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Medvedev, Nikita

Publications and source records attributed to Medvedev, Nikita.

Effect of Auger recombination on transient optical properties in XUV and soft X-ray irradiated silicon nitride

Spatially encoded measurements of transient optical transmissivity became a standard tool for temporal diagnostics of free-electron-laser (FEL) pulses, as well as for the arrival time measurements in X-ray pump and optical probe experiments. The modern experimental techniques can measure changes in optical coefficients with a temporal resolution better than 10 fs. This, in an ideal case, would imply a similar resolution for the temporal pulse properties and the arrival time jitter between the FEL and optical laser pulses. However, carrier transport within the material and out of its surface, as well as carrier recombination may, in addition, significantly decrease the number of carriers. This would strongly affect the transient optical properties, making the diagnostic measurement inaccurate. Below we analyze in detail the effects of those processes on the optical properties of XUV and soft X-ray irradiated Si 3 N 4 , on sub-picosecond timescales. Si 3 N 4 is a wide-gap insulating material widely used for FEL pulse diagnostics. Theoretical predictions are compared with the published results of two experiments at FERMI and LCLS facilities, and with our own recent measurement. The comparison indicates that three body Auger recombination strongly affects the optical response of Si 3 N 4 after its collisional ionization stops. By deconvolving the contribution of Auger recombination, in future applications one could regain a high temporal resolution for the reconstruction of the FEL pulse properties measured with a Si 3 N 4 -based diagnostics tool.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Fundamental Phenomena and Applications of Swift Heavy Ion Irradiations

This review concentrates on the specific properties and characteristics of damage structures generated with high-energy ions in the electronic energy loss regime. Irradiation experiments with so-called swift heavy ions (SHIs) find applications in many different fields, with examples presented in ion-track nanotechnology, radiation hardness analysis of functional materials, and laboratory tests of cosmic radiation. The basics of the SHI-solid interaction are described with special attention to processes in the electronic subsystem. The broad spectrum of damage phenomena is exemplified for various materials and material classes, along with a description of typical characterization techniques. This review also presents state-of-the-art modeling efforts that try to account for the complexity of the coupled processes of the electronic and atomic subsystems. Lastly, a brief discussion at the end of this review on SHI phenomena induced by fission fragments in nuclear materials will highlight the relevance of energetic ion irradiation in nuclear technology applications.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Spectroscopic Signature of Chemical Bond Dissociation Revealed by Calculated Core-Electron Spectra

The advent of ultrashort soft X-ray pulse sources permits the use of established gas-phase spectroscopy methods to investigate ultrafast photochemistry in isolated molecules with element and site specificity. In the present study, we simulate excited-state wavepacket dynamics of a prototypical process, the ultrafast photodissociation of methyl iodide. Using the simulation, we calculate time-dependent excited-state carbon edge photoelectron and Auger electron spectra. We observe distinct signatures in both types of spectra and show their direct connection to C–I bond dissociation and charge rearrangement processes in the molecule. Finally, we demonstrate at the CH 3 I molecule that the observed signatures allow us to map the time-dependent dynamics of ultrafast photoinduced bond breaking with unprecedented detail.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Time-resolved ionization measurements with intense ultrashort XUV and X-ray free-electron laser pulses

Abstract Modern free-electron lasers (FEL) operating in XUV (extreme ultraviolet) or X-ray range allow an access to novel research areas. One instance is the ultrafast ionization of a solid by an intense femtosecond FEL pulse in XUV which consequently leads to a change of the complex index of refraction on an ultrashort timescale. The photoionization and subsequent impact ionization resulting in electronic and atomic dynamics are modeled with our hybrid code XTANT(X-ray thermal and non-thermal transitions) and a Monte Carlo code XCASCADE(X-ray-induced electron cascades). The simulations predict the temporal kinetics of FEL-induced electron cascades and thus yield temporally and spatially resolved information on the induced changes of the optical properties. In a series of experiments at FERMI and LCLS, single shot measurements with spatio-temporal encoding of the ionization process have been performed by a correlation of the FEL pump pulse with an optical femtosecond probe pulse. An excellent agreement between the experiment and the simulation has been found. Furthermore, we demonstrate that such kind of experiments forms the basis for pulse duration and arrival time jitter monitoring as currently under development for XUV-FELs.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Thermal x-ray diffraction and near-field phase contrast imaging

Using higher-order coherence of thermal light sources, the resolution power of standard x-ray imaging techniques can be enhanced. Here in this work, we applied the higher-order measurement to far-field x-ray diffraction and near-field phase contrast imaging (PCI), in order to achieve superresolution in x-ray diffraction and obtain enhanced intensity contrast in PCI. The cost of implementing such schemes is minimal compared to the methods that achieve similar effects by using entangled x-ray photon pairs.

47 OTHER INSTRUMENTATION↗

Radiation damage free ghost diffraction with atomic resolution

The x-ray free electron lasers can enable diffractive structural determination of protein nanocrystals and single molecules that are too small and radiation-sensitive for conventional x-ray diffraction. However the electronic form factor may be modified during the ultrashort x-ray pulse due to photoionization and electron cascade caused by the intense x-ray pulse. For general x-ray imaging techniques, the minimization of the effects of radiation damage is of major concern to ensure reliable reconstruction of molecular structure. Here in this paper, we show that radiation damage free diffraction can be achieved with atomic spatial resolution by using x-ray parametric down-conversion and ghost diffraction with entangled photons of x-ray and optical frequencies. We show that the formation of the diffraction patterns satisfies a condition analogous to the Bragg equation, with a resolution that can be as fine as the crystal lattice length scale of several Ångstrom. Since the samples are illuminated by low energy optical photons, they can be free of radiation damage.

74 ATOMIC AND MOLECULAR PHYSICS↗

Ultrafast isomerization in acetylene dication after carbon K-shell ionization

Ultrafast proton migration and isomerization are key processes for acetylene and its ions. However, the mechanism for ultrafast isomerization of acetylene [HCCH]2+ to vinylidene [H2CC]2+ dication remains nebulous. Theoretical studies show a large potential barrier ( > 2 eV) for isomerization on low-lying dicationic states, implying picosecond or longer isomerization timescales. However, a recent experiment at a femtosecond X-ray free-electron laser suggests sub-100 fs isomerization. Here we address this contradiction with a complete theoretical study of the dynamics of acetylene dication produced by Auger decay after X-ray photoionization of the carbon atom K shell. We find no sub-100 fs isomerization, while reproducing the salient features of the time-resolved Coulomb imaging experiment. This work resolves the seeming contradiction between experiment and theory and also calls for careful interpretation of structural information from the widely applied Coulomb momentum imaging method.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