Monitoring Nonadiabatic Electron-Nuclear Dynamics in Molecules by Attosecond Streaking of Photoelectrons
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Kowalewski, Markus↗
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Results for “electron streaking”
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Reconstruction of the complex angle-dependent photoionization transition dipole from a laser-dressed streaking experiment
We study the retrieval of the angular dependence of the photoionization transition dipole phase of an attosecond XUV pulse in order to reconstruct the whole photoelectron wave packet after the photoemission process. Using a one-electron model Ar atom, we show that the full electron wave packet can be reconstructed from IR-free photoelectron angular distributions and the streaking electron spectra in an IR-dressed XUV photoionization, with photoelectrons along the common polarization direction of the two pulses. The method relies on the validity of the strong-field approximation so it is valid only for higher energy photoelectrons. Here, we also point out that a single photoionization group time delay is not enough to represent a photoemission process; instead, a complete characterization of the electron wave packet requires the retrieval of the spectral phase over the whole bandwidth of the wave packet.
74 ATOMIC AND MOLECULAR PHYSICS↗
Implementing time resolved electron temperature capability at the NIF using a streak camera
A new capability on NIF has been implemented to measure the temperature of x-ray emitting sources. Although it is designed primarily for Inertial Confinement Fusion (ICF), it can be used for any hot emitting source that is well modeled. The electron temperature (T e ) of the hot spot within the core of imploded inertial confinement fusion capsules is an effective indicator of implosion performance. Currently, there are spatially and temporally integrated T e inferences using image plates. A temporally resolved measurement of Te will help elucidate the mechanisms for hot spot heating and cooling such as conduction to fuel, alpha-heating, mix and radiative losses. To determine the temporally resolved T e of hot spots, specific filters are added to an existing x-ray streak camera “Streaked Polar Instrumentation for Diagnosing Energetic Radiation (SPIDER)” to probe the emission spectrum during the x-ray burn history of implosions on the National Ignition Facility (NIF). One of the difficulties in inferring the hot spot temperature is the attenuation of the emission due to opacity from the shell and fuel. Therefore, a series of increasingly thick titanium filters were implemented to isolate the emission in specific energy regions that are sensitive to temperatures above 3keV while not significantly influenced by the shell/fuel attenuation. Additionally, a relatively thin zinc filter was used to measure the contribution of colder emission sources. Since the signal levels of the emission through the thicker filters are relatively poor, a dual slit (aperture) was designed to increase detected signal at the higher end of the spectrum. Herein, the design of the filters and slit are described, an overview of the solving technique is provided, and initial electron temperature results are reported.
47 OTHER INSTRUMENTATION↗
Attosecond Streaking Time Delays: Finite-Range Interpretation and Applications
We review theoretical studies of the attosecond streaking time delay concept in photoionization via the investigation of the electron dynamics in the streaking field after the transition of the photoelectron into the continuum upon absorption of an extreme ultraviolet photon. Based on the results, a so-called finite range interpretation was introduced, which highlighted that the delay is accumulated until the streaking pulse ends and, hence, over a finite range of the potential of the parent ion. Following a discussion of the analysis leading to this interpretation, we summarize a few applications which provide insights into different aspects of the streaking time delay concept in photoionization. Besides a review of previously presented results, we give an analysis of the relevance of the first half-cycle of the streaking field and an outlook regarding the perspective of using the streaking method to resolve dynamical changes in the potential that the photoelectron explores during its propagation in the continuum.
72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
Retrieving plasmonic near-field information: A quantum-mechanical model for streaking photoelectron spectroscopy of gold nanospheres
Streaked photoemission from nanostructures is characterized by size- and material-dependent nanometer-scale variations of the induced nanoplasmonic response to the electronic field of the streaking pulse and thus holds promise of allowing photoelectron imaging with both subfemtosecond temporal and nanometer spatial resolution. In order to scrutinize the driven collective electronic dynamics in 10–200-nm-diameter gold nanospheres, we calculated the plasmonic field induced by streaking pulses in the infrared and visible spectral range and developed a quantum-mechanical model for streaked photoemission by extreme ultraviolet pulses. Overall, our simulated photoelectron spectra reveal a significant amplitude enhancement and phase shift of the photoelectron streaking trace relative to calculations that exclude the induced plasmonic field. Both are most pronounced for streaking pulses tuned to the plasmon frequency and retrace the plasmonic electromagnetic field enhancement and phase shift near the nanosphere surface.
