Generation of highly mutually coherent hard-x-ray pulse pairs with an amplitude-splitting delay line
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71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
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Speckle contrast from the split-and-delay unit with seeded X-ray pulses of the MID instrument at European XFEL
We report on the coherence properties and characteristics of the split- and-delay unit at the Materials Imaging and Dynamics instrument of the European XFEL under seeded-beam conditions. Our investigation focuses on the speckle contrast extracted from the scattering patterns from static scatterers and pulse splitting characteristics. Seeded-beam operation enabled a high throughput of the split-and-delay unit. We highlight the invaluable potential of the split-and-delay unit for experimental investigations for enhancing our understanding of ultrafast phenomena in molecular liquids, such as water and aqueous solutions.
Fuoss, Paul↗
Double-pulse speckle contrast correlations with near Fourier transform limited free-electron laser light using hard X-ray split-and-delay
Abstract The ability to deliver two coherent X-ray pulses with precise time-delays ranging from a few femtoseconds to nanoseconds enables critical capabilities of probing ultra-fast phenomena in condensed matter systems at X-ray free electron laser (FEL) sources. Recent progress made in the hard X-ray split-and-delay optics developments now brings a very promising prospect for resolving atomic-scale motions that were not accessible by previous time-resolved techniques. Here, we report on characterizing the spatial and temporal coherence properties of the hard X-ray FEL beam after propagating through split-and-delay optics. Speckle contrast analysis of small-angle scattering measurements from nanoparticles reveals well-preserved transverse coherence of the beam. Measuring intensity fluctuations from successive X-ray pulses also reveals that only single or double temporal modes remain in the transmitted beam, corresponding to nearly Fourier transform limited pulses.
42 ENGINEERING↗
Hard x-ray – optical four-wave mixing using a split-and-delay line
New, hard x-ray free electron lasers (FEL) produce intense femtosecond-to-attosecond pulses at angstrom wavelengths, giving access to the fundamental spatial and temporal scales of matter. These revolutionary light sources open the door to applying the suite of nonlinear, optical spectroscopy methods at hard x-ray photon energies. Nonlinear spectroscopy with hard x-rays can allow for measuring the coherence properties of short wavelength excitations with atomic specificity and for understanding how high energy excitations couple to other degrees of freedom in atomic, molecular or condensed-phase systems. As a step in this direction, here we present hard x-ray, optical four-wave mixing (4WM) measurements done at 9.8 keV at the split-and-delay line at the x-ray correlation spectroscopy (XCS) hutch of the Linac Coherent Light Source (LCLS). In this work, we create an x-ray transient grating (TG) from a pair of crossing x-ray beams and diffract optical laser pulses at 400 nm from the TG. The key technical advance here is being able to independently vary the delays of the x-ray pulses. Measurements were made in 3 different solid samples: bismuth germinate (BGO), zinc oxide (ZnO) and yttrium aluminum garnet (YAG). The resulting phase-matched, 4WM signal is measured in two different ways: by varying the x-ray, x-ray pulse delay which can reveal both material and light source coherence properties and also by varying the optical laser delay with respect to the x-ray TG to study how the x-ray excitation couples to the optical properties. Although no coherent 4WM signal was seen in these measurements, the absence of this signal gives important information on experimental requirements for detecting this in future work. Also, our laser-delay scans, although not a new measurement, were applied to different materials than in past work and reveal new examples x-ray induced lattice dynamics in solids. This work represents a key step towards extending nonlinear optics and time-resolved spectroscopy into the hard x-ray regime.
