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At least 361 records · Page 20

Clocking Auger electrons

Intense X-ray free-electron lasers (XFELs) can rapidly excite matter, leaving it in inherently unstable states that decay on femtosecond timescales. The relaxation occurs primarily via Auger emission, so excited-state observations are constrained by Auger decay. In situ measurement of this process is therefore crucial, yet it has thus far remained elusive in XFELs owing to inherent timing and phase jitter, which can be orders of magnitude larger than the timescale of Auger decay. Here we develop an approach termed ‘self-referenced attosecond streaking’ that provides subfemtosecond resolution in spite of jitter, enabling time-domain measurement of the delay between photoemission and Auger emission in atomic neon excited by intense, femtosecond pulses from an XFEL. FUrthermore, using a fully quantum-mechanical description that treats the ionization, core-hole formation and Auger emission as a single process, the observed delay yields an Auger decay lifetime of \(2.2_{ - 0.3}^{ + 0.2}\) fs for the KLL decay channel.

47 OTHER INSTRUMENTATION↗

Ultrafast formation of topological defects in a two-dimensional charge density wave

Topological defects play a central role in dynamical systems undergoing a non-adiabatic transition. In solids, topological defects as a result of femtosecond laser excitation have attracted increasing interest not only because they are key to understanding phase transitions but also because they can generate a variety of hidden orders that are not accessible in thermal equilibrium. Despite the common occurrence of these defects in a non-equilibrium system, the fundamental limit on how fast they can emerge in solids and the generic pathway for defect creation at such fast timescales have remained open questions. Here we apply ultrafast electron diffraction to study the reciprocal-space signatures of transient defects in a two-dimensional charge density wave, where simultaneous measurements of both defect and phonon dynamics yield a microscopic view of defect formation in the femtosecond regime. We find that one-dimensional domain walls are generated well within 1 ps following photoexcitation, during which the defect growth is not dictated by the amplitude of the order parameter but is mediated by a non-thermal population of longitudinal optical phonons. In conclusion, our work provides a framework for the ultrafast engineering of topological defects that are coupled to specific collective modes, which will prove useful for the dynamical control of non-equilibrium phases in correlated materials.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

A self-referenced in-situ arrival time monitor for X-ray free-electron lasers

We present a novel, highly versatile, and self-referenced arrival time monitor for measuring the femtosecond time delay between a hard X-ray pulse from a free-electron laser and an optical laser pulse, measured directly on the same sample used for pump-probe experiments. Two chirped and picosecond long optical supercontinuum pulses traverse the sample with a mutually fixed time delay of 970 fs, while a femtosecond X-ray pulse arrives at an instant in between both pulses. Behind the sample the supercontinuum pulses are temporally overlapped to yield near-perfect destructive interference in the absence of the X-ray pulse. Stimulation of the sample with an X-ray pulse delivers non-zero contributions at certain optical wavelengths, which serve as a measure of the relative arrival time of the X-ray pulse with an accuracy of better than 25 fs. We find an excellent agreement of our monitor with the existing timing diagnostics at the SACLA XFEL with a Pearson correlation value of 0.98. We demonstrate a high sensitivity to measure X-ray pulses with pulse energies as low as 30 μJ. Using a free-flowing liquid jet as interaction sample ensures the full replacement of the sample volume for each X-ray/optical event, thus enabling its utility even at MHz repetition rate XFEL sources.

47 OTHER INSTRUMENTATION↗

Hydrogen isotope analysis in W-tiles using fs-LIBS

Abstract Laser-Induced Breakdown Spectroscopy (LIBS) is a promising technology for in-situ analysis of Plasma-Facing Components in magnetic confinement fusion facilities. It is of major interest to monitor the hydrogen isotope retention i.e. tritium and deuterium over many operation hours to guarantee safety and availability of the future reactor. In our studies we use ultraviolet femtosecond laser pulses to analyze tungsten (W) tiles that were exposed to a deuterium plasma in the linear plasma device PSI-2, which mimics conditions at the first wall. A high-resolution spectrometer is used to detect the Balmer- $$\alpha$$ α transition of the surface from implanted hydrogen isotopes (H and D). We use Calibration Free CF-LIBS to quantify the amount of deuterium stored in W. This proof-of-principle study shows the applicability of femtosecond lasers for the detection of low deuterium concentration as present in first wall material of prevailing fusion experiments.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Coherence mapping to identify the intermediates of multi-channel dissociative ionization

