Table-top interferometry on extreme time and wavelength scales.

Short-pulse metrology and dynamic studies in the extreme ultraviolet (XUV) spectral range greatly benefit from interferometric measurements. In this contribution a Michelson-type all-reflective split-and-delay autocorrelator operating in a quasi amplitude splitting mode is presented. The autocorrelator works under a grazing incidence angle in a broad spectral range (10 nm - 1 µm) providing collinear propagation of both pulse replicas and thus a constant phase difference across the beam profile. The compact instrument allows for XUV pulse autocorrelation measurements in the time domain with a single-digit attosecond precision and a useful scan length of about 1 ps enabling a decent resolution of E/ΔE = 2000 at 26.6 eV. Its performance for selected spectroscopic applications requiring moderate resolution at short wavelengths is demonstrated by characterizing a sharp electronic transition at 26.6 eV in Ar gas. The absorption of the 11th harmonic of a frequency-doubled Yb-fiber laser leads to the well-known 3s3p64p1P1 Fano resonance of Ar atoms. We benchmark our time-domain interferometry results with a high-resolution XUV grating spectrometer and find an excellent agreement. The common-path interferometer opens up new opportunities for short-wavelength femtosecond and attosecond pulse metrology and dynamic studies on extreme time scales in various research fields.

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.

Shaping femtosecond laser pulses at short wavelength with grazing-incidence optics.

We present the design of an extreme ultraviolet (XUV) pulse shaper relying on reflective optics. The instrument will allow tailoring of the time-frequency spectrum of femtosecond pulses generated by seeded free-electron lasers (FEL) and high-harmonic generation (HHG) sources down to a central wavelength of ~15 nm. The device is based on the geometry of a 4f grating compressor that is a standard concept in ultrafast laser science and technology. We apply it to shorter wavelengths using grazing-incidence optics operated under ultra-high vacuum conditions. The design blaze angle and the line density of the gratings allow the manipulation of all different harmonics typical for seeded FEL and HHG photon sources without the need of realignment of the instrument and even simultaneously in multi-color experiments. A proof-of-principle pulse shaping experiment using 266 nm laser light has been performed, demonstrating relative phase-control of femtosecond UV pulses.

A sensitive EUV Schwarzschild microscope for plasma studies with sub-micrometer resolution.

We present an extreme ultraviolet (EUV) microscope using a Schwarzschild objective which is optimized for single-shot sub-micrometer imaging of laser-plasma targets. The microscope has been designed and constructed for imaging the scattering from an EUV-heated solid-density hydrogen jet. Imaging of a cryogenic hydrogen target was demonstrated using single pulses of the free-electron laser in Hamburg (FLASH) free-electron laser at a wavelength of 13.5 nm. In a single exposure, we observe a hydrogen jet with ice fragments with a spatial resolution in the sub-micrometer range. In situ EUV imaging is expected to enable novel experimental capabilities for warm dense matter studies of micrometer-sized samples in laser-plasma experiments.

Equilibration dynamics and conductivity of warm dense hydrogen.

We investigate subpicosecond dynamics of warm dense hydrogen at the XUV free-electron laser facility (FLASH) at DESY (Hamburg). Ultrafast impulsive electron heating is initiated by a ≤ 300-fs short x-ray burst of 92-eV photon energy. A second pulse probes the sample via x-ray scattering at jitter-free variable time delay. We show that the initial molecular structure dissociates within (0.9 ± 0.2) ps, allowing us to infer the energy transfer rate between electrons and ions. We evaluate Saha and Thomas-Fermi ionization models in radiation hydrodynamics simulations, predicting plasma parameters that are subsequently used to calculate the static structure factor. A conductivity model for partially ionized plasma is validated by two-temperature density-functional theory coupled to molecular dynamic simulations and agrees with the experimental data. Our results provide important insights and the needed experimental data on transport properties of dense plasmas.

Hidden charge states in soft-x-ray laser-produced nanoplasmas revealed by fluorescence spectroscopy.

