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- ItemIntracycle interference in ionization of Ar by a laser assisted XUV pulse(Bristol : IOP Publ., 2017) Arbó, D.G.; López, S. D.; Kubin, M.; Hummert, J.; Vrakking, M.J.J.; Kornilov, O.Synopsis We present a theoretical and experimental study of the subcycle interference in laser assisted XUV ionization of Ar atoms. Averaging over the focal volume happens to blur the intracycle interference, which thus cannot be measured directly. We show that even at these conditions, the intracycle interference can be obtained through the subtraction of two different angle and energy-resolved distributions at slightly different laser intensities.
- ItemReactive species driven oxidative modifications of peptides—Tracing physical plasma liquid chemistry(Melville, NY : American Inst. of Physics, 2021) Wenske, Sebastian; Lackmann, Jan-Wilm; Busch, Larissa Milena; Bekeschus, Sander; von Woedtke, Thomas; Wende, KristianThe effluence of physical plasma consists of a significant share of reactive species, which may interact with biomolecules and yield chemical modifications comparable to those of physiological processes, e.g., post-translational protein modifications (oxPTMs). Consequentially, the aim of this work is to understand the role of physical plasma-derived reactive species in the introduction of oxPTM-like modifications in proteins. An artificial peptide library consisting of ten peptides was screened against the impact of two plasma sources, the argon-driven MHz-jet kINPen and the helium-driven RF-jet COST-Jet. Changes in the peptide molecular structure were analyzed by liquid chromatography–mass spectrometry. The amino acids cysteine, methionine, tyrosine, and tryptophan were identified as major targets. The introduction of one, two, or three oxygen atoms was the most common modification observed. Distinct modification patterns were observed for nitration (+N + 2O–H), which occurred in kINPen only (peroxynitrite), and chlorination (+Cl–H) that was exclusive for the COST-Jet in the presence of chloride ions (atomic oxygen/hypochlorite). Predominantly for the kINPen, singlet oxygen-related modifications, e.g., cleavage of tryptophan, were observed. Oxidation, carbonylation, and double oxidations were attributed to the impact of hydroxyl radicals and atomic oxygen. Leading to a significant change in the peptide side chain, most of these oxPTM-like modifications affect the secondary structure of amino acid chains, and amino acid polarity/functionality, ultimately modifying the performance and stability of cellular proteins.
- ItemIntracluster Coulombic decay following intense NIR ionization of clusters(Bristol : IOP Publ., 2015) Schütte, Bernd; Arbeiter, Mathias; Fennel, Thomas; Jabbari, Ghazal; Gokhberg, Kirill; Kuleff, Alexander I.; Vrakking, Marc J. J.; Rouzée, ArnaudWe report on the observation of a novel intracluster Coulombic decay process following Rydberg atom formation in clusters ionized by intense near-infrared fields. A new decay channel emerges, in which a Rydberg atom relaxes to the ground state by transferring its excess energy to a weakly bound electron in the environment that is emitted from the cluster. We find evidence for this process in the electron spectra, where a peak close to the corresponding atomic ionization potential is observed. For Ar clusters, a decay time of 87 ps is measured, which is significantly longer than in previous time-resolved studies of interatomic Coulombic decay.
- ItemCorrelated electronic decay following intense near-infrared ionization of clusters(Bristol : IOP Publ., 2015) Schütte, Bernd; Arbeiter, Mathias; Fennel, Thomas; Jabbari, Ghazal; Kuleff, Alexander I.; Vrakking, Marc J. J.; Rouzée, ArnaudWe report on a novel correlated electronic decay process following extensive Rydberg atom formation in clusters ionized by intense near-infrared fields. A peak close to the atomic ionization potential is found in the electron kinetic energy spectrum. This new contribution is attributed to an energy transfer between two electrons, where one electron decays from a Rydberg state to the ground state and transfers its excess energy to a weakly bound cluster electron in the environment that can escape from the cluster. The process is a result of nanoplasma formation and is therefore expected to be important, whenever intense laser pulses interact with nanometer-sized particles.
- ItemInteratomic Coulombic Decay Processes after Multiple Valence Excitations in Ne Clusters(Bristol : IOP Publ., 2015) Iablonskyi, D.; Nagaya, K.; Fukuzawa, H.; Motomura, K.; Kumagai, Y.; Mondal, S.; Tachibana, T.; Takanashi, T.; Nishiyama, T.; Matsunami, K.; Johnsson, P.; Piseri, P.; Sansone, G.; Dubrouil, A.; Reduzzi, M.; Carpeggiani, P.; Vozzi, C.; Devetta, M.; Negro, M.; Faccialà, D.; Calegari, F.; Trabattoni, A.; Castrovilli, M.; Ovcharenko, Y.; Möller, T.; Mudrich, M.; Stienkemeier, F.; Coreno, M.; Alagia, M.; Schütte, B.; Berrah, N.; Callegari, C.; Plekan, O.; Finetti, P.; Spezzani, C.; Ferrari, E.; Allaria, E.; Penco, G.; Serpico, C.; De Ninno, G.; Diviacco, B.; Di Mitri, S.; Giannessi, L.; Prince, K..; Yao, M.; Ueda, K.We present a comprehensive analysis of autoionization processes in Ne clusters (~5000 atoms) after multiple valence excitations by free electron laser radiation. The evolution from 2-body interatomic Coulombic decay (ICD) to 3-body ICD is demonstrated when changing from surface to bulk Frenkel exciton excitation. Super Coster-Kronig type 2-body ICD is observed at Wannier exciton which quenches the main ICD channel.