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
Elucidating structural order and disorder phenomena in mullite-type Al{sub 4}B{sub 2}O{sub 9} by automated electron diffraction tomography
The crystal structure and disorder phenomena of Al{sub 4}B{sub 2}O{sub 9}, an aluminum borate from the mullite-type family, were studied using automated diffraction tomography (ADT), a recently established method for collection and analysis of electron diffraction data. Al{sub 4}B{sub 2}O{sub 9}, prepared by sol-gel approach, crystallizes in the monoclinic space group C2/m. The ab initio structure determination based on three-dimensional electron diffraction data from single ordered crystals reveals that edge-connected AlO{sub 6} octahedra expanding along the b axis constitute the backbone. The ordered structure (A) was confirmed by TEM and HAADF-STEM images. Furthermore, disordered crystals with diffuse scattering along the b axis are observed. Analysis of the modulation pattern implies a mean superstructure (AAB) with a threefold b axis, where B corresponds to an A layer shifted by ½a and ½c. Diffraction patterns simulated for the AAB sequence including additional stacking disorder are in good agreement with experimental electron diffraction patterns. - Graphical abstract: Crystal structure and disorder phenomena of B-rich Al{sub 4}B{sub 2}O{sub 9} studied by automated electron diffraction tomography (ADT) and described by diffraction simulation using DISCUS. - Highlights: • Ab-initio structure solution by electron diffraction from single nanocrystals. • Detected modulation corresponding mainly to three-fold superstructure. • Diffuse diffraction streaks caused by stacking faults in disordered crystals. • Observed streaks explained by simulated electron diffraction patterns.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
The Echo 4 electron beam experiment - Television observation of artificial auroral streaks indicating strong beam interactions in the high-latitude magnetosphere
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Hallinan, T. J.↗
Simultaneous Spectral Temporal Adaptive Raman Spectrometer - SSTARS
Raman spectroscopy is a prime candidate for the next generation of planetary instruments, as it addresses the primary goal of mineralogical analysis, which is structure and composition. However, large fluorescence return from many mineral samples under visible light excitation can render Raman spectra unattainable. Using the described approach, Raman and fluorescence, which occur on different time scales, can be simultaneously obtained from mineral samples using a compact instrument in a planetary environment. This new approach is taken based on the use of time-resolved spectroscopy for removing the fluorescence background from Raman spectra in the laboratory. In the SSTARS instrument, a visible excitation source (a green, pulsed laser) is used to generate Raman and fluorescence signals in a mineral sample. A spectral notch filter eliminates the directly reflected beam. A grating then disperses the signal spectrally, and a streak camera provides temporal resolution. The output of the streak camera is imaged on the CCD (charge-coupled device), and the data are read out electronically. By adjusting the sweep speed of the streak camera, anywhere from picoseconds to milliseconds, it is possible to resolve Raman spectra from numerous fluorescence spectra in the same sample. The key features of SSTARS include a compact streak tube capable of picosecond time resolution for collection of simultaneous spectral and temporal information, adaptive streak tube electronics that can rapidly change from one sweep rate to another over ranges of picoseconds to milliseconds, enabling collection of both Raman and fluorescence signatures versus time and wavelength, and Synchroscan integration that allows for a compact, low-power laser without compromising ultimate sensitivity.
