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- ItemTuning the Properties and Self-Healing Behavior of Ionically Modified Poly(isobutylene-co-isoprene) Rubber(Washington, DC : Soc., 2017) Suckow, Marcus; Mordvinkin, Anton; Roy, Manta; Singha, Nikhil K.; Heinrich, Gert; Voit, Brigitte; Saalwächter, Kay; Böhme, FrankThe focus of this work is on the nature of self-healing of ionically modified rubbers obtained by reaction of brominated poly(isobutylene-co-isoprene) rubber (BIIR) with various alkylimidazoles such as 1-methylimidazole, 1-butylimidazole, 1-hexylimidazole, 1-nonylimidazole, and 1-(6-chlorohexyl)-1H-imidazole. Based on stress-strain and temperature dependent DMA measurements, a structural influence of the introduced ionic imidazolium moieties on the formation of ionic clusters and, as a consequence, on the mechanical strength and self-healing behavior of the samples could be evidenced. These results are fully supported by a molecular-level assessment of the network structure (cross-link and constraint density) and the dynamics of the ionic clusters using an advanced proton low-field NMR technique. The results show distinct correlations between the macroscopic behavior and molecular chain dynamics of the modified rubbers. In particular, it is shown that the optimization of material properties with regard to mechanical and self-healing behavior is limited by opposing tendencies. Samples with reduced chain dynamics exhibit superior mechanical behavior but lack on self-healing behavior. In spite of these limitations, the overall performance of some of our samples including self-healing behavior exceeds distinctly that of other self-healing rubbers described in the literature so far.
- 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.
- ItemEntropy driven chain effects on ligation chemistry(Cambridge : RSC, 2014) Pahnke, Kai; Brandt, Josef; Gryn'ova, Ganna; Lindner, Peter; Schweins, Ralf; Schmidt, Friedrich Georg; Lederer, Albena; Coote, Michelle L.; Barner-Kowollik, ChristopherWe report the investigation of fundamental entropic chain effects that enable the tuning of modular ligation chemistry – for example dynamic Diels–Alder (DA) reactions in materials applications – not only classically via the chemistry of the applied reaction sites, but also via the physical and steric properties of the molecules that are being joined. Having a substantial impact on the reaction equilibrium of the reversible ligation chemistry, these effects are important when transferring reactions from small molecule studies to larger or other entropically very dissimilar systems. The effects on the DA equilibrium and thus the temperature dependent degree of debonding (%debond) of different cyclopentadienyl (di-)functional poly(meth-)acrylate backbones (poly(methyl methacrylate), poly(iso-butyl methacrylate), poly(tert-butyl methacrylate), poly(iso-butyl acrylate), poly(n-butyl acrylate), poly(tert-butyl acrylate), poly(methyl acrylate) and poly(isobornyl acrylate)), linked via a difunctional cyanodithioester (CDTE) were examined via high temperature (HT) NMR spectroscopy as well as temperature dependent (TD) SEC measurements. A significant impact of not only chain mass and length with a difference in the degree of debonding of up to 30% for different lengths of macromonomers of the same polymer type but – remarkably – as well the chain stiffness with a difference in bonding degrees of nearly 20% for isomeric poly(butyl acrylates) is found. The results were predicted, reproduced and interpreted via quantum chemical calculations, leading to a better understanding of the underlying entropic principles.
- ItemHigh-temperature electromechanical loss in piezoelectric langasite and catangasite crystals(Melville, NY : American Inst. of Physics, 2021) Suhak, Yuriy; Fritze, Holger; Sotnikov, Andrei; Schmidt, Hagen; Johnson, Ward L.Temperature-dependent acoustic loss Q−1 is studied in partially disordered langasite (LGS, La3Ga5SiO14) and ordered catangasite (CTGS, Ca3TaGa3Si2O14) crystals and compared with previously reported CTGS and langatate (LGT, La3Ga5.5Ta0.5O14) data. Two independent techniques, a contactless tone-burst excitation technique and contacting resonant piezoelectric spectroscopy, are used in this study. Contributions to the measured Q−1(T) are determined through fitting to physics-based functions, and the extracted fit parameters, including the activation energies of the processes, are discussed. It is shown that losses in LGS and CTGS are caused by a superposition of several mechanisms, including intrinsic phonon–phonon loss, point-defect relaxations, and conductivity-related relaxations.