- 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.
- ItemAtomic processes in bicircular fields(Bristol : IOP Publ., 2016) Odžak, S.; Hasović, E.; Becker, W.; Milošević, D.B.We investigate laser-assisted electron-ion recombination (LAR), high-order harmonic generation (HHG) and above-threshold ionization (ATI) of argon atoms by a bicircular laser field, which consists of two coplanar counter-rotating circularly polarized fields of frequencies rω and sω. The energy of soft x rays generated in the LAR process is analyzed as a function of the incident electron angle and numerical results of direct recombination of electrons with Ar+ ions are presented. We also present the results of HHG by a bicircular field and confirm the selection rules derived earlier for inert-gas atoms in a p ground state. We show that the photoelectron spectra in the ATI process, presented in the momentum plane, as well as the LAR spectra exhibit the same discrete rotational symmetry as the applied field.
- ItemCoherent interaction of atoms with a beam of light confined in a light cage(London : Nature Publishing Group, 2021) Davidson-Marquis, Flavie; Gargiulo, Julian; Gómez-López, Esteban; Jang, Bumjoon; Kroh, Tim; Müller, Chris; Ziegler, Mario; Maier, Stefan A.; Kübler, Harald; Schmidt, Markus A.; Benson, OliverControlling coherent interaction between optical fields and quantum systems in scalable, integrated platforms is essential for quantum technologies. Miniaturised, warm alkali-vapour cells integrated with on-chip photonic devices represent an attractive system, in particular for delay or storage of a single-photon quantum state. Hollow-core fibres or planar waveguides are widely used to confine light over long distances enhancing light-matter interaction in atomic-vapour cells. However, they suffer from inefficient filling times, enhanced dephasing for atoms near the surfaces, and limited light-matter overlap. We report here on the observation of modified electromagnetically induced transparency for a non-diffractive beam of light in an on-chip, laterally-accessible hollow-core light cage. Atomic layer deposition of an alumina nanofilm onto the light-cage structure was utilised to precisely tune the high-transmission spectral region of the light-cage mode to the operation wavelength of the atomic transition, while additionally protecting the polymer against the corrosive alkali vapour. The experiments show strong, coherent light-matter coupling over lengths substantially exceeding the Rayleigh range. Additionally, the stable non-degrading performance and extreme versatility of the light cage provide an excellent basis for a manifold of quantum-storage and quantum-nonlinear applications, highlighting it as a compelling candidate for all-on-chip, integrable, low-cost, vapour-based photon delay.
- ItemInfluence of 4f filling on electronic and magnetic properties of rare earth-Au surface compounds(Cambridge : RSC Publ., 2020) Fernandez, L.; Blanco-Rey, M.; Castrillo-Bodero, R.; Ilyn, M.; Ali, K.; Turco, E.; Corso, M.; Ormaza, M.; Gargiani, P.; Valbuena, M.A.; Mugarza, A.; Moras, P.; Sheverdyaeva, P.M.; Kundu, Asish K.; Jugovac, M.; Laubschat, C.; Ortega, J.E.; Schiller, F.One-atom-thick rare-earth/noble metal (RE-NM) compounds are attractive materials to investigate two-dimensional magnetism, since they are easy to synthesize into a common RE-NM2 structure with high crystal perfection. Here we perform a comparative study of the GdAu2, HoAu2, and YbAu2 monolayer compounds grown on Au(111). We find the same atomic lattice quality and moiré superlattice periodicity in the three cases, but different electronic properties and magnetism. The YbAu2 monolayer reveals the characteristic electronic signatures of a mixed-valence configuration in the Yb atom. In contrast, GdAu2 and HoAu2 show the trivalent character of the rare-earth and ferromagnetic transitions below 22 K. Yet, the GdAu2 monolayer has an in-plane magnetic easy-axis, versus the out-of-plane one in HoAu2. The electronic bands of the two trivalent compounds are very similar, while the divalent YbAu2 monolayer exhibits different band features. In the latter, a strong 4f-5d hybridization is manifested in neatly resolved avoided crossings near the Fermi level. First principles theory points to a residual presence of empty 4f states, explaining the fluctuating valence of Yb in the YbAu2 monolayer. © The Royal Society of Chemistry.
- ItemNon-instantaneous third-order optical response of gases in low-frequency fields(Washington, DC : Soc., 2022) Morales, Felipe; Richter, Maria; Ivanov, Misha; Husakou, AntonIt is commonly assumed that for low-intensity short optical pulses far from resonance, the third-order optical nonlinear response is instantaneous. We solve the three-dimensional time-dependent Schrödinger equation for the hydrogen atom and show that this is not the case: the polarization is not simply proportional to the cube of the electric field even at low intensities. We analyze the fundamental-frequency and third-harmonic nonlinear susceptibilities of hydrogen, investigate their dependence on intensity, and find that the delays in the Kerr response rapidly approach the femtosecond time-scale at higher intensities, while the delays in the third harmonic generation remain much lower. We also propose an experimental scheme to detect and characterize the above effects.