Blacksberg, Jordana↗
Atomic-Scale Structure and Non-Stoichiometry of Meteoritic Hibonite: A Transmission Electron Microscope Study
Hibonite (CaAl_12O_19) is a common refractory mineral in Ca-Al-rich inclusions (CAIs) in primitive meteorites. Transmission electron microscope (TEM) studies have identified enigmatic planar defects in different occurrences of hibonite in the Allende meteorite that give rise to strong streaking along c* in electron diffraction patterns. Atomic resolution high-angle annular dark-field (HAADF) imaging and energy-dispersive X-ray (EDX) analyses were used to determine the nature and origin of these planar features. HAADF images of hibonite grains reveal lamellar intergrowths of common 1.6 nm spacing, and less commonly 2.0 and 2.5 nm spacings, interspersed in stoichiometric hibonite showing 1.1 nm (002) spacing. Stoichiometric hibonite consists of alternating Ca-containing (“R”) and spinel-structured (“S”) blocks stacked in a sequence RS. In contrast, the 1.6 nm layers result from a doubled S block such that the stacking sequence is RSS, while in the widest defect observed, the stacking sequence is RSSSS. These intergrowths are epitaxial and have coherent, low-strain boundaries with the host hibonite Meteoritic hibonite shows common Ti and Mg substitution for Al in its structure. Atomic-resolution EDX maps of hibonite grains in the Allende CAI confirm the preferred site occupancy of Mg on tetragonal M3 sites in S blocks and of Ti on trigonal bipyramidal M2 and octahedral M4 sites in R blocks. Mg is highly concentrated, but Ti is absent in the planar defects where wider S blocks show Al-rich compositions compared to stoichiometric MgAl_2O_4 spinel. Therefore, Mg likely played the major role in the formation and metastability of planar defects in hibonite. Electron energy loss spectroscopy data from the Ti L_2,3 edge show the presence of mixed Ti oxidation states with ~ 15–20% of Ti as Ti^(3+) in hibonite, suggesting a direct substitution of Ti^(3+) ↔ Al^(3+) in hibonite. The remaining ~ 80–85% of Ti is present as Ti^(4+) and corresponding EDX analyses are consistent with the well-known coupled substitution 2Al^(3+) ↔ Ti^(4+) + Mg^(2+) being the major mechanism for Ti and Mg substitution in hibonite. The formation of planar defects in hibonite occurred during high-temperature nebular condensation or melting/crystallization processes. The occurrence of non-stoichiometric hibonite in the Allende CAI deviates from the mineral formation sequence predicted from equilibrium condensation models. Overall, our atomic resolution TEM observations signify non-equilibrium, kinetic-controlled crystal growth during the high-temperature formation of refractory solids in the early solar nebula.
hibonite↗
Picosecond-resolved X-ray absorption spectroscopy at low signal contrast using a hard X-ray streak camera
A picosecond-resolving hard-X-ray streak camera has been in operation for several years at Sector 7 of the Advanced Photon Source (APS). Several upgrades have been implemented over the past few years to optimize integration into the beamline, reduce the timing jitter, and improve the signal-to-noise ratio. These include the development of X-ray optics for focusing the X-rays into the sample and the entrance slit of the streak camera, and measures to minimize the amount of laser light needed to generate the deflection-voltage ramp. For the latter, the photoconductive switch generating the deflection ramp was replaced with microwave power electronics. With these, the streak camera operates routinely at 88 MHz repetition rate, thus making it compatible with all of the APS fill patterns including use of all the X-rays in the 324-bunch mode. Sample data are shown to demonstrate the performance.
38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
Laser acceleration and deflection of 963 keV electrons with a silicon dielectric structure
Radio frequency particle accelerators are ubiquitous in ultrasmall and ultrafast science, but their size and cost have prompted exploration of compact and scalable alternatives such as the dielectric laser accelerator. We present the first demonstration, to the best of our knowledge, of high gradient laser acceleration and deflection of electrons with a silicon structure. Driven by a 5 nJ, 130 fs mode-locked Ti:sapphire laser at 907 nm wavelength, our devices achieve accelerating gradients in excess of 200 MeV/m and suboptical cycle streaking of 96.30 keV electrons. Lastly, these results pave the way for high gradient silicon dielectric laser accelerators using commercial lasers and subfemtosecond electron beam experiments.
43 PARTICLE ACCELERATORS↗
Characterization of single-shot attosecond pulses with angular streaking photoelectron spectra
Most of the traditional attosecond pulse retrieval algorithms are based on a so-called attosecond streak camera technique, in which the momentum of the electron is shifted by an amount depending on the relative time delay between the attosecond pulse and the streaking infrared pulse. Thus, temporal information of the attosecond pulse is encoded in the amount of momentum shift in the streaked photoelectron momentum spectrogram S(p,τ), where p is the momentum of the electron along the polarization direction and τ is the time delay. An iterative algorithm is then employed to reconstruct the attosecond pulse from the streaking spectrogram. This method, however, cannot be applied to attosecond pulses generated from free-electron x-ray lasers where each single shot is different and stochastic in time. However, using a circularly polarized infrared laser as the streaking field, a two (or three)-dimensional angular streaking electron spectrum can be used to retrieve attosecond pulses for each shot, as well as the time delay with respect to the circularly polarized IR field. Here we show that a retrieval algorithm previously developed for the traditional streaking spectrogram can be modified to efficiently characterize single-shot attosecond pulses. The methods have been applied to retrieve 188 single shots from recent experiments. We analyze the statistical behavior of these 188 pulses in terms of pulse duration, bandwidth, pulse peak energy, and time delay with respect to the IR field. Furthermore, the retrieval algorithm is efficient and can be easily used to characterize a large number of shots in future experiments for attosecond pulses at free-electron x-ray laser facilities.
