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- ItemIR-MALDI Mass Spectrometry Imaging with Plasma Post-Ionization of Nonpolar Metabolites(Columbus, Ohio : American Chemical Society, 2022) Schneemann, Julian; Schäfer, Karl-Christian; Spengler, Bernhard; Heiles, SvenAmbient mass spectrometry imaging (MSI) methods come with the advantage of visualizing biomolecules from tissues with no or minimal sample preparation and operation under atmospheric-pressure conditions. Similar to all other MSI methodologies, however, ambient MSI modalities suffer from a pronounced bias toward either polar or nonpolar analytes due to the underlying desorption and ionization mechanisms of the ion source. In this study, we present the design, construction, testing, and application of an in-capillary dielectric barrier discharge (DBD) module for post-ionization of neutrals desorbed by an ambient infrared matrix-assisted laser desorption/ionization (IR-MALDI) MSI source. We demonstrate that the DBD device enhances signal intensities of nonpolar compounds by up to 104 compared to IR-MALDI without affecting transmission of IR-MALDI ions. This allows performing MSI experiments of mouse tissue and Danaus plexippus caterpillar tissue sections, visualizing the distribution of sterols, fatty acids, monoglycerides, and diglycerides that are not detected in IR-MALDI MSI experiments. The pronounced signal enhancement due to IR-MALDI-DBD compared to IR-MALDI MSI enables mapping of nonpolar analytes with pixel resolutions down to 20 μm in mouse brain tissue and to discern the spatial distribution of sterol lipids characteristic for histological regions of D. plexippus.
- ItemInteratomic and Intermolecular Coulombic Decay(Washington, DC : ACS Publ., 2020) Jahnke, Till; Hergenhahn, Uwe; Winter, Bernd; Dörner, Reinhard; Frühling, Ulrike; Demekhin, Philipp V.; Gokhberg, Kirill; Cederbaum, Lorenz S.; Ehresmann, Arno; Knie, André; Dreuw, AndreasInteratomic or intermolecular Coulombic decay (ICD) is a nonlocal electronic decay mechanism occurring in weakly bound matter. In an ICD process, energy released by electronic relaxation of an excited atom or molecule leads to ionization of a neighboring one via Coulombic electron interactions. ICD has been predicted theoretically in the mid nineties of the last century, and its existence has been confirmed experimentally approximately ten years later. Since then, a number of fundamental and applied aspects have been studied in this quickly growing field of research. This review provides an introduction to ICD and draws the connection to related energy transfer and ionization processes. The theoretical approaches for the description of ICD as well as the experimental techniques developed and employed for its investigation are described. The existing body of literature on experimental and theoretical studies of ICD processes in different atomic and molecular systems is reviewed. © 2020 American Chemical Society
- 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.
- ItemAbove-threshold ionization in a bicircular field: Quantum orbits unfolding in a plane(Bristol : IOP Publ., 2017) Becker, W.; Milošević, D.B.Above-threshold ionization (ATI) of atoms by a strong bicircular laser field is investigated using the strong-field approximation and the quantum-orbit theory. The bicircular field consists of two coplanar counterrotating circularly polarized fields with a frequency ratio of 2:1. The velocity map of the angle-resolved ATI spectra, both for direct and rescattered electrons, reflects the shape of a parametric plot of the bicircular field and its symmetries. It is shown that the main characteristics of the ATI spectra can be explained using only a few quantum orbits having short travel times. We also analyze a recently discovered [Phys. Rev. A 93, 052402(R) (2016)] bicircular-field-induced spin asymmetry of the ATI electrons and show that the momentum dependence of the spin-asymmetry parameter is stronger for longer wavelengths.
- ItemUnified description of low-order above-threshold ionization on and off axis(Bristol : IOP Publ., 2016) Becker, W.; Milošević, D.B.A recently developed unified description of low-order above-threshold ionization (Becker et al 2014 J. Phys. B: At. Mol. Opt. Phys. 47 204022; 2015 J. Phys. B: At. Mol. Opt. Phys. 48 151001) is revisited and extended. By considering the rescattering electron energies and angles at the classical cutoffs and the contributions of particular quantum-orbit solutions, it is shown that summing both the backward- and the forward-scattering contributions, within the low-frequency approximation, it is possible to reproduce the observed features of the ATI spectra both for low and high energies and both on and off the laser-polarization axis in the momentum plane.
- ItemA multiwavelength study of the Stingray Nebula; properties of the nebula, central star, and dust(Bristol : IOP Publ., 2016) Otsuka, Masaaki; Parthasarathy, Mudumba; Tajitsu, Akito; Hubrig, SwetlanaWe performed a detail chemical abundance analysis and photo-ionization modeling of the Stingray Nebula (Hen3-1357, Parthasarathy et al. 1993[1]) to more characterize this PN. We calculated nine elemental abundances using collisionally excited lines (CELs) and recombination lines (RLs). The RL C/O ratio indicates that this PN is O-rich, which is supported by the detection of the broad amorphous silicate features at 9 and 18 μm By photo-ionization modeling, we investigated properties of the central star and derived the gas and dust masses. The nebular elemental abundances, the core-mass of the central star, and the gas mass are in agreement with the AGB model for the initially 1.5 M⊙ stars with the Z = 0.008.
