Browsing by Author "Ueda, Kiyoshi"
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- ItemApplication of Matched-Filter Concepts to Unbiased Selection of Data in Pump-Probe Experiments with Free Electron Lasers(Basel : MDPI, 2017-06-16) Callegari, Carlo; Takanashi, Tsukasa; Fukuzawa, Hironobu; Motomura, Koji; Iablonskyi, Denys; Kumagai, Yoshiaki; Mondal, Subhendu; Tachibana, Tetsuya; Nagaya, Kiyonobu; Nishiyama, Toshiyuki; Matsunami, Kenji; Johnsson, Per; Piseri, Paolo; Sansone, Giuseppe; Dubrouil, Antoine; Reduzzi, Maurizio; Carpeggiani, Paolo; Vozzi, Caterina; Devetta, Michele; Faccialà, Davide; Calegari, Francesca; Castrovilli, Mattea; Coreno, Marcello; Alagia, Michele; Schütte, Bernd; Berrah, Nora; Plekan, Oksana; Finetti, Paola; Ferrari, Eugenio; Prince, Kevin; Ueda, KiyoshiPump-probe experiments are commonly used at Free Electron Lasers (FEL) to elucidate the femtosecond dynamics of atoms, molecules, clusters, liquids and solids. Maximizing the signal-to-noise ratio of the measurements is often a primary need of the experiment, and the aggregation of repeated, rapid, scans of the pump-probe delay is preferable to a single long-lasting scan. The limited availability of beamtime makes it impractical to repeat measurements indiscriminately, and the large, rapid flow of single-shot data that need to be processed and aggregated into a dataset, makes it difficult to assess the quality of a measurement in real time. In post-analysis it is then necessary to devise unbiased criteria to select or reject datasets, and to assign the weight with which they enter the analysis. One such case was the measurement of the lifetime of Intermolecular Coulombic Decay in the weakly-bound neon dimer. We report on the method we used to accomplish this goal for the pump-probe delay scans that constitute the core of the measurement; namely we report on the use of simple auto- and cross-correlation techniques based on the general concept of “matched filter”. We are able to unambiguously assess the signal-to-noise ratio (SNR) of each scan, which then becomes the weight with which a scan enters the average of multiple scans. We also observe a clear gap in the values of SNR, and we discard all the scans below a SNR of 0.45. We are able to generate an average delay scan profile, suitable for further analysis: in our previous work we used it for comparison with theory. Here we argue that the method is sufficiently simple and devoid of human action to be applicable not only in post-analysis, but also for the real-time assessment of the quality of a dataset.
- ItemDeep neural networks for classifying complex features in diffraction images(Woodbury, NY : Inst., 2019) Zimmermann, Julian; Langbehn, Bruno; Cucini, Riccardo; Di Fraia, Michele; Finetti, Paola; LaForge, Aaron C.; Nishiyama, Toshiyuki; Ovcharenko, Yevheniy; Piseri, Paolo; Plekan, Oksana; Prince, Kevin C.; Stienkemeier, Frank; Ueda, Kiyoshi; Callegari, Carlo; Möller, Thomas; Rupp, DanielaIntense short-wavelength pulses from free-electron lasers and high-harmonic-generation sources enable diffractive imaging of individual nanosized objects with a single x-ray laser shot. The enormous data sets with up to several million diffraction patterns present a severe problem for data analysis because of the high dimensionality of imaging data. Feature recognition and selection is a crucial step to reduce the dimensionality. Usually, custom-made algorithms are developed at a considerable effort to approximate the particular features connected to an individual specimen, but because they face different experimental conditions, these approaches do not generalize well. On the other hand, deep neural networks are the principal instrument for today's revolution in automated image recognition, a development that has not been adapted to its full potential for data analysis in science. We recently published [Langbehn et al., Phys. Rev. Lett. 121, 255301 (2018)] the application of a deep neural network as a feature extractor for wide-angle diffraction images of helium nanodroplets. Here we present the setup, our modifications, and the training process of the deep neural network for diffraction image classification and its systematic bench marking. We find that deep neural networks significantly outperform previous attempts for sorting and classifying complex diffraction patterns and are a significant improvement for the much-needed assistance during postprocessing of large amounts of experimental coherent diffraction imaging data.