- ItemUltrafast structural changes in SrTiO3 due to a superconducting phase transition in a YBa2Cu3O7 top layer(College Park, MD : Institute of Physics Publishing, 2010) Lübcke, A.; Zamponi, F.; Loetzsch, R.; Kämpfer, T.; Uschmann, I.; Große, V.; Schmidl, F.; Köttig, T.; Thürk, M.; Schwoerer, H.; Förster, E.; Seidel, P.; Sauerbrey, R.We investigate the structural response of SrTiO3 when Cooper pairs are broken in an epitaxially grown YBa2Cu3O 7 top layer due to both heating and optical excitation. The crystal structure is investigated by static, temperaturedependent and time-resolved x-ray diffraction. In the static case, a large strain field in SrTiO3 is formed in the proximity of the onset of the superconducting phase in the top layer, suggesting a relationship between both effects. For the time-dependent studies, we likewise find a large fraction of the probed volume of the SrTiO3 substrate strained if the top layer is superconducting. Upon optical breaking of Cooper pairs, the observed width of the rocking curve is reduced and its position is slightly shifted towards smaller angles. The dynamical theory of x-ray diffraction is used to model the measured rocking curves. We find that the thickness of the strained layer is reduced by about 200 nm on a sub-ps to ps timescale, but the strain value at the interface between SrTiO3 and YBa2Cu3O7 remains unaffected. © IOP Publishing Ltd and Deutsche Physikalische Gesellschaft.
- ItemResolving ecological feedbacks on the ocean carbon sink in Earth system models(Göttingen : Copernicus Publ., 2021) Armstrong McKay, David I.; Cornell, Sarah E.; Richardson, Katherine; Rockström, JohanThe Earth's oceans are one of the largest sinks in the Earth system for anthropogenic CO2 emissions, acting as a negative feedback on climate change. Earth system models project that climate change will lead to a weakening ocean carbon uptake rate as warm water holds less dissolved CO2 and as biological productivity declines. However, most Earth system models do not incorporate the impact of warming on bacterial remineralisation and rely on simplified representations of plankton ecology that do not resolve the potential impact of climate change on ecosystem structure or elemental stoichiometry. Here, we use a recently developed extension of the cGEnIE (carbon-centric Grid Enabled Integrated Earth system model), ecoGEnIE, featuring a trait-based scheme for plankton ecology (ECOGEM), and also incorporate cGEnIE's temperature-dependent remineralisation (TDR) scheme. This enables evaluation of the impact of both ecological dynamics and temperature-dependent remineralisation on particulate organic carbon (POC) export in response to climate change. We find that including TDR increases cumulative POC export relative to default runs due to increased nutrient recycling (+∼1.3 %), whereas ECOGEM decreases cumulative POC export by enabling a shift to smaller plankton classes (−∼0.9 %). However, interactions with carbonate chemistry cause opposite sign responses for the carbon sink in both cases: TDR leads to a smaller sink relative to default runs (−∼1.0 %), whereas ECOGEM leads to a larger sink (+∼0.2 %). Combining TDR and ECOGEM results in a net strengthening of POC export (+∼0.1 %) and a net reduction in carbon sink (−∼0.7 %) relative to default. These results illustrate the degree to which ecological dynamics and biodiversity modulate the strength of the biological pump, and demonstrate that Earth system models need to incorporate ecological complexity in order to resolve non-linear climate–biosphere feedbacks.
- ItemSpectroscopy and 2.1 µm laser operation of Czochralski-grown Tm3+:YScO3 crystals(Washington, DC : Soc., 2022) Suzuki, Anna; Kalusniak, Sascha; Tanaka, Hiroki; Brützam, Mario; Ganschow, Steffen; Tokurakawa, Masaki; Kränkel, ChristianWe report on growth, temperature-dependent spectroscopy, and laser experiments of Tm3+-doped YScO3 mixed sesquioxide crystals. For the first time, cm3-scale laser quality Tm3+:YScO3 crystals with 2.2 at.% and 3.1 at.% doping levels were grown by the Czochralski method from iridium crucibles. We reveal that the structural disorder in the mixed crystals allows for broad and smooth spectral features even at cryogenic temperatures. We obtained the first continuous wave laser operation in this material at wavelengths around 2100 nm using a laser diode emitting at 780 nm as a pump source. A maximum slope efficiency of 45% was achieved using a Tm3 + (3.1 at.%):YScO3 crystal. Our findings demonstrate the high potential of Tm3+-doped mixed sesquioxides for efficient ultrafast pulse generation in the 2.1 µm range.
