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- ItemExcited state distribution and spin-effects in strong-field excitation of neutral Helium(Bristol : IOP Publ., 2015) Zimmermann, Henri; Eilzer, Sebastian; Eichmann, UlliWe investigated the principal quantum number n distribution of excited states resulting from the interaction of Helium with strong, short laser pulses. We find excellent agreement with predictions of the semiclassical frustrated tunneling ionization (FTI) model [1] as well as fully quantum mechanical calculations. Furthermore, the excitation process directly populates triplet excited states due to the breakdown of the Russel-Saunders coupling scheme for high orbital angular momentum l states of Helium, which are predominantly populated in the strong laser field.
- 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).
- ItemValley control by linearly polarized laser pulses: example of WSe2(Washington, DC : OSA, 2022) Sharma, S.; Elliott, P.; Shallcross, S.Electrons at the band edges of materials are endowed with a valley index, a quantum number locating the band edge within the Brillouin zone. An important question is then how this index may be controlled by laser pulses, with current understanding that it couples exclusively via circularly polarized light. Employing both tight-binding and state-of-the-art time dependent density function theory, we show that on femtosecond time scales valley coupling is a much more general effect. We find that two time separated linearly polarized pulses allow almost complete control over valley excitation, with the pulse time difference and polarization vectors emerging as key parameters for valley control. Our findings highlight the possibility of controlling coherent electronic excitation by successive femtosecond laser pulses, and offer a route towards valleytronics in two-dimensional materials.
- ItemQuantitative hyperspectral coherent diffractive imaging spectroscopy of a solid-state phase transition in vanadium dioxide(Washington, DC [u.a.] : Assoc., 2021) Johnson, Allan S.; Conesa, Jordi Valls; Vidas, Luciana; Perez-Salinas, Daniel; Günther, Christian M.; Pfau, Bastian; Hallman, Kent A.; Haglund, Richard F.; Eisebitt, Stefan; Wall, SimonSolid-state systems can host a variety of thermodynamic phases that can be controlled with magnetic fields, strain, or laser excitation. Many phases that are believed to exhibit exotic properties only exist on the nanoscale, coexisting with other phases that make them challenging to study, as measurements require both nanometer spatial resolution and spectroscopic information, which are not easily accessible with traditional x-ray spectromicroscopy techniques. Here, we use coherent diffractive imaging spectroscopy (CDIS) to acquire quantitative hyperspectral images of the prototypical quantum material vanadium oxide across the vanadium L2,3 and oxygen K x-ray absorption edges with nanometer-scale resolution. We extract the full complex refractive indices of the monoclinic insulating and rutile conducting phases of VO2 from a single sample and find no evidence for correlation-driven phase transitions. CDIS will enable quantitative full-field x-ray spectromicroscopy for studying phase separation in time-resolved experiments and other extreme sample environments where other methods cannot operate.
- ItemSpot profile analysis and lifetime mapping in ultrafast electron diffraction: Lattice excitation of self-organized Ge nanostructures on Si(001)(Melville, NY : AIP Publishing LLC, 2015) Frigge, T.; Hafke, B.; Tinnemann, V.; Witte, T.; Horn-von Hoegen, M.Ultrafast high energy electron diffraction in reflection geometry is employed to study the structural dynamics of self-organized Germanium hut-, dome-, and relaxed clusters on Si(001) upon femtosecond laser excitation. Utilizing the difference in size and strain state the response of hut- and dome clusters can be distinguished by a transient spot profile analysis. Surface diffraction from {105}-type facets provide exclusive information on hut clusters. A pixel-by-pixel analysis of the dynamics of the entire diffraction pattern gives time constants of 40, 160, and 390 ps, which are assigned to the cooling time constants for hut-, dome-, and relaxed clusters.
- ItemTransient magnetic gratings on the nanometer scale(Melville, NY : AIP Publishing LLC, 2020) Weder, D.; von Korff Schmising, C.; Günther, C.M.; Schneider, M.; Engel, D.; Hessing, P.; Strüber, C.; Weigand, M.; Vodungbo, B.; Jal, E.; Liu, X.; Merhe, A.; Pedersoli, E.; Capotondi, F.; Lüning, J.; Pfau, B.; Eisebitt, S.Laser-driven non-local electron dynamics in ultrathin magnetic samples on a sub-10 nm length scale is a key process in ultrafast magnetism. However, the experimental access has been challenging due to the nanoscopic and femtosecond nature of such transport processes. Here, we present a scattering-based experiment relying on a laser-induced electro- and magneto-optical grating in a Co/Pd ferromagnetic multilayer as a new technique to investigate non-local magnetization dynamics on nanometer length and femtosecond timescales. We induce a spatially modulated excitation pattern using tailored Al near-field masks with varying periodicities on a nanometer length scale and measure the first four diffraction orders in an x-ray scattering experiment with magnetic circular dichroism contrast at the free-electron laser facility FERMI, Trieste. The design of the periodic excitation mask leads to a strongly enhanced and characteristic transient scattering response allowing for sub-wavelength in-plane sensitivity for magnetic structures. In conjunction with scattering simulations, the experiment allows us to infer that a potential ultrafast lateral expansion of the initially excited regions of the magnetic film mediated by hot-electron transport and spin transport remains confined to below three nanometers.