47 OTHER INSTRUMENTATION↗
Femtosecond x-ray photon correlation spectroscopy enables direct observations of atomic-scale relaxations of glass forming liquids
Glass-forming liquids exhibit structural relaxation behaviors, reflecting underlying atomic rearrangements on a wide range of timescales and playing a crucial role in determining material properties. However, the relaxation processes on the atomic scale are not well-understood due to the experimental difficulties in directly characterizing the evolving correlations of atomic-scale order in disordered systems. Here, in this study, we harness the coherence and ultrashort pulse characteristics of an x-ray free electron laser to directly probe atomic-scale ultrafast relaxation dynamics in the model system Ge 15 Te 85 . We demonstrate an analysis strategy for determining the intermediate scattering function by extracting the contrast decay of summed scattering patterns from two rapidly successive, nearly identical femtosecond x-ray pulses generated by a split-delay system. The result indicates a full decorrelation of atomic-scale order on the sub-picosecond timescale, supporting the argument for a high-fluidity fragile state of liquid Ge 15 Te 85 above its dynamic crossover temperature. The demonstrated strategy opens an avenue for experimental studies of relaxation dynamics in liquids, glasses, and other highly disordered systems.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Design of an amplitude-splitting hard x-ray delay line with subnanoradian stability
We propose the design and analysis of a hard x-ray split-delay optical arrangement that combines diffractive and crystal optics. Transmission gratings are employed to achieve the much-desired amplitude splitting and recombination of the beam. Asymmetric channel-cut crystals are utilized to tune the relative delay time. The use of a dispersion-compensation arrangement of the crystals allows the system to achieve subnanoradian pointing stability during a delay scan. It further minimizes wavefront distortion and preserves the pulse front and pulse duration. We analyze the performance of a prototype design that can cover a delay time range of 15 ps with a sub-20 fs time resolution at 10 keV. We anticipate that this system can fully satisfy the very demanding stability requirements for performing split-pulse x-ray photon correlation spectroscopy measurements for the investigation of fast atomic scale dynamics in complex disordered matter.
47 OTHER INSTRUMENTATION↗
Data driven drift correction for complex optical systems
To exploit the thousand-fold increase in spectral brightness of modern light sources, increasingly intricate experiments are being conducted that demand extremely precise beam trajectory. Maintaining the optimal trajectory over several hours of an experiment with the needed precision necessitates active drift control. Here, we outline time varying Bayesian optimization (TVBO) as a data driven approach for robust drift correction, and illustrate its application for a split and delay optical system composed of six crystals and twelve input dimensions. Using numerical simulations, we exhibit the application of TVBO for linear drift, non-smooth temporal drift as well as constrained TVBO for multi-objective control settings, representing real-life operating conditions. This approach can be easily adapted to other X-ray beam conditioning and guidance systems, including multi-crystal monochromators and grazing-incidence mirrors, to maintain sub-micrometer and nanoradian beam stability over the course of an experiment spanning several hours.
Bayesian optimization↗
Split-pulse X-ray photon correlation spectroscopy with seeded X-rays from X-ray laser to study atomic-level dynamics
Abstract With their brilliance and temporal structure, X-ray free-electron laser can unveil atomic-scale details of ultrafast phenomena. Recent progress in split-and-delay optics (SDO), which produces two X-ray pulses with time-delays, offers bright prospects for observing dynamics at the atomic-scale. However, their insufficient pulse energy has limited its application either to phenomena with longer correlation length or to measurement with a fixed delay-time. Here we show that the combination of the SDO and self-seeding of X-rays increases the pulse energy and makes it possible to observe the atomic-scale dynamics in a timescale of picoseconds. We show that the speckle contrast in scattering from water depends on the delay-time as expected. Our results demonstrate the capability of measurement using the SDO with seeded X-rays for resolving the dynamics in temporal and spatial scales that are not accessible by other techniques, opening opportunities for studying the atomic-level dynamics.
36 MATERIALS SCIENCE↗
Domain Knowledge Guided Bayesian Optimization For Autonomous Alignment Of Complex Scientific Instruments
Bayesian Optimization (BO) is a powerful tool for optimizing complex non-linear systems. However, its performance degrades in high-dimensional problems with tightly coupled parameters and highly asymmetric objective landscapes, where rewards are sparse. In such needle-in-a-haystack scenarios, even advanced methods like trust-region BO (TurBO) often lead to unsatisfactory results. We propose a domain knowledge guided Bayesian Optimization approach, which leverages physical insight to fundamentally simplify the search problem by transforming coordinates to decouple input features and align the active subspaces with the primary search axes. We demonstrate this approach's efficacy on a challenging 12-dimensional, 6-crystal Split-and-Delay optical system, where conventional approaches, including standard BO, TuRBO and multi-objective BO, consistently led to unsatisfactory results. When combined with an reverse annealing exploration strategy, this approach reliably converges to the global optimum. The coordinate transformation itself is the key to this success, significantly accelerating the search by aligning input co-ordinate axes with the problem's active subspaces. As increasingly complex scientific instruments, from large telescopes to new spectrometers at X-ray Free Electron Lasers are deployed, the demand for robust high-dimensional optimization grows. Our results demonstrate a generalizable paradigm: leveraging physical insight to transform high-dimensional, coupled optimization problems into simpler representations can enable rapid and robust automated tuning for consistent high performance while still retaining current optimization algorithms.
