well as the transition from one phase to the next. Activation energies of 0.43 eV and 0.08 eV for the electron conduction are obtained for both cubic and trigonal phases, respectively. In addition a metal-insulator transition is clearly identified to occur at the onset of the transition between the disordered and the ordered cubic phase.
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    Effect of Ge-doping on the short-wave, mid- and far-infrared intersubband transitions in GaN/AlGaN heterostructures
    (Bristol : IOP, 2017) Lim, Carolin B.; Ajay, Akhil; Lähnemann, Jonas; Bougerol, Catherine; Monroy, Eva
    This paper assesses the effects of Ge-doping on the structural and optical (band-to-band and intersubband (ISB)) properties of GaN/AlGaN multi-quantum wells (QWs) designed to display ISB absorption in the short-wave, mid- and far-infrared ranges (SWIR, MIR, and FIR, respectively). The standard c-plane crystallographic orientation is considered for wells absorbing in the SWIR and MIR spectral regions, whereas the FIR structures are grown along the nonpolar m-axis. In all cases, we compare the characteristics of Ge-doped and Si-doped samples with the same design and various doping levels. The use of Ge appears to improve the mosaicity of the highly lattice-mismatched GaN/AlN heterostructures. However, when reducing the lattice mismatch, the mosaicity is rather determined by the substrate and does not show any dependence on the dopant nature or concentration. From the optical point of view, by increasing the dopant density, we observe a blueshift of the photoluminescence in polar samples due to the screening of the internal electric field by free carriers. In the ISB absorption, on the other hand, there is a systematic improvement of the linewidth when using Ge as a dopant for high doping levels, whatever the spectral region under consideration (i.e. different QW size, barrier composition and crystallographic orientation).
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    Role of interfaces on the stability and electrical properties of Ge2Sb2Te5 crystalline structures
    (London : Nature Publishing Group, 2017) Mio, A.M.; Privitera, S.M.S.; Bragaglia, V.; Arciprete, F.; Cecchi, S.; Litrico, G.; Persch, C.; Calarco, R.; Rimini, E.
    GeSbTe-based materials exhibit multiple crystalline phases, from disordered rocksalt, to rocksalt with ordered vacancy layers, and to the stable trigonal phase. In this paper we investigate the role of the interfaces on the structural and electrical properties of Ge2Sb2Te5. We find that the site of nucleation of the metastable rocksalt phase is crucial in determining the evolution towards vacancy ordering and the stable phase. By properly choosing the substrate and the capping layers, nucleation sites engineering can be obtained, thus promoting or preventing the vacancy ordering in the rocksalt structure or the conversion into the trigonal phase. The vacancy ordering occurs at lower annealing temperatures (170 °C) for films deposited in the amorphous phase on silicon (111), compared to the case of SiO2 substrate (200 °C), or in presence of a capping layer (330 °C). The mechanisms governing the nucleation have been explained in terms of interfacial energies. Resistance variations of about one order of magnitude have been measured upon transition from the disordered to the ordered rocksalt structure and then to the trigonal phase. The possibility to control the formation of the crystalline phases characterized by marked resistivity contrast is of fundamental relevance for the development of multilevel phase change data storage.