Highly charged ions are formed in the center of composite clusters by strong free-electron laser pulses and they emit fluorescence on a femtosecond time scale before competing recombination leads to neutralization of the nanoplasma core. In contrast to mass spectrometry that detects remnants of the interaction, fluorescence in the extreme ultraviolet spectral range provides fingerprints of transient states of high energy density matter. Spectra from clusters consisting of a xenon core and a surrounding argon shell show that a small fraction of the fluorescence signal comes from multiply charged xenon ions in the cluster core. Initially, these ions are as highly charged as the ions in the outer shells of pure xenon clusters with charge states up to at least 11+.

Resolving ultrafast heating of dense cryogenic hydrogen.

We report on the dynamics of ultrafast heating in cryogenic hydrogen initiated by a ≲300 fs, 92 eV free electron laser x-ray burst. The rise of the x-ray scattering amplitude from a second x-ray pulse probes the transition from dense cryogenic molecular hydrogen to a nearly uncorrelated plasmalike structure, indicating an electron-ion equilibration time of ∼0.9 ps. The rise time agrees with radiation hydrodynamics simulations based on a conductivity model for partially ionized plasma that is validated by two-temperature density-functional theory.

Generation of coherent 19- and 38-nm radiation at a free-electron laser directly seeded at 38 nm.

Initiating the gain process in a free-electron laser (FEL) from an external highly coherent source of radiation is a promising way to improve the pulse properties such as temporal coherence and synchronization performance in time-resolved pump-probe experiments at FEL facilities, but this so-called "seeding" suffers from the lack of adequate sources at short wavelengths. We report on the first successful seeding at a wavelength as short as 38.2 nm, resulting in GW-level, coherent FEL radiation pulses at this wavelength as well as significant second harmonic emission at 19.1 nm. The external seed pulses are about 1 order of magnitude shorter compared to previous experiments allowing an ultimate time resolution for the investigation of dynamic processes enabling breakthroughs in ultrafast science with FELs. The seeding pulse is the 21st harmonic of an 800-nm, 15-fs (rms) laser pulse generated in an argon medium. Methods for finding the overlap of seed pulses with electron bunches in spatial, longitudinal, and spectral dimensions are discussed and results are presented. The experiment was conducted at FLASH, the FEL user facility at DESY in Hamburg, Germany.

Ultrafast x-ray scattering of xenon nanoparticles: imaging transient states of matter.

Femtosecond x-ray laser flashes with power densities of up to 10(14) W/cm(2) at 13.7 nm wavelength were scattered by single xenon clusters in the gas phase. Similar to light scattering from atmospheric microparticles, the x-ray diffraction patterns carry information about the optical constants of the objects. However, the high flux of the x-ray laser induces severe transient changes of the electronic configuration, resulting in a tenfold increase of absorption in the developing nanoplasma. The modification in opaqueness can be correlated to strong atomic charging of the particle leading to excitation of Xe(4+). It is shown that single-shot single-particle scattering on femtosecond time scales yields insight into ultrafast processes in highly excited systems where conventional spectroscopy techniques are inherently blind.

Electronic structure of an XUV photogenerated solid-density aluminum plasma.

By use of high intensity XUV radiation from the FLASH free-electron laser at DESY, we have created highly excited exotic states of matter in solid-density aluminum samples. The XUV intensity is sufficiently high to excite an inner-shell electron from a large fraction of the atoms in the focal region. We show that soft-x-ray emission spectroscopy measurements reveal the electronic temperature and density of this highly excited system immediately after the excitation pulse, with detailed calculations of the electronic structure, based on finite-temperature density functional theory, in good agreement with the experimental results.

Observation of ultrafast nonequilibrium collective dynamics in warm dense hydrogen.

