Volt-per-Ångstrom terahertz fields from X-ray free-electron lasers

The electron linear accelerators driving modern X-ray free-electron lasers can emit intense, tunable, quasi-monochromatic terahertz (THz) transients with peak electric fields of V Å ⁻¹ and peak magnetic fields in excess of 10 T when a purpose-built, compact, superconducting THz undulator is implemented. New research avenues such as X-ray movies of THz-driven mode-selective chemistry come into reach by making dual use of the ultra-short GeV electron bunches, possible by a rather minor extension of the infrastructure

Coherent Phonons in Carbon Nanotubes and Graphene

We review recent studies of coherent phonons (CPs) corresponding to the radial breathing mode (RBM) and G-mode in single-wall carbon nanotubes (SWCNTs) and graphene. Because of the bandgap-diameter relationship, RBM-CPs cause bandgap oscillations in SWCNTs, modulating interband transitions at terahertz frequencies. Interband resonances enhance CP signals, allowing for chirality determination. Using pulse shaping, one can selectively excite speci!c-chirality SWCNTs within an ensemble. G-mode CPs exhibit temperature-dependent dephasing via interaction with RBM phonons. Our microscopic theory derives a driven oscillator equation with a density-dependent driving term, which correctly predicts CP trends within and between (2n+m) families. We also find that the diameter can initially increase or decrease. Finally, we theoretically study the radial breathing like mode in graphene nanoribbons. For excitation near the absorption edge, the driving term is much larger for zigzag nanoribbons. We also explain how the armchair nanoribbon width changes in response to laser excitation.Comment: 48 pages, 41 figure

Extreme Ultraviolet Wave Packet Interferometry of the Autoionizing HeNe Dimer

Femtosecond extreme ultraviolet wave packet interferometry (XUV-WPI) was applied to study resonant interatomic Coulombic decay (ICD) in the HeNe dimer. The high demands on phase stability and sensitivity for vibronic XUV-WPI of molecular-beam targets are met using an XUV phase-cycling scheme. The detected quantum interferences exhibit vibronic dephasing and rephasing signatures along with an ultrafast decoherence assigned to the ICD process. A Fourier analysis reveals the molecular absorption spectrum with high resolution. The demonstrated experiment shows a promising route for the real-time analysis of ultrafast ICD processes with both high temporal and high spectral resolution

Auger electron wave packet interferometry on extreme timescales with coherent soft x rays

Wave packet interferometry provides benchmark information on light-induced electronic quantum states by monitoring their relative amplitudes and phases during coherent excitation, propagation,and decay. The relative phase control of soft x-ray pulse replicas on the single-digit attosecond timescale achieved in our experiments makes this method a powerful tool to probe ultrafast quantum phenomena such as the excitation of Auger shake-up states with sub-cycle precision. In this contribution we present first results obtained for different Auger decay channels upon generating L-shell vacancies in argon atoms using Michelson-type all-reflective interferometric autocorrelation at a central free-electron laser photon energy of 274.7 eV

Charge induced chemical dynamics in glycine probed with time resolved Auger electron spectroscopy

In the present contribution, we use x rays to monitor charge induced chemical dynamics in the photoionized amino acid glycine with femtosecond time resolution. The outgoing photoelectron leaves behind the cation in a coherent superposition of quantum mechanical eigenstates. Delayed x ray pulses track the induced coherence through resonant x ray absorption that induces Auger decay. Temporal modulation of the Auger electron signal correlated with specific ions is observed, which is governed by the initial electronic coherence and subsequent vibronic coupling to nuclear degrees of freedom. In the time resolved x ray absorption measurement, we monitor the time frequency spectra of the resulting many body quantum wave packets for a period of 175 fs along different reaction coordinates. Our experiment proves that by measuring specific fragments associated with the glycine dication as a function of the pump probe delay, one can selectively probe electronic coherences at early times associated with a few distinguishable components of the broad electronic wave packet created initially by the pump pulse in the cation. The corresponding coherent superpositions formed by subsets of electronic eigenstates and evolving along parallel dynamical pathways show different phases and time periods in the range of amp; 8722;0.3 0.1 amp; 120587; amp; 8804; amp; 120601; amp; 8804; 0.1 0.2 amp; 120587; and 18.2 1.7 amp; 8722;1.4 amp; 8804; amp; 119879; amp; 8804;23.9 1.2 amp; 8722;1.1 fs. Furthermore, for long delays, the data allow us to pinpoint the driving vibrational modes of chemical dynamics mediating charge induced bond cleavage along different reaction coordinate

Electron population dynamics in resonant non-linear x-ray absorption in nickel at a free-electron laser

