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Airborne high spectral resolution lidar observation of pollution aerosol during EUCAARI-LONGREX

2013, Groß, S., Esselborn, M., Abicht, F., Wirth, M., Fix, A., Minikin, A.

Airborne high spectral resolution lidar observations over Europe during the EUCAARI-LONGREX field experiment in May 2008 are analysed with respect to the optical properties of continental pollution aerosol. Continental pollution aerosol is characterized by its depolarisation and lidar ratio. Over all, the measurements of the lidar ratio and the particle linear depolarization ratio of pollution aerosols provide a narrow range of values. Therefore, this data set allows for a distinct characterization of the aerosol type "pollution aerosol" and thus is valuable both to distinguish continental pollution aerosol from other aerosol types and to determine mixtures with other types of aerosols.

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Dynamical studies on the generation of periodic surface structures by femtosecond laser pulses

2013, Rosenfeld, A., Höhm, S., Bonse, J., Krüger, J.

The dynamics of the formation of laser-induced periodic surface structures (LIPSS) on fused silica upon irradiation with linearly polarized fs-laser pulses (50 fs pulse duration, 800 nm center wavelength) is studied experimentally using a double pulse experiment with cross polarized pulse sequences and a trans illumination femtosecond time-resolved (0.1 ps - 1 ns) pump-probe diffraction approach. The results in both experiments confirm the importance of the ultrafast energy deposition and the laser-induced free-electron plasma in the conduction band of the solids for the formation of LIPSS.

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Femtosecond stimulated Raman spectroscopy of the cyclobutane thymine dimer repair mechanism: A computational study

2014, Ando, H., Fingerhut, B.P., Dorfman, K.E., Biggs, J.D., Mukamel, S.

Cyclobutane thymine dimer, one of the major lesions in DNA formed by exposure to UV sunlight, is repaired in a photoreactivation process, which is essential to maintain life. The molecular mechanism of the central step, i.e., intradimer C-C bond splitting, still remains an open question. In a simulation study, we demonstrate how the time evolution of characteristic marker bands (C=O and C=C/C-C stretch vibrations) of cyclobutane thymine dimer and thymine dinucleotide radical anion, thymidylyl(3′→5′)-thymidine, can be directly probed with femtosecond stimulated Raman spectroscopy (FSRS). We construct a DFT(M05-2X) potential energy surface with two minor barriers for the intradimer C5-C′5 splitting and a main barrier for the C6-C′6 splitting, and identify the appearance of two C5=C6 stretch vibrations due to the C6-C′6 splitting as a spectroscopic signature of the underlying bond splitting mechanism. The sequential mechanism shows only absorptive features in the simulated FSRS signals, whereas the fast concerted mechanism shows characteristic dispersive line shapes. (Figure Presented).

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Photoelectron holography in strong optical and dc electric fields

2014, Stodolna, A., Huismans, Y., Rouzée, A., Lépine, F., Vrakking, M.J.J.

The application of velocity map imaging for the detection of photoelectrons resulting from atomic or molecular ionization allows the observation of interferometric, and in some cases holographic structures that contain detailed information on the target from which the photoelecrons are extracted. In this contribution we present three recent examples of the use of photoelectron velocity map imaging in experiments where atoms are exposed to strong optical and dc electric fields. We discuss (i) observations of the nodal structure of Stark states of hydrogen measured in a dc electric field, (ii) mid-infrared strong-field ionization of metastable Xe atoms and (iii) the reconstruction of helium electronic wavepackets in an attosecond pump-probe experiment. In each case, the interference between direct and indirect electron pathways, reminiscent of the reference and signal waves in holography, is seen to play an important role.

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Graphene Q-switched Yb:KYW planar waveguide laser

2015, Kim, Jun Wan, Young Choi, Sun, Aravazhi, Shanmugam, Pollnau, Markus, Griebner, Uwe, Petrov, Valentin, Bae, Sukang, Jun Ahn, Kwang, Yeom, Dong-Il, Rotermund, Fabian

A diode-pumped Yb:KYW planar waveguide laser, single-mode Q-switched by evanescent-field interaction with graphene, is demonstrated for the first time. Few-layer graphene grown by chemical vapor deposition is transferred onto the top of a guiding layer, which initiates stable Q-switched operation in a 2.4-cm-long waveguide laser operating near 1027 nm. Average output powers up to 34 mW and pulse durations as short as 349 ns are achieved. The measured output beam profile, clearly exhibiting a single mode, agrees well with the theoretically calculated mode intensity distribution inside the waveguide. As the pump power is increased, the repetition rate and pulse energy increase from 191 to 607 kHz and from 7.4 to 58.6 nJ, respectively, whereas the pulse duration decreases from 2.09 μs to 349 ns.

