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- ItemMixed dysprosium-lanthanide nitride clusterfullerenes DyM2N@C80-: I h and Dy2MN@C80- i h (M = Gd, Er, Tm, and Lu): Synthesis, molecular structure, and quantum motion of the endohedral nitrogen atom(Cambridge : RSC Publ., 2019) Schlesier, C.; Liu, F.; Dubrovin, V.; Spree, L.; Büchner, B.; Avdoshenko, S.M.; Popov, A.A.Systematic exploration of the synthesis of mixed-metal Dy-M nitride clusterfullerenes (NCFs, M = Gd, Er, Tm, Lu) is performed, and the impact of the second metal on the relative yield is evaluated. We demonstrate that the ionic radius of the metal appears to be the main factor allowing explanation of the relative yields in Dy-M mixed-metal systems with M = Sc, Lu, Er, and Gd. At the same time, Dy-Tm NCFs show anomalously low yields, which is not consistent with the relatively small ionic radius of Tm3+ but can be explained by the high third ionization potential of Tm. Complete separation of Dy-Gd and Dy-Er, as well as partial separation of Dy-Lu M3N@C80 nitride clusterfullerenes, is accomplished by recycling HPLC. The molecular structures of DyGd2N@C80 and DyEr2N@C80 are analyzed by means of single-crystal X-ray diffraction. A remarkable ordering of mixed-metal nitride clusters is found despite similar size and electronic properties of the metals. Possible pyramidalization of the nitride clusters in these and other nitride clusterfullerenes is critically analyzed with the help of DFT calculations and reconstruction of the nitrogen inversion barrier in M3N@C80 molecules is performed. Although a double-well potential with a pyramidal cluster structure is found to be common for most of them, the small size of the inversion barrier often leads to an apparent planar structure of the cluster. This situation is found for those M3N@C80 molecules in which the energy of the lowest vibrational level exceeds that of the inversion barrier, including Dy3N@C80 and DyEr2N@C80. The genuine pyramidal structure can be observed by X-ray diffraction only when the lowest vibrational level is below the inversion barrier, such as those found in Gd3N@C80 and DyGd2N@C80. The quantum nature of molecular vibrations becomes especially apparent when the size of the inversion barrier is comparable to the energy of the lowest vibrational levels.
- 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.
- ItemAnalysis of electronic properties frommagnetotransport measurements on Ba(Fe1-xNix)2As2 thin films(Basel : MDPI AG, 2020) Shipulin, I.; Richter, S.; Thomas, A.A.; Nielsch, K.; Hühne, R.; Martovitsky, V.We performed a detailed structural, magnetotransport, and superconducting analysis of thin epitaxial Ba(Fe1-xNix)2As2 films with Ni doping of x = 0.05 and 0.08, as prepared by pulsed laser deposition. X-ray diffraction studies demonstrate the high crystalline perfection of the films, which have a similar quality to single crystals. Furthermore, magnetotransport measurements of the films were performed in magnetic fields up to 9 T. The results we used to estimate the density of electronic states at the Fermi level, the coefficient of electronic heat capacity, and other electronic parameters for this compound, in their dependence on the dopant concentration within the framework of the Ginzburg-Landau-Abrikosov-Gorkov theory. The comparison of the determined parameters with measurement data on comparable Ba(Fe1-xNix)2As2 single crystals shows good agreement, which confirms the high quality of the obtained films.
- ItemLayered manganese bismuth tellurides with GeBi4Te7- and GeBi6Te10-type structures: Towards multifunctional materials(London : RSC Publ., 2019) Souchay, Daniel; Nentwig, Markus; Günther, Daniel; Keilholz, Simon; de Boor, Johannes; Zeugner, Alexander; Isaeva, Anna; Ruck, Michael; Wolter, Anja U.B.; Büchnerde, Bernd; Oeckler, OliverThe crystal structures of new layered manganese bismuth tellurides with the compositions Mn0.85(3)Bi4.10(2)Te7 and Mn0.73(4)Bi6.18(2)Te10 were determined by single-crystal X-ray diffraction, including the use of microfocused synchrotron radiation. These analyses reveal that the layered structures deviate from the idealized stoichiometry of the 12P-GeBi4Te7 (space group P3m1) and 51R-GeBi6Te10 (space group R3m) structure types they adopt. Modified compositions Mn1-xBi4+2x/3Te7 (x = 0.15-0.2) and Mn1-xBi6+2x/3Te10 (x = 0.19-0.26) assume cation vacancies and lead to homogenous bulk samples as confirmed by Rietveld refinements. Electron diffraction patterns exhibit no diffuse streaks that would indicate stacking disorder. The alternating quintuple-layer [M2Te3] and septuple-layer [M3Te4] slabs (M = mixed occupied by Bi and Mn) with 1 : 1 sequence (12P stacking) in Mn0.85Bi4.10Te7 and 2 : 1 sequence (51R stacking) in Mn0.81Bi6.13Te10 were also observed in HRTEM images. Temperature-dependent powder diffraction and differential scanning calorimetry show that the compounds are high-temperature phases, which are metastable at ambient temperature. Magnetization measurements are in accordance with a MnII oxidation state and point at predominantly ferromagnetic coupling in both compounds. The thermoelectric figures of merit of n-type conducting Mn0.85Bi4.10Te7 and Mn0.81Bi6.13Te10 reach zT = 0.25 at 375 °C and zT = 0.28 at 325 °C, respectively. Although the compounds are metastable, compact ingots exhibit still up to 80% of the main phases after thermoelectric measurements up to 400 °C. © The Royal Society of Chemistry 2019.