We investigate ultrafast (fs) electron dynamics in a liquid hydrogen sample, isochorically and volumetrically heated to a moderately coupled plasma state. Thomson scattering measurements using 91.8 eV photons from the free-electron laser in Hamburg (FLASH at DESY) show that the hydrogen plasma has been driven to a nonthermal state with an electron temperature of 13 eV and an ion temperature below 0.1 eV, while the free-electron density is 2.8x10{20} cm{-3}. For dense plasmas, our experimental data strongly support a nonequilibrium kinetics model that uses impact ionization cross sections based on classical free-electron collisions.

Fragmentation and ionization dynamics of C60 in elliptically polarized femtosecond laser fields.

Ionization and fragmentation of C60 fullerenes is studied in elliptically polarized, intense fs laser fields at 797 nm [I=(0.5-4.3)x10;{14} W cm;{-2}] and contrasted with Xe+, utilizing time-of-flight mass spectrometry. Very pronounced changes of parent and fragment ion yield as a function of ellipticity are observed. At lower intensities reduction of the ion yield for circular polarization establishes a coherent two-photon process connected with the key role of the LUMO+1(t_{1g}) "doorway state" and multielectron dynamics. Comparison with the behavior at 399 nm corroborates this finding. At high intensities enhanced fragmentation is observed which is tentatively attributed to returning loops of electron trajectories by the combined action of the C60+ field and the circular laser field.

Photochemical processes in doped argon-neon core-shell clusters: the effect of cage size on the dissociation of molecular oxygen.

The caging effect of the host environment on photochemical reactions of molecular oxygen is investigated using monochromatic synchrotron radiation and spectrally resolved fluorescence. Oxygen doped clusters are formed by coexpansion of argon and oxygen, by pickup of molecular oxygen or by multiple pickup of argon and oxygen by neon clusters. Sequential pickup provides radially ordered core-shell structures in which a central oxygen molecule is surrounded by argon layers of variable thickness inside large neon clusters. Pure argon and core-shell argon-neon clusters excited with approximately 12 eV monochromatic synchrotron radiation show strong fluorescence in the vacuum ultraviolet (vuv) spectral range. When the clusters are doped with O2, fluorescence in the visible (vis) spectral range is observed and the vuv radiation is found to be quenched. Energy-resolved vis fluorescence spectra show the 2 1Sigma+-->1 1Sigma+(ArO(1S)-->ArO(1D)) transition from argon oxide as well as the vibrational progression A '3Delta u(nu'=0)-->X 3Sigmag*(nu") of O2 indicating that molecular oxygen dissociates and occasionally recombines depending on the experimental conditions. Both the emission from ArO and O2 as well the vuv quenching by oxygen are found to depend on the excitation energy, providing evidence that the energy transfer from the photoexcited cluster to the embedded oxygen proceeds via the O2+ ground state. The O2+ decays via dissociative recombination and either reacts with Ar resulting in electronically excited ArO or it recombines to O2 within the Ar cage. Variation of the Ar layer thickness in O2-Ar-Ne core-shell clusters shows that a stable cage is formed by two solvation layers.

Bremsstrahlung and line spectroscopy of warm dense aluminum plasma heated by xuv free-electron-laser radiation.

We report the creation of solid-density aluminum plasma using free-electron laser (FEL) radiation at 13.5nm wavelength. Ultrashort pulses were focused on a bulk Al target, yielding an intensity of 2x10;{14}Wcm;{2} . The radiation emitted from the plasma was measured using an xuv spectrometer. Bremsstrahlung and line intensity ratios yield consistent electron temperatures of about 38eV , supported by radiation hydrodynamics simulations. This shows that xuv FELs heat up plasmas volumetrically and homogeneously at warm-dense-matter conditions, which are accurately characterized by xuv spectroscopy.

Coherent control of bond breaking in amino acid complexes with tailored femtosecond pulses.

Intense femtosecond laser pulses, judiciously tailored in an adaptive, optimal control feedback loop were used to break preferentially the acyl-N ("peptide") bond of Ac-Phe-NHMe that may be regarded as a dipeptide model. We show that coherent excitation of complex wave packets in the strong-field regime allows to cleave strong backbone bonds in the molecular system preferentially, while keeping other more labile bonds intact. These results show the potential of pulse shaping as a powerful complementary analytical tool for protein sequencing of large biopolymers in addition to the well-known mass spectrometry and chemical analysis.

