Multi-resolution electron spectrometer array for future free-electron laser experiments.

The design of an angular array of electron time-of-flight (eToF) spectrometers is reported, intended for non-invasive spectral, temporal, and polarization characterization of single shots of high-repetition rate, quasi-continuous, short-wavelength free-electron lasers (FELs) such as the LCLS II at SLAC. This array also enables angle-resolved, high-resolution eToF spectroscopy to address a variety of scientific questions on ultrafast and nonlinear light-matter interactions at FELs. The presented device is specifically designed for the time-resolved atomic, molecular and optical science endstation (TMO) at LCLS II. In its final version, the spectrometer comprises up to 20 eToF spectrometers aligned to collect electrons from the interaction point, which is defined by the intersection of the incoming FEL radiation and a gaseous target. The full composition involves 16 spectrometers forming a circular equiangular array in the plane normal to the X-ray propagation and four spectrometers at 54.7° angle relative to the principle linear X-ray polarization axis with orientations in the forward and backward direction of the light propagation. The spectrometers are capable of independent and minimally chromatic electrostatic lensing and retardation, in order to enable simultaneous angle-resolved photo- and Auger-Meitner electron spectroscopy with high energy resolution. They are designed to ensure an energy resolution of 0.25 eV across an energy window of up to 75 eV, which can be individually centered via the adjustable retardation to cover the full range of electron kinetic energies relevant to soft X-ray methods, 0-2 keV. The full spectrometer array will enable non-invasive and online spectral-polarimetry measurements, polarization-sensitive attoclock spectroscopy for characterizing the full time-energy structure of SASE or seeded LCLS II pulses, and support emerging trends in molecular-frame spectroscopy measurements.

Laser-induced inner-shell excitations through direct electron re-collision versus indirect collision.

The dynamics and the decay processes of inner-shell excited atoms are of great interest in physics, chemistry, biology, and technology. The highly excited state decays very quickly through different channels, both radiative and non-radiative. It is therefore a long-standing goal to study such dynamics directly in the time domain. Using few-cycle infrared laser pulses, we investigated the excitation and ionization of inner-shell electrons through laser-induced electron re-collision with the original parent ions and measured the dependence of the emitted x-ray spectra on the intensity and ellipticity of the driving laser. These directly re-colliding electrons can be used as the initiating pump step in pump/probe experiments for studying core-hole dynamics at their natural temporal scale. In our experiment we found that the dependence of the x-ray emission spectrum on the laser intensity and polarization state varies distinctly for the two kinds of atomic systems. Relying on our data and numerical simulations, we explain this behavior by the presence of different excitation mechanisms that are contributing in different ratios to the respective overall x-ray emission yields. Direct re-collision excitation competes with indirect collisions with neighboring atoms by electrons having "drifted away" from the original parent ion.

Attosecond transient absorption spooktroscopy: a ghost imaging approach to ultrafast absorption spectroscopy.

The recent demonstration of isolated attosecond pulses from an X-ray free-electron laser (XFEL) opens the possibility for probing ultrafast electron dynamics at X-ray wavelengths. An established experimental method for probing ultrafast dynamics is X-ray transient absorption spectroscopy, where the X-ray absorption spectrum is measured by scanning the central photon energy and recording the resultant photoproducts. The spectral bandwidth inherent to attosecond pulses is wide compared to the resonant features typically probed, which generally precludes the application of this technique in the attosecond regime. In this paper we propose and demonstrate a new technique to conduct transient absorption spectroscopy with broad bandwidth attosecond pulses with the aid of ghost imaging, recovering sub-bandwidth resolution in photoproduct-based absorption measurements.

Development of ultrafast capabilities for X-ray free-electron lasers at the linac coherent light source.

The ability to produce ultrashort, high-brightness X-ray pulses is revolutionizing the field of ultrafast X-ray spectroscopy. Free-electron laser (FEL) facilities are driving this revolution, but unique aspects of the FEL process make the required characterization and use of the pulses challenging. In this paper, we describe a number of developments in the generation of ultrashort X-ray FEL pulses, and the concomitant progress in the experimental capabilities necessary for their characterization and use at the Linac Coherent Light Source. This includes the development of sub-femtosecond hard and soft X-ray pulses, along with ultrafast characterization techniques for these pulses. We also describe improved techniques for optical cross-correlation as needed to address the persistent challenge of external optical laser synchronization with these ultrashort X-ray pulses. This article is part of the theme issue 'Measurement of ultrafast electronic and structural dynamics with X-rays'.

Subfemtosecond K-shell excitation with a few-cycle infrared laser field.

Subfemtosecond bursts of extreme ultraviolet radiation, facilitated by a process known as high-order harmonic generation, are a key ingredient for attosecond metrology, providing a tool to precisely initiate and probe ultrafast dynamics in the microcosms of atoms, molecules, and solids. These ultrashort pulses are always, and as a by-product of the way they are generated, accompanied by laser-induced recollisions of electrons with their parent ions. By using a few-cycle infrared (λ(0)=2.1 µm) driving laser, we were able to directly excite high-energy (∼870 eV) inner-shell electrons through laser-induced electron recollision, opening the door to time-resolved studies of core-level and concomitant multielectron dynamics.

Steady-state solutions of split beams in electron storage rings.

