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- ItemHigh-quality MgB2 nanocrystals synthesized by using modified amorphous nano-boron powders: Study of defect structures and superconductivity properties(College Park, MD : American Institute of Physics, 2019) Bateni, A.; Erdem, E.; Häßler, W.; Somer, M.Nano sized magnesium diboride (MgB2) samples were synthesized using various high-quality nano-B precursor powders. The microscopic defect structures of MgB2 samples were systematically investigated using X-ray powder diffraction, Raman, resistivity measurements and electron paramagnetic resonance spectroscopy. A significant deviation in the critical temperature Tc was observed due to defects and crystal distortion. The symmetry effect of the latter is also reflected on the vibrational modes in the Raman spectra. Scanning electron microscopy analysis demonstrate uniform and ultrafine morphology for the modified MgB2. Defect center in particular Mg vacancies influence the connectivity and the conductivity properties which are crucial for the superconductivity applications.
- ItemMetallofullerene photoswitches driven by photoinduced fullerene-to-metal electron transfer(Cambridge : RSC, 2021) Zalibera, Michal; Ziegs, Frank; Schiemenz, Sandra; Dubrovin, Vasilii; Lubitz, Wolfgang; Savitsky, Anton; Deng, Shihu H.M.; Wang, Xue-Bin; Advoshenko, Stanislav M.; Popov, Alexey A.We report on the discovery and detailed exploration of the unconventional photo-switching mechanism in metallofullerenes, in which the energy of the photon absorbed by the carbon cage π-system is transformed to mechanical motion of the endohedral cluster accompanied by accumulation of spin density on the metal atoms. Comprehensive photophysical and electron paramagnetic resonance (EPR) studies augmented by theoretical modelling are performed to address the phenomenon of the light-induced photo-switching and triplet state spin dynamics in a series of YxSc3−xN@C80 (x = 0–3) nitride clusterfullerenes. Variable temperature and time-resolved photoluminescence studies revealed a strong dependence of their photophysical properties on the number of Sc atoms in the cluster. All molecules in the series exhibit temperature-dependent luminescence assigned to the near-infrared thermally-activated delayed fluorescence (TADF) and phosphorescence. The emission wavelengths and Stokes shift increase systematically with the number of Sc atoms in the endohedral cluster, whereas the triplet state lifetime and S1–T1 gap decrease in this row. For Sc3N@C80, we also applied photoelectron spectroscopy to obtain the triplet state energy as well as the electron affinity. Spin distribution and dynamics in the triplet states are then studied by light-induced pulsed EPR and ENDOR spectroscopies. The spin–lattice relaxation times and triplet state lifetimes are determined from the temporal evolution of the electron spin echo after the laser pulse. Well resolved ENDOR spectra of triplets with a rich structure caused by the hyperfine and quadrupolar interactions with 14N, 45Sc, and 89Y nuclear spins are obtained. The systematic increase of the metal contribution to the triplet spin density from Y3N to Sc3N found in the ENDOR study points to a substantial fullerene-to-metal charge transfer in the excited state. These experimental results are rationalized with the help of ground-state and time-dependent DFT calculations, which revealed a substantial variation of the endohedral cluster position in the photoexcited states driven by the predisposition of Sc atoms to maximize their spin population.
- ItemImpact of plasma jet vacuum ultraviolet radiation on reactive oxygen species generation in bio-relevant liquids([S.l.] : American Institute of Physics, 2015) Jablonowski, H.; Bussiahn, R.; Hammer, M.U.; Weltmann, K.-D.; von Woedtke, T.; Reuter, S.Plasma medicine utilizes the combined interaction of plasma produced reactive components. These are reactive atoms, molecules, ions, metastable species, and radiation. Here, ultraviolet (UV, 100–400 nm) and, in particular, vacuum ultraviolet (VUV, 10–200 nm) radiation generated by an atmospheric pressure argon plasma jet were investigated regarding plasma emission, absorption in a humidified atmosphere and in solutions relevant for plasma medicine. The energy absorption was obtained for simple solutions like distilled water (dH2O) or ultrapure water and sodium chloride (NaCl) solution as well as for more complex ones, for example, Rosewell Park Memorial Institute (RPMI 1640) cell culture media. As moderate stable reactive oxygen species, hydrogen peroxide (H2O2) was studied. Highly reactive oxygen radicals, namely, superoxide anion (O2•−) and hydroxyl radicals (•OH), were investigated by the use of electron paramagnetic resonance spectroscopy. All species amounts were detected for three different treatment cases: Plasma jet generated VUV and UV radiation, plasma jet generated UV radiation without VUV part, and complete plasma jet including all reactive components additionally to VUV and UV radiation. It was found that a considerable amount of radicals are generated by the plasma generated photoemission. From the experiments, estimation on the low hazard potential of plasma generated VUV radiation is discussed.
