@unpublished{HuberPresWittmannetal.2019, author = {Huber, Bernhard and Pres, Sebastian and Wittmann, Emanuel and Dietrich, Lysanne and L{\"u}ttig, Julian and Fersch, Daniel and Krauss, Enno and Friedrich, Daniel and Kern, Johannes and Lisinetskii, Victor and Hensen, Matthias and Hecht, Bert and Bratschitsch, Rudolf and Riedle, Eberhard and Brixner, Tobias}, title = {Space- and time-resolved UV-to-NIR surface spectroscopy and 2D nanoscopy at 1 MHz repetition rate}, issn = {0034-6748}, doi = {10.1063/1.5115322}, url = {http://nbn-resolving.de/urn:nbn:de:bvb:20-opus-191906}, year = {2019}, abstract = {We describe a setup for time-resolved photoemission electron microscopy (TRPEEM) with aberration correction enabling 3 nm spatial resolution and sub-20 fs temporal resolution. The latter is realized by our development of a widely tunable (215-970 nm) noncollinear optical parametric amplifier (NOPA) at 1 MHz repetition rate. We discuss several exemplary applications. Efficient photoemission from plasmonic Au nanoresonators is investigated with phase-coherent pulse pairs from an actively stabilized interferometer. More complex excitation fields are created with a liquid-crystal-based pulse shaper enabling amplitude and phase shaping of NOPA pulses with spectral components from 600 to 800 nm. With this system we demonstrate spectroscopy within a single plasmonic nanoslit resonator by spectral amplitude shaping and investigate the local field dynamics with coherent two-dimensional (2D) spectroscopy at the nanometer length scale ("2D nanoscopy"). We show that the local response varies across a distance as small as 33 nm in our sample. Further, we report two-color pump-probe experiments using two independent NOPA beamlines. We extract local variations of the excited-state dynamics of a monolayered 2D material (WSe2) that we correlate with low-energy electron microscopy (LEEM) and reflectivity (LEER) measurements. Finally, we demonstrate the in-situ sample preparation capabilities for organic thin films and their characterization via spatially resolved electron diffraction and dark-field LEEM.}, language = {en} } @unpublished{StennettBissingerGriesbecketal.2019, author = {Stennett, Tom E. and Bissinger, Philipp and Griesbeck, Stefanie and Ullrich, Stefan and Krummenacher, Ivo and Auth, Michael and Sperlich, Andreas and Stolte, Matthias and Radacki, Krzysztof and Yao, Chang-Jiang and W{\"u}rthner, Frank and Steffen, Andreas and Marder, Todd B. and Braunschweig, Holger}, title = {Near-Infrared Quadrupolar Chromophores Combining Three-Coordinate Boron-Based Superdonor and Superacceptor Units}, series = {Angewandte Chemie, International Edition}, journal = {Angewandte Chemie, International Edition}, doi = {10.1002/anie.201900889}, url = {http://nbn-resolving.de/urn:nbn:de:bvb:20-opus-180391}, year = {2019}, abstract = {In this work, two new quadrupolar A-π-D-π-A chromophores have been prepared featuring a strongly electron- donating diborene core and strongly electron-accepting dimesitylboryl F(BMes2) and bis(2,4,6-tris(trifluoromethyl)phenyl)boryl (BMes2) end groups. Analysis of the compounds by NMR spectroscopy, X-ray crystallography, cyclic voltammetry and UV-vis-NIR absorption and emission spectroscopy indicated that the compounds possess extended conjugated π-systems spanning their B4C8 cores. The combination of exceptionally potent π-donor (diborene) and π- acceptor (diarylboryl) groups, both based on trigonal boron, leads to very small HOMO-LUMO gaps, resulting in strong absorption in the near-IR region with maxima in THF at 840 and 1092 nm, respectively, and very high extinction coefficients of ca. 120,000 M-1cm-1. Both molecules also display weak near-IR fluorescence with small Stokes shifts.}, language = {en} } @unpublished{Reiss2012, author = {Reiss, Harald}, title = {Time scales and existence of time holes in non-transparent media}, url = {http://nbn-resolving.de/urn:nbn:de:bvb:20-opus-73554}, year = {2012}, abstract = {The analysis presented in this paper applies to experimental situations where observers or objects to be studied, all at stationary positions, are located in environments the optical thickness of which is strongly different. Non-transparent media comprise thin metallic films, packed or fluidised beds, superconductors, the Earth's crust, and even dark clouds and other cosmological objects. The analysis applies mapping functions that correlate physical events, e, in non-transparent media, with their images, f(e), tentatively located on standard physical time scale. The analysis demonstrates, however, that physical time, in its rigorous sense, does not exist under non-transparency