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- ItemAttosecond time-resolved photoelectron holography([London] : Nature Publishing Group UK, 2018) Porat, G.; Alon, G.; Rozen, S.; Pedatzur, O.; Krüger, M.; Azoury, D.; Natan, A.; Orenstein, G.; Bruner, B.D.; Vrakking, M. J.J.; Dudovich, N.Ultrafast strong-field physics provides insight into quantum phenomena that evolve on an attosecond time scale, the most fundamental of which is quantum tunneling. The tunneling process initiates a range of strong field phenomena such as high harmonic generation (HHG), laser-induced electron diffraction, double ionization and photoelectron holography - all evolving during a fraction of the optical cycle. Here we apply attosecond photoelectron holography as a method to resolve the temporal properties of the tunneling process. Adding a weak second harmonic (SH) field to a strong fundamental laser field enables us to reconstruct the ionization times of photoelectrons that play a role in the formation of a photoelectron hologram with attosecond precision. We decouple the contributions of the two arms of the hologram and resolve the subtle differences in their ionization times, separated by only a few tens of attoseconds.
- ItemIn situ single-shot diffractive fluence mapping for X-ray free-electron laser pulses([London] : Nature Publishing Group UK, 2018) Schneider, Michael; Günther, Christian M.; Pfau, Bastian; Capotondi, Flavio; Manfredda, Michele; Zangrando, Marco; Mahne, Nicola; Raimondi, Lorenzo; Pedersoli, Emanuele; Naumenko, Denys; Eisebitt, StefanFree-electron lasers (FELs) in the extreme ultraviolet (XUV) and X-ray regime opened up the possibility for experiments at high power densities, in particular allowing for fluence-dependent absorption and scattering experiments to reveal non-linear light-matter interactions at ever shorter wavelengths. Findings of such non-linear effects are met with tremendous interest, but prove difficult to understand and model due to the inherent shot-to-shot fluctuations in photon intensity and the often structured, non-Gaussian spatial intensity profile of a focused FEL beam. Presently, the focused beam is characterized and optimized separately from the actual experiment. Here, we present the simultaneous measurement of XUV diffraction signals from solid samples in tandem with the corresponding single-shot spatial fluence distribution on the actual sample. Our in situ characterization scheme enables direct monitoring of the sample illumination, providing a basis to optimize and quantitatively understand FEL experiments.
- ItemGate-controlled quantum dots and superconductivity in planar germanium([London] : Nature Publishing Group UK, 2018) Hendrickx, N.W.; Franke, D.P.; Sammak, A.; Kouwenhoven, M.; Sabbagh, D.; Yeoh, L.; Li, R.; Tagliaferri, M.L.V.; Virgilio, M.; Capellini, G.; Scappucci, G.; Veldhorst, M.Superconductors and semiconductors are crucial platforms in the field of quantum computing. They can be combined to hybrids, bringing together physical properties that enable the discovery of new emergent phenomena and provide novel strategies for quantum control. The involved semiconductor materials, however, suffer from disorder, hyperfine interactions or lack of planar technology. Here we realise an approach that overcomes these issues altogether and integrate gate-defined quantum dots and superconductivity into germanium heterostructures. In our system, heavy holes with mobilities exceeding 500,000 cm2 (Vs)−1 are confined in shallow quantum wells that are directly contacted by annealed aluminium leads. We observe proximity-induced superconductivity in the quantum well and demonstrate electric gate-control of the supercurrent. Germanium therefore has great promise for fast and coherent quantum hardware and, being compatible with standard manufacturing, could become a leading material for quantum information processing.
- ItemAnisotropic photoemission time delays close to a Fano resonance([London] : Nature Publishing Group UK, 2018) Cirelli, Claudio; Marante, Carlos; Heuser, Sebastian; Petersson, C.L.M.; Galán, Álvaro Jiménez; Argenti, Luca; Zhong, Shiyang; Busto, David; Isinger, Marcus; Nandi, Saikat; Maclot, Sylvain; Rading, Linnea; Johnsson, Per; Gisselbrecht, Mathieu; Lucchini, Matteo; Gallmann, Lukas; Dahlström, J. Marcus; Lindroth, Eva; L’Huillier, Anne; Martín, Fernando; Keller, UrsulaElectron correlation and multielectron effects are fundamental interactions that govern many physical and chemical processes in atomic, molecular and solid state systems. The process of autoionization, induced by resonant excitation of electrons into discrete states present in the spectral continuum of atomic and molecular targets, is mediated by electron correlation. Here we investigate the attosecond photoemission dynamics in argon in the 20-40 eV spectral range, in the vicinity of the 3s -1 np autoionizing resonances. We present measurements of the differential photoionization cross section and extract energy and angle-dependent atomic time delays with an attosecond interferometric method. With the support of a theoretical model, we are able to attribute a large part of the measured time delay anisotropy to the presence of autoionizing resonances, which not only distort the phase of the emitted photoelectron wave packet but also introduce an angular dependence.
- ItemPublisher Correction: Coherent diffractive imaging of single helium nanodroplets with a high harmonic generation source (Nature communications (2017) 8 1 (493))([London] : Nature Publishing Group UK, 2018) Rupp, Daniela; Monserud, Nils; Langbehn, Bruno; Sauppe, Mario; Zimmermann, Julian; Ovcharenko, Yevheniy; Möller, Thomas; Frassetto, Fabio; Poletto, Luca; Trabattoni, Andrea; Calegari, Francesca; Nisoli, Mauro; Sander, Katharina; Peltz, Christian; Vrakking, Marc J.; Fennel, Thomas; Rouzée, ArnaudIn the original version of this Article, the affiliation for Luca Poletto was incorrectly given as 'European XFEL GmbH, Holzkoppel 4, 22869 Schenefeld, Hamburg, Germany', instead of the correct 'CNR, Istituto di Fotonica e Nanotecnologie Padova, Via Trasea 7, 35131 Padova, Italy'. This has now been corrected in both the PDF and HTML versions of the Article.