74 ATOMIC AND MOLECULAR PHYSICS↗
Performance of a hardened x-ray streak camera at Lawrence Livermore National Laboratory’s National Ignition Facility
Electron tubes continue to provide the highest speeds possible for recording dynamics of hot high-energy density plasmas. Standard streak camera drive electronics and CCD readout are not compatible with the radiation environment associated with high DT fusion yield inertial confinement fusion experiments >10 13 14 MeV DT neutrons or >10 9 n cm -2 ns -1 . Here, we describe a hardened x-ray streak camera developed for the National Ignition Facility and present preliminary results from the first experiment on which it has participated, recording the time-resolved bremsstrahlung spectrum from the core of an inertial confinement fusion implosion at more than 40× the operational neutron yield limit of the previous National Ignition Facility x-ray streak cameras.
47 OTHER INSTRUMENTATION↗
Streamers at the Subnanosecond Breakdown of Argon and Nitrogen in Nonuniform Electric Field at Both Polarities
An ICCD camera was used to study plasma glow at the stage of the streamer (ionization wave) formation in the tip–plane gap with a length of 3 mm filled with argon or nitrogen at a pressure of 12.5–400 kPa. Positive and negative nanosecond voltage pulses were applied across the gap. Images of streamer were obtained at different time at its propagation along the gap. A streak-camera equipped with a spectrometer was used to measure time evolution of the radiation intensity of nitrogen molecules at a wavelength of 337.1 nm in several regions along the gap at the negative polarity. Average streamer velocity (1.8 cm/ns) was estimated from experimental data at atmospheric pressure of nitrogen. Amplitude–time characteristics of voltage, discharge current and the current of runaway electron beam behind the aluminum-foil anode with a thickness of 10 μm were measured. Reasons for a diffuse discharge under the given experimental conditions were discussed.
70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
Megahertz-compatible angular streaking with few-femtosecond resolution at x-ray free-electron lasers
Highly brilliant, coherent, femtosecond x-ray pulses delivered by free-electron lasers (FELs) constitute one of the pillars of modern ultrafast science. Next generation FEL facilities provide up to megahertz repetition rates and pulse durations down to the attosecond regime utilizing self-amplification of spontaneous emission. However, the stochastic nature of this generation mechanism demands single-shot pulse characterization to perform meaningful experiments. Here we demonstrate a fast yet robust online analysis technique capable of megahertz-rate mapping of the temporal intensity structure and arrival time of x-ray FEL pulses with few-femtosecond resolution. We performed angular streaking measurements of both neon photo- and Auger electrons and show their applicability for a direct time-domain feedback system during ongoing experiments. Here, the fidelity of the real-time pulse characterization algorithm is corroborated by resolving isolated x-ray pulses and double pulse trains with few-femtosecond substructure, thus paving the way for x-ray-pump–x-ray-probe FEL science at repetition rates compatible with the demands of LCLS-II and European XFEL.
74 ATOMIC AND MOLECULAR PHYSICS↗
THz-driven zero-slippage IFEL scheme for phase space manipulation
Not Available
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
Temporal profile measurements of relativistic electron bunch based on wakefield generation
A complete characterization of the time-resolved longitudinal beam phase space is important to optimize the final performances of an accelerator, and in particular this is crucial for Free Electron Laser (FEL) facilities. In this study we propose a novel method to characterize the profile of a relativistic electron bunch by passively streaking the beam using its self-interaction with the transverse wakefield excited by the bunch itself passing off-axis through a dielectric-lined or a corrugated waveguide. Results of a proof-of-principle experiment at the SwissFEL Injector Test Facility are discussed.
43 PARTICLE ACCELERATORS↗
Gated Photocathode Design for the P510 Electron Tube used in the National Ignition Facility (NIF) Optical Streak Cameras
Abstract not provided
42 ENGINEERING↗