conditions. A proof of this conclusion is attempted in three steps: i) the theorem "there is no time without space and events" is accepted, (ii) images f[e(s,t)] do not constitute a dense, uncountably infinite set, and (iii) sets of images that are not uncountably infinite do not create physical time but only time-like sequences. As a consequence, mapping f[e(s,t)] in non-transparent space does not create physical analogues to the mathematical structure of the ordered, dense half-set R+ of real numbers, and reverse mapping, f-1f[e(s,t)], the mathematical inverse problem, would not allow unique identification and reconstruction of original events from their images. In these cases, causality as well as invariance of physical processes under time reversal, might be violated. An interesting problem is whether temporal cloaking (a time hole) in a transparent medium, as very recently reported in the literature, can be explained by the present analysis. Existence of time holes could perhaps be possible, not in transparent but in non-transparent media, as follows from the sequence of images, f[e(s,t)], that is not uncountably infinite, in contrast to R+. Impacts are expected for understanding physical diffusion-like, radiative transfer processes and stability models to protect superconductors against quenchs. There might be impacts also in relativity, quantum mechanics, nuclear decay, or in systems close to their phase transitions. The analysis is not restricted to objects of laboratory dimensions.}, subject = {Zeitrichtung}, language = {en} } @unpublished{Reiss2012, author = {Reiss, Harald}, title = {Physical time and existence of time holes in non-transparent media}, url = {http://nbn-resolving.de/urn:nbn:de:bvb:20-opus-67268}, year = {2012}, abstract = {The analysis presented in this paper applies to experimental situations where observers or objects to be studied (both stationary, with respect to each other) are located in environments the optical thickness of which is strongly different. By their large optical thickness, non-transparent media are clearly distinguished from their transparent counterparts. Non-transparent media comprise thin metallic films, packed or fluidised beds, the Earth's crust, and even dark clouds and other cosmological objects. As a representative example, a non-transparent slab is subjected to transient disturbances, and a rigorous analysis is presented whether physical time reasonably could be constructed under such condition. The analysis incorporates mapping functions that correlate physical events, e, in non-transparent media, with their images, f(e), tentatively located on a standard physical time scale. The analysis demonstrates, however, that physical time, in its rigorous sense, does not exist under non-transparency conditions. A proof of this conclusion is attempted in three steps: i) the theorem "there is no time without space and events" is accepted, (ii) images f[e(s,t)] do not constitute a dense, uncountably infinite set, and (iii) sets of images that are not uncountably infinite do not create physical time but only time-like sequences. As a consequence, mapping f[e(s,t)] in non-transparent space does not create physical analogues to the mathematical structure of the ordered, dense half-set R+ of real numbers, and reverse mapping, f-1f[e(s,t)] would not allow unique identification and reconstruction of original events from their images. In these cases, causality and determinism, as well as invariance of physical processes under time reversal, might be violated. Existence of time holes could be possible, as follows from the sequence of images, f[e(s,t)], that is not uncountably infinite, in contrast to R+. Practical impacts are expected for understanding physical diffusion-like, radiative transfer processes, stability models to protect superconductors against quenchs or for description of their transient local pair density and critical currents. Impacts would be expected also in mathematical formulations (differential equations) of classical physics, in relativity and perhaps in quantum mechanics, all as far as transient processes in non-transparent space would be concerned. An interesting problem is whether temporal cloaking (a time hole) in a transparent medium, as very recently reported in the literature, can be explained by the present analysis. The analysis is not restricted to objects of laboratory dimensions: Because of obviously existing radiation transfer analogues, it is tempting to discuss consequences also for much larger structures in particular if an origin of time is postulated.}, subject = {Strahlungstransport}, language = {en} }