- ItemDirect Observation of Shock-Induced Disordering of Enstatite Below the Melting Temperature(Hoboken, NJ [u.a.] : Wiley, 2020) Hernandez, J.-A.; Morard, G.; Guarguaglini, M.; Alonso-Mori, R.; Benuzzi-Mounaix, A.; Bolis, R.; Fiquet, G.; Galtier, E.; Gleason, A.E.; Glenzer, S.; Guyot, F.; Ko, B.; Lee, H.J.; Mao, W.L.; Nagler, B.; Ozaki, N.; Schuster, A.K.; Shim, S.H.; Vinci, T.; Ravasio, A.We report in situ structural measurements of shock-compressed single crystal orthoenstatite up to 337 ± 55 GPa on the Hugoniot, obtained by coupling ultrafast X-ray diffraction to laser-driven shock compression. Shock compression induces a disordering of the crystalline structure evidenced by the appearance of a diffuse X-ray diffraction signal at nanosecond timescales at 80 ± 13 GPa on the Hugoniot, well below the equilibrium melting pressure (>170 GPa). The formation of bridgmanite and post-perovskite have been indirectly reported in microsecond-scale plate-impact experiments. Therefore, we interpret the high-pressure disordered state we observed at nanosecond scale as an intermediate structure from which bridgmanite and post-perovskite crystallize at longer timescales. This evidence of a disordered structure of MgSiO3 on the Hugoniot indicates that the degree of polymerization of silicates is a key parameter to constrain the actual thermodynamics of shocks in natural environments. © 2020. The Authors.
- Item500,000 Years of Environmental History in Eastern Anatolia: The PALEOVAN Drilling Project(Sapporo : IODP, 2012) Litt, T.; Anselmetti, F.S.; Baumgarten, H.; Beer, J.; Cagatay, N.; Cukur, D.; Damci, E.; Glombitza, C.; Haug, G.; Heumann, G.; Kallmeyer, H.; Kipfer, R.; Krastel, S.; Kwiecien, O.; Meydan, A.F.; Orcen, S.; Pickarski, N.; Randlett, M.-E.; Schmincke, H.-U.; Schubert, C.J.; Sturm, M.; Sumita, M.; Stockhecke, M.; Tomonaga, Y.; Vigliotti, L.; Wonik, T.International Continental Scientific Drilling Program (ICDP) drilled a complete succession of the lacustrine sediment sequence deposited during the last ~500,000 years in Lake Van, Eastern Anatolia (Turkey). Based on a detailed seismic site survey, two sites at a water depth of up to 360 m were drilled in summer 2010, and cores were retrieved from sub-lake-floor depths of 140 m (Northern Basin) and 220 m (Ahlat Ridge). To obtain a complete sedimentary section, the two sites were multiple-cored in order to investigate the paleoclimate history of a sensitive semi-arid region between the Black, Caspian, and Mediterranean seas. Further scientific goals of the PALEOVAN project are the reconstruction of earthquake activity, as well as the temporal, spatial, and compositional evolution of volcanism as reflected in the deposition of tephra layers. The sediments host organic matter from different sources and hence composition, which will be unravelled using biomarkers. Pathways for migration of continental and mantle-derived noble gases will be analyzed in pore waters. Preliminary 40Ar/39Ar single crystal dating of tephra layers and pollen analyses suggest that the Ahlat Ridge record encompasses more than half a million years of paleoclimate and volcanic/geodynamic history, providing the longest continental record in the entire Near East to date.
- ItemMagnetic field and angle-dependent photoluminescence of a fiber-coupled nitrogen vacancy rich diamond(Melville, NY : American Inst. of Physics, 2021) Wunderlich, Ralf; Staacke, Robert; Knolle, Wolfgang; Abel, Bernd; Meijer, JanHere, we investigate the magnetic field dependent photoluminescence (PL) of a fiber-coupled diamond single crystal with a high density of nitrogen vacancy (NV) centers. Angle-dependent magnetic field sweep measurements between 0 and 111 mT were performed using an oscillating illumination combined with lock-in techniques. Besides the expected superposed PL of differently oriented NV centers, a zoo of features in the PL are found. These features can be associated with level anti-crossings and cross relaxations. In particular, PL measurements allowed us to detect auto-cross relaxation between coupled NV centers. Moreover, the PL measurements at low magnetic fields show dips suggesting an interaction of NV centers with additional spin defects. The results presented here are not only a study for NV-based fiber-coupled sensors made of diamond, but also show a way to investigate with manageable effort and purely an optical multispin interaction with at least one NV center as a constituent.