- ItemElectron dynamics in laser-driven atoms near the continuum threshold(Washington, DC : OSA, 2021) Liu, Mingqing; Xu, Songpo; Hu, Shilin; Becker, Wilhelm; Quan, Wei; Liu, Xiaojun; Chen, JingStrong-field ionization and Rydberg-state excitation (RSE) near the continuum threshold exhibit two phenomena that have attracted a lot of recent attention: the low-energy structure (LES) just above and frustrated tunneling ionization just below the threshold. The former becomes apparent for longer laser wavelengths, while the latter has been especially investigated in the near infrared; both have been treated as separate phenomena so far. Here we present a unified perspective based on electron trajectories, which emphasizes the very important role of the electron-ion Coulomb interaction as expected in this energy region. Namely, those trajectories that generate the LES can also be recaptured into a Rydberg state. The coherent superposition of the contributions of such trajectories with different travel times (each generating one of the various LES peaks) causes an oscillation in the intensity dependence of the RSE yield, which is especially noticeable for longer wavelengths. The theory is illustrated by RSE experiments at 1800 nm, which agree very well with the theory with respect to position and period of the oscillation. The wavelength scaling of the RSE oscillation is also discussed. Our work establishes a solid relationship between processes below and above the threshold and sheds new light on atomic dynamics driven by intense laser fields in this critical energy region.
- ItemReconstruction of the time-dependent electronic wave packet arising from molecular autoionization(Washington, DC [u.a.] : Assoc., 2018) Bello, Roger Y.; Canton, Sophie E.; Jelovina, Denis; Bozek, John D.; Rude, Bruce; Smirnova, Olga; Ivanov, Mikhail Y.; Palacios, Alicia; Martín, FernandoAutoionizing resonances are paradigmatic examples of two-path wave interferences between direct photoionization, which takes a few attoseconds, and ionization via quasi-bound states, which takes much longer. Time-resolving the evolution of these interferences has been a long-standing goal, achieved recently in the helium atom owing to progress in attosecond technologies. However, already for the hydrogen molecule, similar time imaging has remained beyond reach due to the complex interplay between fast nuclear and electronic motions. We show how vibrationally resolved photoelectron spectra of H2 allow one to reconstruct the associated subfemtosecond autoionization dynamics by using the ultrafast nuclear dynamics as an internal clock, thus forgoing ultrashort pulses. Our procedure should be general for autoionization dynamics in molecules containing light nuclei, which are ubiquitous in chemistry and biology.
- ItemPhotodissociation of aligned CH3I and C6H3F2I molecules probed with time-resolved Coulomb explosion imaging by site-selective extreme ultraviolet ionization(Melville, NY : AIP Publishing LLC, 2018) Amini, Kasra; Savelyev, Evgeny; Brauße, Felix; Berrah, Nora; Bomme, Cédric; Brouard, Mark; Burt, Michael; Christensen, Lauge; Düsterer, Stefan; Erk, Benjamin; Höppner, Hauke; Kierspel, Thomas; Krecinic, Faruk; Lauer, Alexandra; Lee, Jason W. L.; Müller, Maria; Müller, Erland; Mullins, Terence; Redlin, Harald; Schirmel, Nora; Thøgersen, Jan; Techert, Simone; Toleikis, Sven; Treusch, Rolf; Trippel, Sebastian; Ulmer, Anatoli; Vallance, Claire; Wiese, Joss; Johnsson, Per; Küpper, Jochen; Rudenko, Artem; Rouzée, Arnaud; Stapelfeldt, Henrik; Rolles, Daniel; Boll, RebeccaWe explore time-resolved Coulomb explosion induced by intense, extreme ultraviolet (XUV) femtosecond pulses from a free-electron laser as a method to image photo-induced molecular dynamics in two molecules, iodomethane and 2,6-difluoroiodobenzene. At an excitation wavelength of 267 nm, the dominant reaction pathway in both molecules is neutral dissociation via cleavage of the carbon-iodine bond. This allows investigating the influence of the molecular environment on the absorption of an intense, femtosecond XUV pulse and the subsequent Coulomb explosion process. We find that the XUV probe pulse induces local inner-shell ionization of atomic iodine in dissociating iodomethane, in contrast to non-selective ionization of all photofragments in difluoroiodobenzene. The results reveal evidence of electron transfer from methyl and phenyl moieties to a multiply charged iodine ion. In addition, indications for ultrafast charge rearrangement on the phenyl radical are found, suggesting that time-resolved Coulomb explosion imaging is sensitive to the localization of charge in extended molecules.