Identifying the short-lived intermediates and reaction mechanisms of multi-channel radical cation fragmentation processes remains a current and important challenge to understanding and predicting mass spectra. We find that coherent oscillations in the femtosecond time-dependent yields of several product ions following ultrafast strong-field ionization represent spectroscopic signatures that elucidate their mechanism of formation and identify the intermediate(s) they originate from. Experiments on endo-dicyclopentadiene show that vibrational frequencies from various intermediates are mapped onto their resulting products. Aided by ab initio methods, we identify the vibrational modes of both the cleaved and intact molecular ion intermediates. These results confirm stepwise and concerted fragmentation pathways of the dicyclopentadiene ion. This study highlights the power of tracking the femtosecond dynamics of all product ions simultaneously and sheds further light onto one of the fundamental reaction mechanisms in mass spectrometry, the retro-Diels Alder reaction.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

All hard X-ray transient grating spectroscopy

Optical-domain transient grating (TG) spectroscopy is the ideal tool to investigate transport phenomena in gases, liquids and solids, but it is limited to typically micron-size grating periods. Extreme-Ultraviolet TG has represented a major leap forward to access the mesoscopic scales. Hard X-ray TGs open access in principle to the nanoscale. Hard X-ray TGs were recently generated using the Talbot effect and probed by optical pulses, but these hinder exploiting the advantages of the nanoscale gratings. Here, we present an all-X-ray TG study, in which few-femtosecond hard X-ray pulses are used both for excitation and probing. Our experiment was performed on an amorphous film of an FeGd alloy and on a thin silicon single crystal. The results show a manifestation of the TG induced by the X-ray pump and probe pulses in the form of Talbot carpets, as well as temporal evolution of the grating in crystalline silicon showing coherent optical phonons. Ultrafast all-X-ray TG spectroscopy has the potential to study fundamental excitations with femtosecond time resolution and nanometer spatial sensitivity.

Ferrari, Eugenio [Deutsches Elektronen-Synchrotron↗

Petahertz electronics

Petahertz, or lightwave, electronics uses tailored optical waveforms to control charge carriers in an electronic circuit at petahertz frequencies. This may enable faster processing than conventional pulsed electronics, which cannot be scaled beyond gigahertz frequencies. In recent years, petahertz-scale currents driven by optical fields have been measured in solid-state systems and nanoscale structures, with several proof-of-principle demonstrations of sub-optical-cycle current generation and optical-field-resolved waveform detection at the sub-femtosecond to few-femtosecond scale. Recent work has taken the first steps towards digital and quantum operation by exploring optical-field-driven logic and memory functionality. Here, in this Review, we discuss the progress towards sub-cycle field-driven current injection, highlighting key theoretical concepts, experimental milestones, and questions remaining as we push towards realizing petahertz electronics for ultrafast optical waveform analysis, digital logic, communications, and quantum computation.

Heide, Christian↗

Dynamics of nanoscale phase decomposition in laser ablation

Abstract Laser ablation is a process that bears both fundamental physics interest and has wide industrial applications. For decades, the lack of probes on the relevant time and length scales has prevented access to the highly nonequilibrium phase decomposition processes triggered by laser excitation. In this study, a close integration of time-resolved probing by intense femtosecond X-ray pulses with large-scale atomistic modeling has yielded unique insights into the ablation dynamics of thin gold films irradiated by femtosecond laser pulses. The emergence and growth of nanoscale density heterogeneities in the expanding ablation plume, predicted in the simulations, are mapped to the rapid evolution of distinct small angle diffraction features. This mapping enables identification of the characteristic signatures of different phase decomposition processes occurring simultaneously in the plume, which are driven by photomechanical and thermodynamic driving forces. Beyond the specific insights into the ablation phenomenon, this study demonstrates the power of joint X-ray probing and atomistic modeling of material dynamics under extreme conditions of thermal and mechanical nonequilibrium.