FOS: Computer and information sciences↗
Understanding attosecond streaking
Abstract This tutorial provides an overview on the theory of attosecond streaking, a pump-probe scheme to extract timing information of ionization processes that has been widely used in the past decade. Emphasis is put on the origin of the Coulomb-laser-coupling (CLC) term, which is crucial in the interpretation of streaking delays. Having gained a proper understanding of how the CLC terms in various publications relate to each other, we will be able to analyze in which regime the streaking delay can be split into a measurement-induced CLC term and a ‘pure’ ionization delay and under which conditions this splitting may break down. Thus we address the long-standing question of the validity of the widely applied interpretation of the streaking delay as a sum of the CLC term and a ‘pure’ ionization delay.
Physics↗
Network-Wide Traffic Signal Control Using Bilinear System Modeling and Adaptive Optimization
This study proposes a new multi-input multi-output optimal bilinear signal control method in which a bilinear dynamic model approximation is used to capture the nonlinear dynamics of the urban traffic networks. With signal green time splits as the control input and traffic delay changes as the output for each intersections in the network, a bilinear system model was developed, which, on the basis of linear system modeling, takes interactions among traffic delays and signal timing splits into consideration. Based on the bilinear system modeling framework, we conducted two steps in each time interval to derive traffic control strategies: (1) we used the normalized least-squared algorithm to estimate system parameters; and (2) we solved an online optimization problem to obtain the updated traffic control inputs for the signal timing that minimizes future traffic delays. We evaluated the proposed method in a microscopic traffic simulation environment (VISSIM) with a 35-intersection network of Bellevue city in Washington. Two different traffic demand patterns: (1) normal traffic demands; and (2) time-varying traffic demands were simulated to compare the performance of different control strategies. Experimental results show that (1) the proposed bilinear system model can better describe traffic system dynamics than linear-model based methods, such as our previously developed linear-quadratic regulator control; and (2) the proposed method outperforms the state-of-the-art signal control strategies, namely the max-pressure and the self-organizing traffic light control methods. We have also shown that the proposed method is applicable to all other possible network layouts and signal controller phasing structures.
42 ENGINEERING↗
Ultrafast heat transfer in single palladium nanocrystals seen with an X-ray free-electron laser
We report transient highly strained structural states in individual palladium (Pd) nanocrystals, electronically heated using an optical laser, which precede their uniform thermal expansion. Using an X-ray free-electron laser probe, the evolution of individual 111 Bragg peaks is measured as a function of delay time at various laser fluences. Above a laser fluence threshold at a sufficient pump-probe delay, the Bragg peak splits into multiple peaks, indicating heterogeneous strain, before returning to a single peak, corresponding to even heat distribution throughout the lattice expanded crystal. Our findings are supported by a lattice displacement and strain model of a single nanocrystal at different delay times, which agrees with the experimental data. Our observations have implications for understanding femtosecond laser interactions with metals and the potential photo-catalytic performance of Pd.
36 MATERIALS SCIENCE↗
A database of thermally activated delayed fluorescent molecules auto-generated from scientific literature with ChemDataExtractor
A database of thermally activated delayed fluorescent (TADF) molecules was automatically generated from the scientific literature. It consists of 25,482 data records with an overall precision of 82%. Among these, 5,349 records have chemical names in the form of SMILES strings which are represented with 91% accuracy; these are grouped in a subsidiary database. Each data record contains one of the following four properties: maximum emission wavelength (λ EM ), photoluminescence quantum yield (PLQY), singlet-triplet energy splitting (ΔE ST ), and delayed lifetime (τ D ). The databases were created through text mining using ChemDataExtractor, a chemistry-aware natural-language-processing toolkit, which has been adapted for TADF research. The text-mined corpus consisted of 2,733 papers from the Royal Society of Chemistry and Elsevier. To the best of our knowledge, these databases are the first databases that have been auto-generated for TADF molecules from existing publications. The databases have been publicly released for experimental and computational applications in the TADF research field.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Electron beam echoes in the IOTA ring
This study is a continuation of previous efforts to demonstrate the possibility of electron beam echo generation in the IOTA ring. Transverse beam echoes are conventionally produced by a dipole kick followed by a single quadrupole kick. We seek to use multiple quadrupole kicks over successive turns to generate an echo larger than that from a single kick. We use beam echo theory and simulations to model and predict the expected echo generated by multiple quadrupole kicks. We also run simulated scans over various parameters relevant to the echo to optimize the echo amplitude, including delay time, quadrupole strength, tune split, and pulse number. Effects due to quantum excitation and synchrotron damping (which are particularly relevant with electrons) were also considered in simulation. Results indicate that given sufficient quadrupole kick strength, we should expect to be able to measure electron beam echoes in the IOTA ring.