Recently, a novel operation method for synchrotron light sources with transversely split beams has been explored to fulfill the rising demand for flexible and high-throughput X-ray sources required in such diverse fields as time-resolved X-ray spectroscopy, molecular chemistry in organic cells, high-resolution medical imaging, quantum materials science or sustainable energy research. Within that novel operation mode, additional stable regions are produced in the horizontal phase space by operating an electron storage ring on a resonance that is driven by the nonlinear sextupole or octupole magnets. In the longitudinal phase space, a similar split can be produced by introducing an oscillation of the synchrotron phase via a modulation of the phase of the radiofrequency resonator. Strong radiation damping in electron storage rings, however, has to be overcome before additional regions in phase space can become populated by particles and form stable islands. This damping mechanism changes the dynamics of the system and causes diffusion between the different islands in phase space, raising the question what kind of equilibrium state exists in the asymptotic temporal limit. In this paper, a finite-differences approximation in rotating action-angle coordinates is used to solve the Vlasov-Fokker-Planck equation and to study the obtained equilibrium states for the longitudinal as well as the transverse case. The number of solution vectors and the magnitude of the corresponding singular values of the matrix of the underlying finite-differences equation are used as abstract indicators to define the required parameter set that provides stable additional beamlets. As a consequence, the beamlets have a stability that is close to that of the main beam in terms of diffusion caused by the radiation damping and quantum excitation.

Artificial intelligence for online characterization of ultrashort X-ray free-electron laser pulses.

X-ray free-electron lasers (XFELs) as the world's brightest light sources provide ultrashort X-ray pulses with a duration typically in the order of femtoseconds. Recently, they have approached and entered the attosecond regime, which holds new promises for single-molecule imaging and studying nonlinear and ultrafast phenomena such as localized electron dynamics. The technological evolution of XFELs toward well-controllable light sources for precise metrology of ultrafast processes has been, however, hampered by the diagnostic capabilities for characterizing X-ray pulses at the attosecond frontier. In this regard, the spectroscopic technique of photoelectron angular streaking has successfully proven how to non-destructively retrieve the exact time-energy structure of XFEL pulses on a single-shot basis. By using artificial intelligence techniques, in particular convolutional neural networks, we here show how this technique can be leveraged from its proof-of-principle stage toward routine diagnostics even at high-repetition-rate XFELs, thus enhancing and refining their scientific accessibility in all related disciplines.

Attosecond coherent electron motion in Auger-Meitner decay.

In quantum systems, coherent superpositions of electronic states evolve on ultrafast time scales (few femtoseconds to attoseconds; 1 attosecond = 0.001 femtoseconds = 10-18 seconds), leading to a time-dependent charge density. Here we performed time-resolved measurements using attosecond soft x-ray pulses produced by a free-electron laser, to track the evolution of a coherent core-hole excitation in nitric oxide. Using an additional circularly polarized infrared laser pulse, we created a clock to time-resolve the electron dynamics and demonstrated control of the coherent electron motion by tuning the photon energy of the x-ray pulse. Core-excited states offer a fundamental test bed for studying coherent electron dynamics in highly excited and strongly correlated matter.

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 [Formula: see text]J. 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.

Site-specific interrogation of an ionic chiral fragment during photolysis using an X-ray free-electron laser.

Short-wavelength free-electron lasers with their ultrashort pulses at high intensities have originated new approaches for tracking molecular dynamics from the vista of specific sites. X-ray pump X-ray probe schemes even allow to address individual atomic constituents with a 'trigger'-event that preludes the subsequent molecular dynamics while being able to selectively probe the evolving structure with a time-delayed second X-ray pulse. Here, we use a linearly polarized X-ray photon to trigger the photolysis of a prototypical chiral molecule, namely trifluoromethyloxirane (C3H3F3O), at the fluorine K-edge at around 700 eV. The created fluorine-containing fragments are then probed by a second, circularly polarized X-ray pulse of higher photon energy in order to investigate the chemically shifted inner-shell electrons of the ionic mother-fragment for their stereochemical sensitivity. We experimentally demonstrate and theoretically support how two-color X-ray pump X-ray probe experiments with polarization control enable XFELs as tools for chiral recognition.

TIMI 3 flow after primary angioplasty is an important predictor for outcome in patients with acute myocardial infarction.

BACKGROUND: Growing evidence suggests that poor coronary blood flow after primary percutaneous coronary intervention (PCI) is associated with unfavorable clinical out-come. We retrospectively evaluated data from our single center "real world patients" database of patients undergoing primary PCI to determine differences in clinical and angiographic patterns in patients with or without restoring thrombolysis in myocardial infarction (TIMI) flow 3. METHODS AND RESULTS: Between 2001 and 2006, 500 patients underwent primary PCI for STEMI. In 430 patients, post-interventional TIMI flow 3 could be established. In this group, in-hospital mortality was significant lower (6.4% Vs. 32.9%; P < 0.0001), left ventricular ejection fraction was better (51.3 Vs. 44.2%; P < 0.0001), and prehospital fibrinolytic therapy (6.3% Vs. 14.3%; P = 0.015), cardiogenic shock (10.9% Vs. 24.3%; P = 0.002) and use of intra-aortic balloon pump were all more unlikely (5.8% Vs. 11.4%; P = 0.045) compared to patients with TIMI flow < or = 2. In patients with post-interventional TIMI flow < or = 2 the left anterior descending coronary artery (LAD) was significantly more often seen as the target vessel (54.3% Vs. 44.6%; P = 0.039). A regressions analysis showed that predictors leading to such flow patterns are diabetes (P = 0.013), pre-hospital fibrinolytic therapy (P = 0.017), cardiogenic shock (P = 0.002) and a 3-vessel disease (P = 0.003). After 6 months, patients without restored normal TIMI flow had worse New York Heart Association functional class (NYHA), and had to undergo repeat coronary angiography more often. CONCLUSION: Post-interventional TIMI flow < or = 2 is strongly associated with adverse out-come during hospitalization and after 6 months following hospitalization.