- ItemAttosecond recorder of the polarization state of light([London] : Nature Publishing Group UK, 2018) Jiménez-Galán, Álvaro; Dixit, Gopal; Patchkovskii, Serguei; Smirnova, Olga; Morales, Felipe; Ivanov, MishaHigh harmonic generation in multi-color laser fields opens the opportunity of generating isolated attosecond pulses with high ellipticity. Such pulses hold the potential for time-resolving chiral electronic, magnetization, and spin dynamics at their natural timescale. However, this potential cannot be realized without characterizing the exact polarization state of light on the attosecond timescale. Here we propose and numerically demonstrate a complete solution of this problem. Our solution exploits the extrinsic two-dimensional chirality induced in an atom interacting with the chiral attosecond pulse and a linearly polarized infrared probe. The resulting asymmetry in the photoelectron spectra allows to reconstruct the complete polarization state of the attosecond pulse, including its possible time dependence. The challenging problem of distinguishing circularly polarized, partially polarized, or unpolarized pulses in the extreme ultraviolet range is also resolved. We expect this approach to become the core ingredient for attosecond measurements of chiral-sensitive processes in gas and condensed phase.
- ItemCompetition between proton transfer and intermolecular Coulombic decay in water([London] : Nature Publishing Group UK, 2018) Richter, Clemens; Hollas, Daniel; Saak, Clara-Magdalena; Förstel, Marko; Miteva, Tsveta; Mucke, Melanie; Björneholm, Olle; Sisourat, Nicolas; Slavíček, Petr; Hergenhahn, UweIntermolecular Coulombic decay (ICD) is a ubiquitous relaxation channel of electronically excited states in weakly bound systems, ranging from dimers to liquids. As it is driven by electron correlation, it was assumed that it will dominate over more established energy loss mechanisms, for example fluorescence. Here, we use electron–electron coincidence spectroscopy to determine the efficiency of the ICD process after 2a1 ionization in water clusters. We show that this efficiency is surprisingly low for small water clusters and that it gradually increases to 40–50% for clusters with hundreds of water units. Ab initio molecular dynamics simulations reveal that proton transfer between neighboring water molecules proceeds on the same timescale as ICD and leads to a configuration in which the ICD channel is closed. This conclusion is further supported by experimental results from deuterated water. Combining experiment and theory, we infer an intrinsic ICD lifetime of 12–52 fs for small water clusters.
- ItemPublisher Correction: Nanoplasmonic electron acceleration by attosecond-controlled forward rescattering in silver clusters (Nature communications (2017) 8 1 (1181))([London] : Nature Publishing Group UK, 2018) Passig, Johannes; Zherebtsov, Sergey; Irsig, Robert; Arbeiter, Mathias; Peltz, Christian; Göde, Sebastian; Skruszewicz, Slawomir; Meiwes-Broer, Karl-Heinz; Tiggesbäumker, Josef; Kling, Matthias F.; Fennel, ThomasThe original PDF version of this Article contained an error in Equation 1. The original HTML version of this Article contained errors in Equation 2 and Equation 4. These errors have now been corrected in both the PDF and the HTML versions of the Article. The original PDF version of this Article contained an error in Equation 1. A dot over the first occurrence of the variable ri was missing, and incorrectly read: (Formula Presented). The correct form of Equation 1 is as follows: (Formula Presented). This has now been corrected in the PDF version of the Article. The HTML version was correct from the time of publication. The original HTML version of this Article contained errors in Equation 2 and Equation 4. In Equation 2, a circle over the first occurrence of the variable ri replaced the intended dot, and incorrectly read: (Formula Presented). The correct form of Equation 2 is as follows: (Formula Presented). In Equation 4, circles over the first and fifth occurrences of the variable ri replaced the intended dots, and incorrectly read: (Formula Presented). The correct form of Equation 4 is as follows: (Formula Presented). This has now been corrected in the HTML version of the Article. The PDF version was correct from the time of publication.
- ItemPolymerization driven monomer passage through monolayer chemical vapour deposition graphene([London] : Nature Publishing Group UK, 2018-10-3) Zhang, Tao; Liao, Zhongquan; Sandonas, Leonardo Medrano; Dianat, Arezoo; Liu, Xiaoling; Xiao, Peng; Amin, Ihsan; Gutierrez, Rafael; Chen, Tao; Zschech, Ehrenfried; Cuniberti, Gianaurelio; Jordan, RainerMass transport through graphene is receiving increasing attention due to the potential for molecular sieving. Experimental studies are mostly limited to the translocation of protons, ions, and water molecules, and results for larger molecules through graphene are rare. Here, we perform controlled radical polymerization with surface-anchored self-assembled initiator monolayer in a monomer solution with single-layer graphene separating the initiator from the monomer. We demonstrate that neutral monomers are able to pass through the graphene (via native defects) and increase the graphene defects ratio (Raman ID/IG) from ca. 0.09 to 0.22. The translocations of anionic and cationic monomers through graphene are significantly slower due to chemical interactions of monomers with the graphene defects. Interestingly, if micropatterned initiator-monolayers are used, the translocations of anionic monomers apparently cut the graphene sheet into congruent microscopic structures. The varied interactions between monomers and graphene defects are further investigated by quantum molecular dynamics simulations.