- ItemLaser cooling in Yb:KY3F10: a comparison with Yb:YLF(Washington, DC : Optica, 2022) Püschel, Stefan; Mauerhoff, Felix; Kränkel, Christian; Tanaka, HirokiLaser cooling by anti-Stokes fluorescence is a technology to realize all-solid-state optical cryocoolers. We grew Yb3+-doped KY3F10 (Yb:KYF) crystals as novel laser cooling media and compare their cooling performance to Yb3+-doped LiYF4 (Yb:YLF) crystals also grown in our institute. We present temperature-dependent absorption and emission cross sections as well as the fluorescence lifetime of Yb:KYF, and calculate its material figure-of-merit for laser cooling. Yb:KYF exhibits a higher figure-of-merit than Yb:YLF at temperatures below 200 K. This is because, in contrast to Yb:YLF, the excitation transition from the second-highest Stark level of the ground state is best-suited for cryogenic cooling in Yb:KYF. Thus, it has the potential to achieve unprecedentedly low temperatures below the boiling point of liquid nitrogen. In this work, we observe the first laser cooling of Yb:KYF, and obtain a background absorption coefficient of ∼10−4 cm−1, which is among the lowest ever reported for Yb3+-doped fluoride crystals. A simple model calculation predicts that our Yb:KYF and Yb:YLF crystals can potentially be cooled down to ≈100 K in a high-power cooling setup. Our Yb:KYF crystals still leave room for further improvement through the optimization of the growth process and the use of purer raw materials.
- ItemMomentum-resolved superconducting gap in the bulk of Ba1-xK xFe2As2 from combined ARPES and μSR measurements(Milton Park : Taylor & Francis, 2009) Evtushinsky, D.V.; Inosov, D.S.; Zabolotnyy, V.B.; Viazovska, M.S.; Khasanov, R.; Amato, A.; Klauss, H.-H.; Luetkens, H.; Niedermayer, Ch.; Sun, G.L.; Hinkov, V.; Lin, C.T.; Varykhalov, A.; Koitzsch, A.; Knupfer, M.; Büchner, B.; Kordyuk, A.A.; Borisenko, S.V.Here we present a calculation of the temperature-dependent London penetration depth, λ(T), in Ba1-xKxFe 2As2 (BKFA) on the basis of the electronic band structure (Zabolotnyy et al 2009 Nature 457 569, Zabolotnyy et al 2009 Physica C 469 448) and momentum-dependent superconducting gap (Evtushinsky et al 2009 Phys. Rev. B 79 054517) extracted from angleresolved photoemission spectroscopy (ARPES) data. The results are compared to the direct measurements of λ(T) by muon spin rotation (μSR) (Khasanov et al 2009 Phys. Rev. Lett. 102 187005). The value of λ(T = 0), calculated with no adjustable parameters, equals 270 nm, while the directly measured one is 320 nm; the temperature dependence λ(T) is also easily reproduced. Such agreement between the two completely different approaches allows us to conclude that ARPES studies of BKFA are bulk-representative. Our review of the available experimental studies of the superconducting gap in the new ironbased superconductors in general allows us to state that most of them bear two nearly isotropic gaps with coupling constants 2ΔkBTc = 2.5±1.5 and 7±2.
- ItemValence effect on the thermopower of Eu systems(College Park, MD : American Physical Society, 2020) Stockert, U.; Seiro, S.; Seiro, S.; Caroca-Canales, N.; Hassinger, E.; Hassinger, E.; Geibel, C.We investigated the thermoelectric transport properties of EuNi2P2 and EuIr2Si2 to evaluate the relevance of Kondo interaction and valence fluctuations in these materials. While the thermal conductivities behave conventionally, the thermopower curves exhibit large values with pronounced maxima as typically observed in Ce- and Yb-based heavy-fermion materials. However, neither the positions of these maxima nor the absolute thermopower values at low temperature are in line with the heavy-fermion scenario and the moderately enhanced effective charge carrier masses. Instead, we may relate the thermopower in our materials to the temperature-dependent Eu valence by taking into account changes in the chemical potential. Our analysis confirms that valence fluctuations play an important role in EuNi2P2 and EuIr2Si2.