- ItemEvidence for Efficient Pathway to Produce Slow Electrons by Ground-state Dication in Clusters(Bristol : IOP Publ., 2017) You, Daehyun; Fukuzawa, Hironobu; Sakakibara, Yuta; Takanashi, Tsukasa; Ito, Yuta; Maliyar, Gianluigi G.; Motomura, Koji; Nagaya, Kiyonobu; Nishiyama, Toshiyuki; Asa, Kazuki; Sato, Yuhiro; Saito, Norio; Oura, Masaki; Schöffler, Markus; Kastirke, Gregor; Hergenhahn, Uwe; Stumpf, Vasili; Gohkberg, Kirill; Kuleff, Alexander I.; Cederbaum, Lorenz S.; Ueda, KiyoshiWe present an experimental evidence for a so-far unobserved, but potentially very important step relaxation cascades following inner-shell ionization of a composite system: Multiply charged ionic states created after Auger decay may be neutralized by electron transfer from a neighboring species, producing at the same time a low-energy free electron. This electron transfer-mediated decay (ETMD) called process is effective even after Auger decay into the dicationic ground state. Here, we report the ETMD of Ne2+ produced after Ne 1s photoionization in Ne-Kr mixed clusters.
- ItemRoadmap of ultrafast x-ray atomic and molecular physics(Bristol : IOP Publ., 2018-01-09) Young, Linda; Ueda, Kiyoshi; Gühr, Markus; Bucksbaum, Philip H.; Simon, Marc; Mukamel, Shaul; Rohringer, Nina; Prince, Kevin C.; Masciovecchio, Claudio; Meyer, Michael; Rudenko, Artem; Rolles, Daniel; Bostedt, Christoph; Fuchs, Matthias; Reis, David A.; Santra, Robin; Kapteyn, Henry; Murnane, Margaret; Ibrahim, Heide; Légaré, François; Vrakking, Marc; Isinger, Marcus; Kroon, David; Gisselbrecht, Mathieu; L’Huillier, Anne; Wörner, Hans Jakob; Leone, Stephen R.X-ray free-electron lasers (XFELs) and table-top sources of x-rays based upon high harmonic generation (HHG) have revolutionized the field of ultrafast x-ray atomic and molecular physics, largely due to an explosive growth in capabilities in the past decade. XFELs now provide unprecedented intensity (1020 W cm−2) of x-rays at wavelengths down to ∼1 Ångstrom, and HHG provides unprecedented time resolution (∼50 attoseconds) and a correspondingly large coherent bandwidth at longer wavelengths. For context, timescales can be referenced to the Bohr orbital period in hydrogen atom of 150 attoseconds and the hydrogen-molecule vibrational period of 8 femtoseconds; wavelength scales can be referenced to the chemically significant carbon K-edge at a photon energy of ∼280 eV (44 Ångstroms) and the bond length in methane of ∼1 Ångstrom. With these modern x-ray sources one now has the ability to focus on individual atoms, even when embedded in a complex molecule, and view electronic and nuclear motion on their intrinsic scales (attoseconds and Ångstroms). These sources have enabled coherent diffractive imaging, where one can image non-crystalline objects in three dimensions on ultrafast timescales, potentially with atomic resolution. The unprecedented intensity available with XFELs has opened new fields of multiphoton and nonlinear x-ray physics where behavior of matter under extreme conditions can be explored. The unprecedented time resolution and pulse synchronization provided by HHG sources has kindled fundamental investigations of time delays in photoionization, charge migration in molecules, and dynamics near conical intersections that are foundational to AMO physics and chemistry. This roadmap coincides with the year when three new XFEL facilities, operating at Ångstrom wavelengths, opened for users (European XFEL, Swiss-FEL and PAL-FEL in Korea) almost doubling the present worldwide number of XFELs, and documents the remarkable progress in HHG capabilities since its discovery roughly 30 years ago, showcasing experiments in AMO physics and other applications. Here we capture the perspectives of 17 leading groups and organize the contributions into four categories: ultrafast molecular dynamics, multidimensional x-ray spectroscopies; high-intensity x-ray phenomena; attosecond x-ray science.