Free-electron lasers provide bright, ultrashort, and monochromatic x-ray pulses, enabling novel spectroscopic measurements not only with femtosecond temporal resolution: The high fluence of their x-ray pulses can also easily enter the regime of the non-linear x-ray–matter interaction. Entering this regime necessitates a rigorous analysis and reliable prediction of the relevant non-linear processes for future experiment designs. Here, we show non-linear changes in the L3-edge absorption of metallic nickel thin films, measured with fluences up to 60 J/cm2. We present a simple but predictive rate model that quantitatively describes spectral changes based on the evolution of electronic populations within the pulse duration. Despite its simplicity, the model reaches good agreement with experimental results over more than three orders of magnitude in fluence, while providing a straightforward understanding of the interplay of physical processes driving the non-linear changes. Our findings provide important insights for the design and evaluation of future high-fluence free-electron laser experiments and contribute to the understanding of non-linear electron dynamics in x-ray absorption processes in solids at the femtosecond timescale

Photon shot-noise limited transient absorption soft X-ray spectroscopy at the European XFEL

Femtosecond transient soft X-ray Absorption Spectroscopy (XAS) is a very promising technique that can be employed at X-ray Free Electron Lasers (FELs) to investigate out-of-equilibrium dynamics for material and energy research. Here we present a dedicated setup for soft X-rays available at the Spectroscopy & Coherent Scattering (SCS) instrument at the European X-ray Free Electron Laser (EuXFEL). It consists of a beam-splitting off-axis zone plate (BOZ) used in transmission to create three copies of the incoming beam, which are used to measure the transmitted intensity through the excited and unexcited sample, as well as to monitor the incoming intensity. Since these three intensity signals are detected shot-by-shot and simultaneously, this setup allows normalized shot-by-shot analysis of the transmission. For photon detection, the DSSC imaging detector, which is capable of recording up to 800 images at 4.5 MHz frame rate during the FEL burst, is employed and allows approaching the photon shot-noise limit. We review the setup and its capabilities, as well as the online and offline analysis tools provided to users

Electronic quantum coherence in glycine molecules probed with ultrashort x ray pulses in real time

Here, we use x rays to create and probe quantum coherence in the photoionized amino acid glycine. The outgoing photoelectron leaves behind the cation in a coherent superposition of quantum mechanical eigenstates. Delayed x ray pulses track the induced coherence through resonant x ray absorption that induces Auger decay and by photoelectron emission from sequential double photoionization. Sinusoidal temporal modulation of the detected signal at early times 0 to 25 fs is observed in both measurements. Advanced ab initio many electron simulations allow us to explain the first 25 fs of the detected coherent quantum evolution in terms of the electronic coherence. In the kinematically complete x ray absorption measurement, we monitor its dynamics for a period of 175 fs and observe an evolving modulation that may implicate the coupling of electronic to vibronic coherence at longer time scales. Our experiment provides a direct support for the existence of long lived electronic coherence in photoionized biomolecule

Thomson Scattering at FLASH - Status Report

The basic idea is to implement Thomson scattering with free electron laser (FEL) radiation at near-solid density plasmas as a diagnostic method which allows the determination of plasma temperatures and densities in the warm dense matter (WDM) regime (free electron density of n{sub e} = 10{sup 21}-10{sup 26} cm{sup -3} with temperatures of several eV). The WDM regime [1] at near-solid density (n{sub e} = 10{sup 21}-10{sup 22} cm{sup -3}) is of special interest because, it is where the transition from an ideal plasma to a degenerate, strongly coupled plasma occurs. A systematic understanding of this largely unknown WDM domain is crucial for the modeling and understanding of contemporary plasma experiments, like laser shock-wave or Z-pinch experiments as well as for inertial confinement fusion (ICF) experiments as the plasma evolution follows its path through this domain

The Heisenberg-RIXS instrument at the European XFEL

Resonant Inelastic X-ray Scattering (RIXS) is an ideal X-ray spectroscopy method to push the combination of energy and time resolutions to the Fourier transform ultimate limit, because it is unaffected by the core-hole lifetime energy broadening. And in pump-probe experiments the interaction time is made very short by the same core-hole lifetime. RIXS is very photon hungry so it takes great advantage from high repetition rate pulsed X-ray sources like the European XFEL. The hRIXS instrument is designed for RIXS experiments in the soft X-ray range with energy resolution approaching the Fourier and the Heisenberg limits. It is based on a spherical grating with variable line spacing (VLS) and a position-sensitive 2D detector. Initially, two gratings are installed to adequately cover the whole photon energy range. With optimized spot size on the sample and small pixel detector the energy resolution can be better than 40 meV at any photon energy below 1000 eV. At the SCS instrument of the European XFEL the spectrometer can be easily positioned thanks to air-pads on a high-quality floor, allowing the scattering angle to be continuously adjusted over the 65-145 deg range. It can be coupled to two different sample interaction chamber, one for liquid jets and one for solids, each equipped at the state-of-the-art and compatible for optical laser pumping in collinear geometry. The measured performances, in terms of energy resolution and count rate on the detector, closely match design expectations. hRIXS is open to public users since the summer of 2022.Comment: 43 pages, 12 figures, Supplemental Materia