Sun, Yanwen (ORCID:0000000159266565)↗

Expansion dynamics and chemistry evolution in ultrafast laser filament produced plasmas

Laser ablation in conjunction with optical emission spectroscopy is a potential non-contact, standoff detection method for all elements in the periodic table and certain isotopes such as radionuclides. Currently, significant development efforts are on-going to use ultrafast laser filaments for remote sensing. The application of filaments is of particular interest in extending the range of stand-off capability associated with elemental and isotopic detection via laser-induced breakdown spectroscopy. In this study, we characterize the expansion dynamics and chemical evolution of filament-produced uranium (U) plasmas. Laser filaments are generated in the laboratory by loosely focusing 35 femtosecond (fs), 6 milli Joule (mJ) pulses in air. Two-dimensional spectrally-integrated and time-resolved imaging was performed to study hydrodynamics and evolution of U atomic and UO molecular emission in filament-produced U plasmas. Our results highlight that filament ablation of U plasmas gives a cylindrical plasma plume morphology with an appearance of plume splitting into slow and fast moving components at later times of its evolution. Emission from the slow-moving region shows no distinct spectral features (i.e. broadband-like) and is contributed in part by nanoparticles generated during ultrafast laser ablation. Additionally, we find U atoms and U oxide molecules (i.e. UO, UxOy) co-exist in the filament produced plasma, which can be attributed to the generation of low-temperature plasma conditions during filament ablation

(140.3440) Laser-induced breakdown, (280.5395) Pla↗

An excited state dynamics driven reaction: wavelength-dependent photoisomerization quantum yields in [Ru(bpy) 2 (dmso) 2 ] 2+

We report the excited-state behavior of a structurally simple bis -sulfoxide complex, cis -S,S-[Ru(bpy) 2 (dmso) 2 ] 2+ , as investigated by femtosecond pump–probe spectroscopy. The results reveal that a single photon prompts phototriggered isomerization of one or both dmso ligands to yield a mixture of cis -S,O-[Ru(bpy) 2 (dmso) 2 ] 2+ and cis -O,O-[Ru(bpy) 2 (dmso) 2 ] 2+ . The quantum yields of isomerization of each product and relative product distribution are dependent upon the excitation wavelength, with longer wavelengths favoring the double isomerization product, cis -O,O-[Ru(bpy) 2 (dmso) 2 ] 2+ . Transient absorption measurements on cis -O,O-[Ru(bpy) 2 (dmso) 2 ] 2+ do not reveal an excited-state isomerization pathway to produce either the S,O or S,S isomers. Femtosecond pulse shaping experiments reveal no change in the product distribution. Pump–repump–probe transient absorption spectroscopy of cis -S,S-[Ru(bpy) 2 (dmso) 2 ] 2+ shows that a pump–repump time delay of 3 ps dramatically alters the S,O:O,O product ratio; pump–repump–probe transient absorption spectroscopy of cis -O,O-[Ru(bpy) 2 (dmso) 2 ] 2+ with a time delay of 3 ps uncovers an excited-state isomerization pathway to produce the S,O isomer. In conjunction with low-temperature steady-state emission spectroscopy, these results are interpreted in the context of an excited-state bifurcating pathway, in which the isomerization product distribution is determined not by thermodynamics, but rather as a dynamics driven reaction.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Modular droplet injector for sample conservation providing new structural insight for the conformational heterogeneity in the disease-associated NQO1 enzyme

Droplet injection strategies are a promising tool to reduce the large amount of sample consumed in serial femtosecond crystallography (SFX) measurements at X-ray free electron lasers (XFELs) with continuous injection approaches. Here, we demonstrate a new modular microfluidic droplet injector (MDI) design that was successfully applied to deliver microcrystals of the human NAD(P)H:quinone oxidoreductase 1 (NQO1) and phycocyanin. We investigated droplet generation conditions through electrical stimulation for both protein samples and implemented hardware and software components for optimized crystal injection at the Macromolecular Femtosecond Crystallography (MFX) instrument at the Stanford Linac Coherent Light Source (LCLS). Under optimized droplet injection conditions, we demonstrate that up to 4-fold sample consumption savings can be achieved with the droplet injector. In addition, we collected a full data set with droplet injection for NQO1 protein crystals with a resolution up to 2.7 Å, leading to the first room-temperature structure of NQO1 at an XFEL. NQO1 is a flavoenzyme associated with cancer, Alzheimer's and Parkinson's disease, making it an attractive target for drug discovery. Further, our results reveal for the first time that residues Tyr128 and Phe232, which play key roles in the function of the protein, show an unexpected conformational heterogeneity at room temperature within the crystals. These results suggest that different substates exist in the conformational ensemble of NQO1 with functional and mechanistic implications for the enzyme's negative cooperativity through a conformational selection mechanism. Our study thus demonstrates that microfluidic droplet injection constitutes a robust sample-conserving injection method for SFX studies on protein crystals that are difficult to obtain in amounts necessary for continuous injection, including the large sample quantities required for time-resolved mix-and-inject studies.