72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
The Atlantic Jet Response to Stratospheric Events: A Regime Perspective
The tropospheric response to Sudden Stratospheric Warmings (SSWs) is associated with an equatorward shift in the midlatitude jet and associated storm tracks, while Strong Polar Vortex (SPV) events elicit a contrasting response. Recent analyses of the North Atlantic jet using probability density functions of a jet latitude index have identified three preferred jet latitudes, raising the question of whether the tropospheric response to SSWs and SPVs results from a change in relative frequencies of these preferred jet regimes rather than a systematic jet shift. We explore this question using atmospheric reanalysis data from 1979 to 2018 (26 SSWs and 33 SPVs), and a 202-years integration of the Whole Atmosphere Community Climate Model (92 SSWs and 68 SPVs). Following SSWs, the northern jet regime becomes less common and the central and southern regimes become more common. These changes occur almost immediately following “split” vortex events, but are more delayed following “displacement” events. In contrast, the northern regime becomes more frequent and the southern regime less frequent following SPV events. Following SSWs, composites of 500-hPa geopotential heights, surface air temperatures, and precipitation most closely resemble composites of the southern jet regime, and are generally opposite in sign to the composites of the northern jet regime. These comparisons are reversed following SPVs. Thus, one possible interpretation is that the two southernmost regimes appear to be favored following SSWs, while the southernmost regime becomes less common following SPVs.
54 ENVIRONMENTAL SCIENCES↗
Multi-delay coherence imaging spectroscopy optimized for ion temperature measurements in the divertor plasma of the Wendelstein 7-X stellarator
A new coherence imaging spectroscopy (CIS) diagnostic optimized to measure the C 2+ impurity ion temperature T i spatial distribution in the divertor plasma of the W7-X stellarator is designed, tested, and validated. Using CIS to obtain T i in the edge of magnetically confined plasmas has historically been challenging because Doppler broadening and Zeeman splitting have comparable effects on the shape of spectral emission lines. To distinguish between these two mechanisms, a novel approach to birefringent crystal design is employed to minimize the diagnostic’s sensitivity to Zeeman splitting. The recently developed pixelated multi-delay CIS approach is also used to obtain four times as much spectral information as traditional CIS approaches. The T i -optimized CIS diagnostic is validated in a long-pulse W7-X plasma by comparison with a high-resolution spectrometer whose sightlines overlap with the CIS field of view. The CIS and spectrometer T i profiles have the same shape and agree to within 10% on average and 25% in the worst case. Images of the T i distribution near the divertor show toroidally elongated bands aligned with the magnetic field, with T i ranging between 10 and 40 eV.
70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
High-energy X-ray radiography with apodized petawatt laser beams
We have produced laser wakefield-accelerated electron beams with energies of 2 GeV in Target Area 1 of the ZEUS facility. These electron beams oscillate in the accelerating structure that is produced in the wake of an ultrashort laser pulse (25 fs). These ’betatron’ oscillations result in the emission of a collimated (4 mrad divergence) beam of high-energy X-ray/gamma photons (on the order of several hundred keV). In this work, we demonstrate the capabilities of the ZEUS laser system by showing that apodizing the laser beam in the near field allows for the production of high-quality betatron X-rays for radiography purposes. This demonstrates that a high-power, large-aperture laser beam could be split into multiple parts to drive betatron X-ray sources from multiple angles or temporal delays into a High Energy Density (HED) target to be probed, enabling pump-probe measurements at multiple temporal delays or tomography on a single shot.
70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
Constraints on the Hubble constant from supernova Refsdal’s reappearance
The Hubble constant measures the expansion rate of the Universe, but different methods give inconsistent values. Kelly et al. studied a supernova that had its light split into multiple images by the gravitational lensing of a foreground galaxy cluster. They combined measurements of the time delay between the multiple images with predictions made by multiple lensing models of the cluster. Furthermore, this approach allowed the authors to make a blinded measurement of the Hubble constant, finding a value that is more consistent with that derived from the cosmic microwave background than with the cosmic distance ladder.
79 ASTRONOMY AND ASTROPHYSICS↗