Strain wave pathway to semiconductor-to-metal transition revealed by time-resolved X-ray powder diffraction.

One of the main challenges in ultrafast material science is to trigger phase transitions with short pulses of light. Here we show how strain waves, launched by electronic and structural precursor phenomena, determine a coherent macroscopic transformation pathway for the semiconducting-to-metal transition in bistable Ti3O5 nanocrystals. Employing femtosecond powder X-ray diffraction, we measure the lattice deformation in the phase transition as a function of time. We monitor the early intra-cell distortion around the light absorbing metal dimer and the long range deformations governed by acoustic waves propagating from the laser-exposed Ti3O5 surface. We developed a simplified elastic model demonstrating that picosecond switching in nanocrystals happens concomitantly with the propagating acoustic wavefront, several decades faster than thermal processes governed by heat diffusion.

Inception of electronic damage of matter by photon-driven post-ionization mechanisms.

"Probe-before-destroy" methodology permitted diffraction and imaging measurements of intact specimens using ultrabright but highly destructive X-ray free-electron laser (XFEL) pulses. The methodology takes advantage of XFEL pulses ultrashort duration to outrun the destructive nature of the X-rays. Atomic movement, generally on the order of >50 fs, regulates the maximum pulse duration for intact specimen measurements. In this contribution, we report the electronic structure damage of a molecule with ultrashort X-ray pulses under preservation of the atoms' positions. A detailed investigation of the X-ray induced processes revealed that X-ray absorption events in the solvent produce a significant number of solvated electrons within attosecond and femtosecond timescales that are capable of coulombic interactions with the probed molecules. The presented findings show a strong influence on the experimental spectra coming from ionization of the probed atoms' surroundings leading to electronic structure modification much faster than direct absorption of photons. This work calls for consideration of this phenomenon in cases focused on samples embedded in, e.g., solutions or in matrices, which in fact concerns most of the experimental studies.

Femtosecond phase-transition in hard x-ray excited bismuth.

The evolution of bismuth crystal structure upon excitation of its A1g phonon has been intensely studied with short pulse optical lasers. Here we present the first-time observation of a hard x-ray induced ultrafast phase transition in a bismuth single crystal at high intensities (~1014 W/cm2). The lattice evolution was followed using a recently demonstrated x-ray single-shot probing setup. The time evolution of the (111) Bragg peak intensity showed strong dependence on the excitation fluence. After exposure to a sufficiently intense x-ray pulse, the peak intensity dropped to zero within 300 fs, i.e. faster than one oscillation period of the A1g mode at room temperature. Our analysis indicates a nonthermal origin of a lattice disordering process, and excludes interpretations based on electron-ion equilibration process, or on thermodynamic heating process leading to plasma formation.

Spatial displacement of forward-diffracted X-ray beams by perfect crystals.

Time-delayed, narrow-band echoes generated by forward Bragg diffraction of an X-ray pulse by a perfect thin crystal are exploited for self-seeding at hard X-ray free-electron lasers. Theoretical predictions indicate that the retardation is strictly correlated to a transverse displacement of the echo pulses. This article reports the first experimental observation of the displaced echoes. The displacements are in good agreement with simulations relying on the dynamical diffraction theory. The echo signals are characteristic for a given Bragg reflection, the structure factor and the probed interplane distance. The reported results pave the way to exploiting the signals as an online diagnostic tool for hard X-ray free-electron laser seeding and for dynamical diffraction investigations of strain at the femtosecond timescale.

Simulation of FEL pulse length calculation with THz streaking method.

Having accurate and comprehensive photon diagnostics for the X-ray pulses delivered by free-electron laser (FEL) facilities is of utmost importance. Along with various parameters of the photon beam (such as photon energy, beam intensity, etc.), the pulse length measurements are particularly useful both for the machine operators to measure the beam parameters and monitor the stability of the machine performance, and for the users carrying out pump-probe experiments at such facilities to better understand their measurement results. One of the most promising pulse length measurement techniques used for photon diagnostics is the THz streak camera which is capable of simultaneously measuring the lengths of the photon pulses and their arrival times with respect to the pump laser. This work presents simulations of a THz streak camera performance. The simulation procedure utilizes FEL pulses with two different photon energies in hard and soft X-ray regions, respectively. It recreates the energy spectra of the photoelectrons produced by the photon pulses and streaks them by a single-cycle THz pulse. Following the pulse-retrieval procedure of the THz streak camera, the lengths were calculated from the streaked spectra. To validate the pulse length calculation procedure, the precision and the accuracy of the method were estimated for streaking configuration corresponding to previously performed experiments. The obtained results show that for the discussed setup the method is capable of measuring FEL pulses with about a femtosecond accuracy and precision.

Absolute pulse energy measurements of soft x-rays at the Linac Coherent Light Source.