Control of giant breathing motion in c60 with temporally shaped laser pulses.

Femtosecond laser pulses tailored with closed-loop, optimal control feedback were used to excite oscillations in C60 with large amplitude by coherent heating of nuclear motion. A characteristic pulse sequence results in significant enhancement of C2 evaporation, a typical energy loss channel of vibrationally hot C60. The separation between subsequent pulses in combination with complementary two-color pump-probe data and time-dependent density functional theory calculations give direct information on the multielectron excitation via the t(1g) resonance followed by efficient coupling to the radial symmetric a(g)(1) breathing mode.

Emission of thermally activated electrons from rare gas clusters irradiated with intense VUV light pulses from a free electron laser.

The ionization dynamics of Ar and Xe clusters irradiated with intense vacuum ultraviolet light from a free-electron laser is investigated using photoelectron spectroscopy. Clusters comprising between 70 and 900 atoms were irradiated with femtosecond pulses at 95 nm wavelength (approximately 13 eV photon energy) and a peak intensity of approximately 4 x 10(12) W/cm2. A broad thermal distribution of emitted electrons from clusters with a maximum kinetic energy up to 30-40 eV is observed. The observation of relatively low-energy photoelectrons is in good agreement with calculations using a time-dependent Thomas-Fermi model and gives experimental evidence of an outer ionization process of the clusters, due to delayed thermoelectronic emission.

Fragmentation dynamics of fullerenes in intense femtosecond-laser fields: loss of small neutral fragments on a picosecond time scale.

The fragmentation dynamics of C60 irradiated with intense femtosecond laser pulses is studied with one-color pump-probe spectroscopy. Small neutral fragments (C, C2, and C3) are formed by an 800-nm pump pulse which are then postionized by a delayed probe pulse. The respective ion signals detected by the time-of-flight mass spectrometry dramatically increase on a time scale of 10-20 ps.

Multiple ionization of rare gas atoms irradiated with intense VUV radiation.

The interaction of intense vacuum-ultraviolet radiation from a free-electron laser with rare gas atoms is investigated. The ionization products of xenon and argon atomic beams are analyzed with time-of-flight mass spectroscopy. At 98 nm wavelength and approximately 10(13) W/cm(2) multiple charged ions up to Xe6+ (Ar4+) are detected. From the intensity dependence of multiple charged ion yields the mechanisms of multiphoton processes were derived. In the range of approximately 10(12)-10(13) W/cm(2) the ionization is attributed to sequential multiphoton processes. The production of multiple charged ions saturates at 5-30 times lower power densities than at 193 and 564 nm wavelength, respectively.

Isotopic effect on the cage-induced quenching of OH(A)/OD(A) inside small argon clusters.

In this paper we report on the isotopic effect on the cage-induced excited-state quenching inside small Ar(m) clusters (m<10(2)) solvated in large Ne(N) clusters (N approximately 7.5x10(3)). Excited OH(A)/OD(A) fragments are produced by photodissociation of H2O and D2O molecules and the quenching agents are correspondingly H or D atoms. The decrease of the fluorescence yield with the size of the cluster m>m0 is observed in both cases and it is attributed to the formation of the cage of argon atoms around the doped molecule. Interestingly, more atoms are needed to induce the fluorescence quenching of OD*(A) fragments, m0=21+/-3, compared to the electronically excited state quenching of OH*(A) molecules, 11+/-2. A diffusion model containing two free parameters, the quenching cross section sigmaq and the number of argon atoms forming the cage m0, explains the effect in terms of the residence time of the hydrogen atom inside the cage. We suggest that the melting of the doped rare gas clusters is responsible for the different predissociation dynamics. The quenching cross section obtained from the experimental data is in good agreement with former experiments.