- ItemPentacene in 1,3,5-Tri(1-naphtyl)benzene: A Novel Standard for Transient EPR Spectroscopy at Room Temperature(Wien [u.a.] : Springer, 2021) Schröder, Mirjam; Rauber, Daniel; Matt, Clemens; Kay, Christopher W. M.Testing and calibrating an experimental setup with standard samples is an essential aspect of scientific research. Single crystals of pentacene in p-terphenyl are widely used for this purpose in transient electron paramagnetic resonance (EPR) spectroscopy. However, this sample is not without downsides: the crystals need to be grown and the EPR transitions only appear at particular orientations of the crystal with respect to the external magnetic field. An alternative host for pentacene is the glass-forming 1,3,5-tri(1-naphtyl)benzene (TNB). Due to the high glass transition point of TNB, an amorphous glass containing randomly oriented pentacene molecules is obtained at room temperature. Here we demonstrate that pentacene dissolved in TNB gives a typical “powder-like” transient EPR spectrum of the triplet state following pulsed laser excitation. From the two-dimensional data set, it is straightforward to obtain the zero-field splitting parameters and relative populations by spectral simulation as well as the B1 field in the microwave resonator. Due to the simplicity of preparation, handling and stability, this system is ideal for adjusting the laser beam with respect to the microwave resonator and for introducing students to transient EPR spectroscopy. © 2021, The Author(s).
- ItemThe interplay between spin densities and magnetic superexchange interactions: Case studies of monoand trinuclear bis(oxamato)-type complexes(Frankfurt am Main : Beilstein-Institut zur Förderung der Chemischen Wissenschaften, 2017) Aliabadi, A.; Büchner, B.; Kataev, V.; Rüffer, T.For future molecular spintronic applications the possibility to modify and tailor the magnetic properties of transition-metal complexes is very promising. One of such possibilities is given by the countless derivatization offered by carbon chemistry. They allow for altering chemical structures and, in doing so, to tune magnetic properties of molecular spin-carrying compounds. With emphasis on the interplay of the spin density distribution of mononuclear and magnetic superexchange couplings of trinuclear bis(oxamato)- type complexes we review on efforts on such magneto-structural correlations.
- ItemHigh-field ESR studies of the quantum spin magnet CaCu2O 3(Milton Park : Taylor & Francis, 2006) Goiran, M.; Costes, M.; Broto, J.M.; Chou, F.C.; Klingeler, R.; Arushanov, E.; Drechsler, S.-L.; Büchner, B.; Kataev, V.We report an electron spin resonance (ESR) study of the s = 1/2 Heisenberg pseudo-ladder magnet CaCu2O3 in pulsed magnetic fields up to 40 T. At sub-terahertz frequencies we observe an ESR signal originating from a small amount of uncompensated spins residing presumably at the imperfections of the strongly antiferromagnetically correlated host spin lattice. The data give evidence that these few per cent of 'extra' spin states are coupled strongly to the bulk spins and are involved in the antiferromagnetic (AF) ordering at TN = 25 K. By mapping the frequency/resonance field diagram we have determined a small gap for magnetic excitations below TN of the order of ~0.3–0.8 meV. Such a small value of the gap explains the occurrence of the spin-flop transition in CaCu2O3 at weak magnetic fields μ0Hsf ~ 3 T. Qualitative changes of the ESR response with the increasing field strength give indications that strong magnetic fields reduce the AF correlations and may even suppress the long-range magnetic order in CaCu2O3. ESR data support scenarios with a significant role of the 'extra' spin states for the properties of low-dimensional quantum magnets.