2019, Yang, W., Velkos, G., Liu, F., Sudarkova, S.M., Wang, Y., Zhuang, J., Zhang, H., Li, X., Zhang, X., Büchner, B., Avdoshenko, S.M., Popov, A.A., Chen, N.

A new class of single-molecule magnets (SMMs) based on Dy-oxide clusterfullerenes is synthesized. Three isomers of Dy2O@C82 with Cs(6), C3v(8), and C2v(9) cage symmetries are characterized by single-crystal X-ray diffraction, which shows that the endohedral Dy−(µ2-O)−Dy cluster has bent shape with very short Dy−O bonds. Dy2O@C82 isomers show SMM behavior with broad magnetic hysteresis, but the temperature and magnetization relaxation depend strongly on the fullerene cage. The short Dy−O distances and the large negative charge of the oxide ion in Dy2O@C82 result in the very strong magnetic anisotropy of Dy ions. Their magnetic moments are aligned along the Dy−O bonds and are antiferromagnetically (AFM) coupled. At low temperatures, relaxation of magnetization in Dy2O@C82 proceeds via the ferromagnetically (FM)-coupled excited state, giving Arrhenius behavior with the effective barriers equal to the AFM-FM energy difference. The AFM-FM energy differences of 5.4–12.9 cm−1 in Dy2O@C82 are considerably larger than in SMMs with {Dy2O2} bridges, and the Dy∙∙∙Dy exchange coupling in Dy2O@C82 is the strongest among all dinuclear Dy SMMs with diamagnetic bridges. Dy-oxide clusterfullerenes provide a playground for the further tuning of molecular magnetism via variation of the size and shape of the fullerene cage.

2021, Graf, Lukas, Krupskaya, Yulia, Büchner, Bernd, Knupfer, Martin

We have experimentally determined the momentum dependence of the electronic excitation spectra of para-quaterphenyl single crystals. The parallel arrangement of para-quaterphenyl molecules results in a strong Coulomb coupling of the molecular excitons. Such crystals have been considered to be a very good realization of the Frenkel exciton model, including the formation of H-type aggregates. Our data reveal an unexpected exciton dispersion of the upper Davydov component, which cannot be rationalized in terms of inter-molecular Coulomb coupling of the excitons. A significant reduction of the nearest neighbor coupling due to additional charge-transfer processes is able to provide an explanation of the data. Furthermore, the spectral onset of the excitation spectrum, which represents a heavy exciton resulting from exciton-phonon coupling, also shows a clear dispersion, which had been unknown so far. Finally, an optically forbidden excitation about 1 eV above the excitation onset is observed. © 2021 Author(s).

2017, Patchkovskii, Serguei, Schuurman, Michael S.

We present derivation and implementation of the multiconfigurational strong-field approximation with Gaussian nuclear wave packets (MC-SFA-GWP) - a version of the molecular strong-field approximation which treats all electronic and nuclear degrees of freedom, including their correlations, quantum mechanically. The technique allows realistic simulation of high-order-harmonic emission in polyatomic molecules without invoking reduced-dimensionality models for the nuclear motion or the electronic structure. We use MC-SFA-GWP to model isotope effects in high-order-harmonic-generation (HHG) spectroscopy of methane. The HHG emission in this molecule transiently involves the strongly vibronically coupled F22 electronic state of the CH4+ cation. We show that the isotopic HHG ratio in methane contains signatures of (a) field-free vibronic dynamics at the conical intersection (CI); (b) resonant features in the recombination cross sections; (c) laser-driven bound-state dynamics; as well as (d) the well-known short-time Gaussian decay of the emission. We assign the intrinsic vibronic feature (a) to a relatively long-lived (≥4 fs) vibronic wave packet of the singly excited ν4 (t2) and ν2 (e) vibrational modes, strongly coupled to the components of the F22 electronic state. We demonstrate that these physical effects differ in their dependence on the wavelength, intensity, and duration of the driving pulse, allowing them to be disentangled. We thus show that HHG spectroscopy provides a versatile tool for exploring both conical intersections and resonant features in photorecombination matrix elements in the regime not easily accessible with other techniques.

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.

2017, Schumacher, P., Mayr, S.G., Rauschenbach, B.

Germanium thin films were deposited by Pulsed Laser Deposition (PLD) onto single crystal Ge (100) and Si (100) substrates with a native oxide film on the surface. The topography of the surface was investigated by Atomic Force Microscopy (AFM) to evaluate the scaling behavior of the surface roughness of amorphous and polycrystalline Ge films grown on substrates with different roughnesses. Roughness evolution was interpreted within the framework of stochastic rate equations for thin film growth. Here the Kardar-Parisi-Zhang equation was used to describe the smoothening process. Additionally, a roughening regime was observed in which 3-dimensional growth occurred. Diffusion of the deposited Ge adatoms controlled the growth of the amorphous Ge thin films. The growth of polycrystalline thin Ge films was dominated by diffusion processes only in the initial stage of the growth.

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.

2021, Suzuki, Anna, Kränkel, Christian, Tokurakawa, Masaki

We 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.

2020, Boy, Johannes, Handwerg, Martin, Mitdank, Rüdiger, Galazka, Zbigniew, Fischer, Saskia F.

The temperature dependence of the charge carrier density, mobility, and Seebeck coefficient of melt-grown, bulk ZnGa2O4 single crystals was measured between 10 K and 310 K. The electrical conductivity at room temperature is about σ = 286 S/cm due to a high electron concentration of n = 3.26 × 1019 cm−3 caused by unintentional doping. The mobility at room temperature is μ = 55 cm2/V s, whereas the scattering on ionized impurities limits the mobility to μ = 62 cm2/Vs for temperatures lower than 180 K. The Seebeck coefficient relative to aluminum at room temperature is SZnGa2O4−Al = (−125 ± 2) μV/K and shows a temperature dependence as expected for degenerate semiconductors. At low temperatures, around 60 K, we observed the maximum Seebeck coefficient due to the phonon drag effect. © 2020 Author(s). All article content, except where otherwise noted, is licensed under a Creative Commons Attribution (CC BY) license (http://creativecommons.org/licenses/by/4.0/).

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, Oliver

The 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.

2021, Wunderlich, Ralf, Staacke, Robert, Knolle, Wolfgang, Abel, Bernd, Meijer, Jan

Here, 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.