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Scanning single quantum emitter fluorescence lifetime imaging: Quantitative analysis of the local density of photonic states

2014, Schell, A.W., Engel, P., Werra, J.F.M., Wolff, C., Busch, K., Benson, O.

Their intrinsic properties render single quantum systems as ideal tools for quantum enhanced sensing and microscopy. As an additional benefit, their size is typically on an atomic scale that enables sensing with very high spatial resolution. Here, we report on utilizing a single nitrogen vacancy center in nanodiamond for performing three-dimensional scanning-probe fluorescence lifetime imaging microscopy. By measuring changes of the single emitter's lifetime, information on the local density of optical states is acquired at the nanoscale. Three-dimensional ab initio discontinuous Galerkin time-domain simulations are used in order to verify the results and to obtain additional insights. This combination of experiment and simulations to gather quantitative information on the local density of optical states is of direct relevance for the understanding of fundamental quantum optical processes as well as for the engineering of novel photonic and plasmonic devices.

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Nonlinear optical mechanism of forming periodical nanostructures in large bandgap dielectrics

2013, Grunwald, R., Das, S.K., Debroy, A., McGlynn, E., Messaoudi, H.

Nonlinear excitation mechanisms of plasmons and their influence on femtosecond-laser induced sub-wavelength ripple generation on dielectric and semiconducting transparent materials are discussed. The agreement of theoretical and experimental data indicates the relevance of the model.

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Photoluminescence lineshape of ZnO

2014, Ullrich, B., Singh, A.K., Bhowmick, M., Barik, P., Ariza-Flores, D., Xi, H., Tomm, J.W.

The merger of the absorption coefficient dispersion, retrieved from transmission by the modified Urbach rule introduced by Ullrich and Bouchenaki [Jpn. J. Appl. Phys. 30, L1285, 1991], with the extended Roosbroeck-Shockley relation reveals that the optical absorption in ZnO distinctively determines the photoluminescence lineshape. Additionally, the ab initio principles employed enable the accurate determination of the carrier lifetime without further specific probing techniques.

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Excited-state relaxation of hydrated thymine and thymidine measured by liquid-jet photoelectron spectroscopy: experiment and simulation

2015, Buchner, Franziska, Nakayama, Akira, Yamazaki, Shohei, Ritze, Hans-Hermann, Lübcke, Andrea

Time-resolved photoelectron spectroscopy is performed on thymine and thymidine in aqueous solution to study the excited-state relaxation dynamics of these molecules. We find two contributions with sub-ps lifetimes in line with recent excited-state QM/MM molecular dynamics simulations (J. Chem. Phys.2013, 139, 214304). The temporal evolution of ionization energies for the excited ππ* state along the QM/MM molecular dynamics trajectories were calculated and are compatible with experimental results, where the two contributions correspond to the relaxation paths in the ππ* state involving different conical intersections with the ground state. Theoretical calculations also show that ionization from the nπ* state is possible at the given photon energies, but we have not found any experimental indication for signal from the nπ* state. In contrast to currently accepted relaxation mechanisms, we suggest that the nπ* state is not involved in the relaxation process of thymine in aqueous solution.

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Preparation of clay mineral samples for high resolution x-ray imaging

2013, Abbati, G., Seim, C., Legall, H., Stiel, H., Thomas, N., Wilhein, T.

In the development of optimum ceramic materials for plastic forming, it is of fundamental importance to gain insight into the compositions of the clay minerals. Whereas spectroscopic methods are adequate for determining the elemental composition of a given sample, a knowledge of the spatial composition, together with the shape and size of the particles leads to further, valuable insight. This requires an imaging technique such as high resolution X-ray microscopy. In addition, fluorescence spectroscopy provides a viable element mapping technique. Since the fine particle fraction of the materials has a major effect on physical properties like plasticity, the analysis is focused mainly on the smallest particles. To separate these from the bigger agglomerates, the raw material has to pass through several procedures like centrifugation and filtering. After that, one has to deposit a layer of appropriate thickness on to a suitable substrate. These preparative techniques are described here, starting from the clay mineral raw materials and proceeding through to samples that are ready to analyze. First results using high resolution x-ray imaging are shown.