- ItemRoadmap on photonic, electronic and atomic collision physics: I. Light-matter interaction(Bristol : IOP Publ., 2019) Ueda, Kiyoshi; Sokell, Emma; Schippers, Stefan; Aumayr, Friedrich; Sadeghpour, Hossein; Burgdörfer, Joachim; Lemell, Christoph; Tong, Xiao-Min; Pfeifer, Thomas; Calegari, Francesca; Palacios, Alicia; Martin, Fernando; Corkum, Paul; Sansone, Giuseppe; Gryzlova, Elena V.; Grum-Grzhimailo, Alexei N.; Piancastelli, Maria Novella; Weber, Peter M.; Steinle, Tobias; Amini, Kasra; Biegert, Jens; Berrah, Nora; Kukk, Edwin; Santra, Robin; Müller, Alfred; Dowek, Danielle; Lucchese, Robert R.; McCurdy, C. William; Bolognesi, Paola; Avaldi, Lorenzo; Jahnke, Till; Schöffler, Markus S.; Dörner, Reinhard; Mairesse, Yann; Nahon, Laurent; Smirnova, Olga; Schlathölter, Thomas; Campbell, Eleanor E.B.; Rost, Jan-Michael; Meyer, Michael; Tanaka, Kazuo A.We publish three Roadmaps on photonic, electronic and atomic collision physics in order to celebrate the 60th anniversary of the ICPEAC conference. In Roadmap I, we focus on the light-matter interaction. In this area, studies of ultrafast electronic and molecular dynamics have been rapidly growing, with the advent of new light sources such as attosecond lasers and x-ray free electron lasers. In parallel, experiments with established synchrotron radiation sources and femtosecond lasers using cutting-edge detection schemes are revealing new scientific insights that have never been exploited. Relevant theories are also being rapidly developed. Target samples for photon-impact experiments are expanding from atoms and small molecules to complex systems such as biomolecules, fullerene, clusters and solids. This Roadmap aims to look back along the road, explaining the development of these fields, and look forward, collecting contributions from twenty leading groups from the field. © 2019 IOP Publishing Ltd.
- ItemThree-Dimensional Shapes of Spinning Helium Nanodroplets(College Park, Md. : APS, 2018) Langbehn, Bruno; Sander, Katharina; Ovcharenko, Yevheniy; Peltz, Christian; Clark, Andrew; Coreno, Marcello; Cucini, Riccardo; Drabbels, Marcel; Finetti, Paola; Di Fraia, Michele; Giannessi, Luca; Grazioli, Cesare; Iablonskyi, Denys; LaForge, Aaron C.; Nishiyama, Toshiyuki; Oliver Álvarez de Lara, Verónica; Piseri, Paolo; Plekan, Oksana; Ueda, Kiyoshi; Zimmermann, Julian; Prince, Kevin C.; Stienkemeier, Frank; Callegari, Carlo; Fennel, Thomas; Rupp, Daniela; Möller, ThomasA significant fraction of superfluid helium nanodroplets produced in a free-jet expansion has been observed to gain high angular momentum resulting in large centrifugal deformation. We measured single-shot diffraction patterns of individual rotating helium nanodroplets up to large scattering angles using intense extreme ultraviolet light pulses from the FERMI free-electron laser. Distinct asymmetric features in the wide-angle diffraction patterns enable the unique and systematic identification of the three-dimensional droplet shapes. The analysis of a large data set allows us to follow the evolution from axisymmetric oblate to triaxial prolate and two-lobed droplets. We find that the shapes of spinning superfluid helium droplets exhibit the same stages as classical rotating droplets while the previously reported metastable, oblate shapes of quantum droplets are not observed. Our three-dimensional analysis represents a valuable landmark for clarifying the interrelation between morphology and superfluidity on the nanometer scale.