59 BASIC BIOLOGICAL SCIENCES↗

Low-temperature nanoscale heat transport in a gadolinium iron garnet heterostructure probed by ultrafast x-ray diffraction

Time-resolved x-ray diffraction has been used to measure the low-temperature thermal transport properties of a Pt/Gd3Fe5O12//Gd3Ga5O12 metal/oxide heterostructure relevant to applications in spin caloritronics. A pulsed femtosecond optical signal produces a rapid temperature rise in the Pt layer, followed by heat transport into the Gd3Fe5O12 (GdIG) thin film and the Gd3Ga5O12 (GGG) substrate. The time dependence of x-ray diffraction from the GdIG layer was tracked using an accelerator-based femtosecond x-ray source. The ultrafast diffraction measurements probed the intensity of the GdIG (1 −1 2) x-ray reflection in a grazing-incidence x-ray diffraction geometry. The comparison of the variation of the diffracted x-ray intensity with a model including heat transport and the temperature dependence of the GdIG lattice parameter allows the thermal conductance of the Pt/GdIG and GdIG//GGG interfaces to be determined. Complementary synchrotron x-ray diffraction studies of the low-temperature thermal expansion properties of the GdIG layer provide a precise calibration of the temperature dependence of the GdIG lattice parameter. The interfacial thermal conductance of the Pt/GdIG and GdIG//GGG interfaces determined from the time-resolved diffraction study is of the same order of magnitude as previous reports for metal/oxide and epitaxial dielectric interfaces. The thermal parameters of the Pt/GdIG//GGG heterostructure will aid in the design and implementation of thermal transport devices and nanostructures.

36 MATERIALS SCIENCE↗

Element-specific ultrafast lattice dynamics in FePt nanoparticles

Light–matter interaction at the nanoscale in magnetic alloys and heterostructures is a topic of intense research in view of potential applications in high-density magnetic recording. While the element-specific dynamics of electron spins is directly accessible to resonant x-ray pulses with femtosecond time structure, the possible element-specific atomic motion remains largely unexplored. We use ultrafast electron diffraction (UED) to probe the temporal evolution of lattice Bragg peaks of FePt nanoparticles embedded in a carbon matrix following excitation by an optical femtosecond laser pulse. The diffraction interference between Fe and Pt sublattices enables us to demonstrate that the Fe mean square vibration amplitudes are significantly larger that those of Pt as expected from their different atomic mass. Both are found to increase as energy is transferred from the laser-excited electrons to the lattice. Contrary to this intuitive behavior, we observe a laser-induced lattice expansion that is larger for Pt than for Fe atoms during the first picosecond after laser excitation. This effect points to the strain-wave driven lattice expansion with the longitudinal acoustic Pt motion dominating that of Fe.

36 MATERIALS SCIENCE↗

(Cd,Mg)Te crystals for picosecond-response optical-to-x-ray radiation detectors

We demonstrate a photodetector sensitive to both optical and x-ray picosecond pulses based on our in-house grown cadmium magnesium telluride (Cd,Mg)Te single crystal. Specifically, we developed In-doped Cd0.96Mg0.04Te material and discuss its femtosecond optical photoresponse, as well as the detector performance, such as <100-pA dark current and up to 0.22-mA/W responsivity for 780-nm wavelength optical radiation. The detector exposed to Ti fluorescence (K alpha) x-ray pulses at 4.5 keV, generated by a free-electron laser beam with the central energy of 9.8 keV and <100 fs pulse width, exhibited readout-electronics-limited 200-ps full-width-at-half-maximum photoresponse, demonstrating that it is suitable for coarse timing in free-electron laser x-ray/optical femtosecond pump–probe spectroscopy applications.