This paper reports novel measurements of x-ray optical radiation on an absolute scale from the intense and ultra-short radiation generated in the soft x-ray regime of a free electron laser. We give a brief description of the detection principle for radiation measurements which was specifically adapted for this photon energy range. We present data characterizing the soft x-ray instrument at the Linac Coherent Light Source (LCLS) with respect to the radiant power output and transmission by using an absolute detector temporarily placed at the downstream end of the instrument. This provides an estimation of the reflectivity of all x-ray optical elements in the beamline and provides the absolute photon number per bandwidth per pulse. This parameter is important for many experiments that need to understand the trade-offs between high energy resolution and high flux, such as experiments focused on studying materials via resonant processes. Furthermore, the results are compared with the LCLS diagnostic gas detectors to test the limits of linearity, and observations are reported on radiation contamination from spontaneous undulator radiation and higher harmonic content.

High-precision x-ray FEL pulse arrival time measurements at SACLA by a THz streak camera with Xe clusters.

The accurate measurement of the arrival time of a hard X-ray free electron laser (FEL) pulse with respect to a laser is of utmost importance for pump-probe experiments proposed or carried out at FEL facilities around the world. This manuscript presents the latest device to meet this challenge, a THz streak camera using Xe gas clusters, capable of pulse arrival time measurements with an estimated accuracy of several femtoseconds. An experiment performed at SACLA demonstrates the performance of the device at photon energies between 5 and 10 keV with variable photon beam parameters.

Photoemission of cooper pairs from aromatic hydrocarbons.

We report the discovery of the formation of an electron Cooper pair approximately 40 eV above the double-ionization threshold in benzene, naphthalene, anthracene, and coronene after absorption of a single photon. We have measured the ratios of doubly to singly charged parent ions of the above mentioned molecules as well as pyrrole and furan by using monochromatized synchrotron radiation up to 100 eV above the corresponding thresholds. We also recorded photoelectron spectra of benzene and naphthalene at selected energies. The electron-pair formation is based on the specific structure of the molecules and does not exist for pyrrole and furan.

Large molecules reveal a linear length scaling for double photoionization.

We have measured the ratio of doubly to singly charged parent ions of benzene, naphthalene, anthracene, and pentacene using monochromatized synchrotron radiation up to 30 eV above the corresponding threshold. Our measurements show a striking similarity between the ratio of doubly charged to all parent ions and the ratio for helium. Moreover, the magnitudes of the ratios for these molecules scale linearly with their lengths with an amazing accuracy. A high ratio, i.e., a high relative double-photoionization probability, makes a molecule an important source of low-energy electrons that can promote radiation damage of biomolecules [B. Boudaïffa et al., Science 287, 1658 (2000)].

Two-photon inner-shell ionization in the extreme ultraviolet.

We have observed the simultaneous inner-shell absorption of two extreme-ultraviolet photons by a Xe atom in an experiment performed at the short-wavelength free electron laser facility FLASH. Photoelectron spectroscopy permitted us to unambiguously identify a feature resulting from the ionization of a single electron of the 4d subshell of Xe by two photons each of energy (93±1) eV. The feature's intensity has a quadratic dependence on the pulse energy. The results are discussed and interpreted within the framework of recent results of ion spectroscopy experiments of Xe obtained at ultrahigh irradiance in the extreme-ultraviolet regime.

Extreme ultraviolet laser excites atomic giant resonance.

Exceptional behavior of light-matter interaction in the extreme ultraviolet is demonstrated. The photoionization of different rare gases was compared at the free-electron laser in Hamburg, FLASH, by applying ion spectroscopy at the wavelength of 13.7 nm and irradiance levels of thousands of terawatts per square centimeter. In the case of xenon, the degree of nonlinear photoionization was found to be significantly higher than for neon, argon, and krypton. This target specific behavior cannot be explained by the standard theories developed for optical strong-field phenomena. We suspect that the collective giant 4d resonance of xenon is the driving force behind the effect that arises in this spectral range.

Spatio-temporal coherence of free electron laser pulses in the soft x-ray regime.

The temporal coherence properties of soft x-ray free electron laser pulses at FLASH are measured at 23.9 nm by interfering two time-delayed partial beams directly on a CCD camera. The partial beams are obtained by wave front beam splitting in an autocorrelator operating at photon energies from h nu = 30 to 200 eV. At zero delay a visibility of (0.63+/- 0.04) is measured. The delay of one partial beam reveals a coherence time of 6 fs at 23.9 nm. The visibility further displays a non-monotonic decay, which can be rationalized by the presence of multiple pulse structure.

Experimental evidence for modulations in the relative double-photoionization cross section of C60 from threshold up to 280 eV.

The relative double-photoionization cross section of neutral C60 clusters was investigated using monochromatized synchrotron radiation between 18 and 283 eV. Our measurement of the double-to-single photoionization ratio reveals two modulating components that are superimposed on a smooth ratio curve from threshold (19.0 eV) up to 280 eV, when inner-shell excitations become possible. The maxima in the modulation can be related to geometrical dimensions of the C60 cluster.