- ItemInvestigating the magnetic and magnetocaloric behaviors of LiSm(PO3)4(London : RSC Publishing, 2023) Tran, T.A.; Petrov, Dimitar N.; Phan, T.L.; Tu, B. D.; Nhat, H.N.; Tran, H.C.; Weise, B.; Cwik, J.; Koshkid'ko, Yu S.; Manh, T.V.; Hoang, T.P.; Dang, N.T.We report a detailed study on the magnetic behaviors and magnetocaloric (MC) effect of a single crystal of lithium samarium tetraphosphate, LiSm(PO3)4. The analyses of temperature-dependent magnetization data have revealed magnetic ordering established with decreasing temperature below Tp, where Tp is the minimum of a dM/dT vs. T curve and varies as a linear function of the applied field H. The Curie temperature has been extrapolated from Tp(H) data, as H → 0, to be about 0.51 K. The establishment of magnetic-ordering causes a substantial change in the heat capacity Cp. Above Tp, the crystal exhibits paramagnetic behavior. Using the Curie-Weiss (CW) law and Arrott plots, we have found the crystal to have a CW temperature θCW ≈ −36 K, and short-range magnetic order associated with a coexistence of antiferromagnetic and ferromagnetic interactions ascribed to the couplings of magnetic dipoles and octupoles at the Γ7 and Γ8 states. An assessment of the MC effect has shown increases in value of the absolute magnetic-entropy change (|ΔSm|) and adiabatic-temperature change (ΔTad) when lowering the temperature to 2 K, and increasing the magnetic-field H magnitude. Around 2 K, the maximum value of |ΔSm| is about 3.6 J kg−1 K−1 for the field H = 50 kOe, and ΔTad is about 5.8 K for H = 20 kOe, with the relative cooling power (RCP) of ∼82.5 J kg−1. In spite of a low MC effect in comparison to Li(Gd,Tb,Ho)(PO3)4, the absence of magnetic hysteresis reflects that LiSm(PO3)4 is also a candidate for low-temperature MC applications below 25 K.
- ItemTowards time resolved core level photoelectron spectroscopy with femtosecond x-ray free-electron lasers(College Park, MD : Institute of Physics Publishing, 2008) Pietzsch, A.; Föhlisch, A.; Beye, M.; Deppe, M.; Hennies, F.; Nagasono, M.; Suljotil, E.; Wurth, W.; Gahl, C.; Dörich, K.; Melnikov, A.We have performed core level photoelectron spectroscopy on a W(110) single crystal with femtosecond XUV pulses from the free-electron laser at Hamburg (FLASH). We demonstrate experimentally and through theoretical modelling that for a suitable range of photon fluences per pulse, time-resolved photoemission experiments on solid surfaces are possible. Using FLASH pulses in combination with a synchronized optical laser, we have performed femtosecond time-resolved core-level photoelectron spectroscopy and observed sideband formation on the W 4f lines indicating a cross correlation between femtosecond optical and XUV pulses. © IOP Publishing Ltd and Deutsche Physikalische Gesellschaft.
- ItemSpin-glass state and reversed magnetic anisotropy induced by Cr doping in the Kitaev magnet α-RuCl3(College Park, MD : American Physical Society, 2019) Bastien, G.; Roslova, M.; Haghighi, M.H.; Mehlawat, K.; Hunger, J.; Isaeva, A.; Doert, T.; Vojta, M.; Büchner, B.; Wolter, A.U.B.Magnetic properties of the substitution series Ru1-xCrxCl3 were investigated to determine the evolution from the anisotropic Kitaev magnet α-RuCl3 with Jeff=1/2 magnetic Ru3+ ions to the isotropic Heisenberg magnet CrCl3 with S=3/2 magnetic Cr3+ ions. Magnetization measurements on single crystals revealed a reversal of the magnetic anisotropy under doping, which we argue to arise from the competition between anisotropic Kitaev and off-diagonal interactions on the Ru-Ru links and approximately isotropic Cr-Ru and isotropic Cr-Cr interactions. In addition, combined magnetization, ac susceptibility, and specific-heat measurements clearly show the destabilization of the long-range magnetic order of α-RuCl3 in favor of a spin-glass state of Ru1-xCrxCl3 for a low doping of x≤0.1. The corresponding freezing temperature as a function of Cr content shows a broad maximum around x ≤ 0.45.