Instruments & Instrumentation↗

Efficient laser-driven proton acceleration from a petawatt contrast-enhanced second harmonic mixed-glass laser system

Efficient laser-driven plasma acceleration of ion beams requires precision control of the target–plasma profile, which is crucial to optimize the laser energy transfer. Along the laser propagation direction, this can be achieved by tailoring the temporal structure of the laser pulse. We show for the first time that frequency-doubling of a short pulse (hundreds-femtosecond range) petawatt-class mixed-glass laser system, which results in temporal intensity contrast enhancement, enables surface and volumetric laser–energy coupling, and the acceleration of proton beams from few-nanometer-thick foil targets. Experimentally, maximum ion energies and laser-to-proton energy conversion efficiencies were found to be both maximized at optimum laser and target conditions manifested when the normalized target density nearly equalizes the normalized laser vector potential, which is in agreement with theory and simulations. These signatures are recognized as a unique indication of the interaction between ultra-intense laser pulses with high temporal intensity contrast and ultra-thin nanometer-scale targets. Transverse modulations of accelerated proton beams in the form of bubble- and ring-like structures measured in the thinnest targets provide additional evidence of volumetric laser-driven particle acceleration regimes and transitional features in ultra-thin foil targets specific to laser–plasma interactions characterized by a high temporal intensity contrast. These results open avenues in the generation of high contrast laser pulses from short-pulse-femtosecond petawatt mixed-glass laser systems and demonstrate the feasibility of this technique for applications requiring high laser intensity contrast with high efficiency.

Physics↗

Resonant double-core excitations with ultrafast, intense X-ray pulses

Intense few-to-sub-femtosecond soft X-ray pulses can produce neutral, two-site excited double-core-hole states by promoting two core electrons to the same unoccupied molecular orbital. We theoretically investigate double nitrogen K-edge excitations of nitrous oxide (N$_2$O) with multiconfigurational electronic structure calculations. We show that the second core-excitation energy is reduced with respect to its ground state value. A site-selective double core-excitation mechanism using intense few-femtosecond x-rays is investigated using time-dependent Schrodinger equation (TDSE) simulations. The subsequent two-step Auger-Meitner and two-electrons-one-electron decay spectra of the double core-excited states are analysed using a Mulliken population analysis of the multiconfirational wavefunctions. The change in the electron emission lineshape between the absorption of 1 or 2 photons in the resonant core-excitation is predicted by combining this approach with the TDSE simulations. Furthermore, we examine the possibility of resolving the double core-excited states with X-ray pump-probe techniques by calculating the chemical shifts of the core-electron binding energy of the core-excited states and decay products.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Generation and regulation of electromagnetic pulses induced by hybrid laser pulses interacting with solid targets

In inertial confinement fusion, electromagnetic pulses (EMPs) can be produced during high-power laser interacting with solid targets, which are intimately related to laser intensity and laser energy. In this study, EMPs generated by hybrid laser pulses coupling with targets are recorded and analyzed. The results indicate that a single picosecond laser gives birth to the most intense EMPs, but they are remarkably suppressed when a nanosecond laser-shooting target is triggered before the picosecond and femtosecond laser. One possible hypothesis is proposed based on x-rays inducing pre-ablation that generates pre-plasma at the surfaces of the picosecond target and femtosecond target, leading to a sharp drop both in the energy and number of the emitting hot electrons and protons. Here, the findings will deepen our understanding of the mechanism of EMPs' generation and will also open a new avenue to regulate EMPs by hybrid laser pulses.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

High-resolution analogue of time-domain phonon spectroscopy in the transmission electron microscope

Femtosecond photoexcitation of semiconducting materials leads to the generation of coherent acoustic phonons (CAPs), the behaviours of which are linked to intrinsic and engineered electronic, optical and structural properties. While often studied with pump-probe spectroscopic techniques, the influence of nanoscale structure and morphology on CAP dynamics can be challenging to resolve with these all-optical methods. Here, we used ultrafast electron microscopy (UEM) to resolve variations in CAP dynamics caused by differences in the degree of crystallinity in as-prepared and annealed GaAs lamellae. Following in situ femtosecond photoexcitation, we directly imaged the generation and propagation dynamics of hypersonic CAPs in a mostly amorphous and, following an in situ photothermal anneal, a mostly crystalline lamella. Subtle differences in both the initial hypersonic velocities and the asymptotic relaxation behaviours were resolved via construction of space-time contour plots from phonon wavefronts. Comparison to bulk sound velocities in crystalline and amorphous GaAs reveals the influence of the mixed amorphous-crystalline morphology on CAP dispersion behaviours. Further, an increase in the asymptotic velocity following annealing establishes the sensitivity of quantitative UEM imaging to both structural and compositional variations through differences in bonding and elasticity. Lastly, implications of extending the methods and results reported here to elucidating correlated electronic, optical and structural behaviours in semiconducting materials are discussed.

42 ENGINEERING↗