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High power mid-infrared (MID-IR) laser systems delivering ultrashort pulses at high repetition rates are of considerable interest for vibrational spectroscopy, label-free microscopy, ultrafast dynamics and HHG studies. To meet these requirements, we developed an optical parametric chirped-pulse amplifier (OPCPA) with a difference frequency generation (DFG) stage to provide an efficient platform to down-convert a 200 W Yb-YAG pump laser into the MID-IR range. The MID-IR pulses are tunable from 4.2-11 μm, with a maximum pulse energy around 9 μm with 2.2 μJ at 200 kHz supporting a Fourier limit of 50 fs. In addition, thermal parameters of various nonlinear crystals are reviewed for high power MID-IR OPCPAs.

Physical review / A covering atomic, molecular, and optical physics and quantum information 101(6), 063412 (2020). doi:10.1103/PhysRevA.101.063412, Focused short-wavelength free-electron laser (FEL) pulses interacting with gas phase samples can induce by inner-shell ionization a short-lived population inversion, followed by coherent collective emission of directed, short, and strong radiation bursts. We extend our studies into the warm-dense matter (WDM) regime by investigating the nanoplasmas produced in an ensemble of nanometer-sized clusters by FEL irradiation. Here, additional pathways can also lead to strong, laserlike emission: Electron-ion collisions can yield a long-lived population inversion, and subsequent amplified spontaneous emission. We observe amplified spontaneous emission (ASE) in the extreme ultraviolet in xenon clusters excited by soft x-ray FEL pulses, we diagnose the generated nanoplasmas by fluorescence spectroscopy, and we study under various cluster and FEL parameters the directed ASE from the Xe$^{2+}$ 65 nm line. We show its exponential increase as a function of FEL irradiation power, and an accompanying collisional broadening of the emission spectra. These findings are corroborated by extensive numerical simulations based on theory, combining detailed hydrodynamic and kinetic simulations with time-dependent calculations of radiation transport, amplification, and collective emission in the WDM nanoplasma. Our theoretical findings underline that population inversion is due to electron-ion collisions and that the observed decoherence processes can be empirically characterized by a phenomenological decoherence time in the range of 100–200 fs., Published by Inst., Woodbury, NY

Free-electron lasers (FELs) generate femtosecond XUV and X-ray pulses at peak powers in the gigawatt range. The FEL user facility FLASH at DESY (Hamburg, Germany) is driven by a superconducting linear accelerator with up to 8000 pulses per second. Since 2014, two parallel undulator beamlines, FLASH1 and FLASH2, have been in operation. In addition to the main undulator, the FLASH1 beamline is equipped with an undulator section, sFLASH, dedicated to research and development of fully coherent extreme ultraviolet photon pulses using external seed lasers. In this contribution, the first simultaneous lasing of the three FELs at 13.4 nm, 20 nm and 38.8 nm is presented.

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.

The XUV free electron laser FLASH, has been recently operated in the high-gain harmonic generation (HGHG) mode. We characterized the laser-induced energy modulation, as well as the temporal profile of the seeded FEL pulses. FEL saturation was reached for the 7th harmonic of the 266 nm seed laser.

Scientific reports 7(1), 2431(2017). doi:10.1038/s41598-017-02184-3, Free-electron lasers are unique sources of intense and ultra-short x-ray pulses that led to major scientific breakthroughs across disciplines from matter to materials and life sciences. The essential element of these devices are micrometer-sized electron bunches with high peak currents, low energy spread, and low emittance. Advanced FEL concepts such as seeded amplifiers rely on the capability of analyzing and controlling the electron beam properties with few-femtosecond time resolution. One major challenge is to extract tomographic slice parameters instead of projected electron beam properties. Here, we demonstrate that a radio-frequency deflector in combination with a dipole spectrometer not only allows for single-shot extraction of a seeded FEL pulse profile, but also provides information on the electron slice emittance and energy spread. The seeded FEL power profile can be directly related to the derived slice emittance as a function of intra-bunch coordinate with a resolution down to a few femtoseconds., Published by Springer Nature, London

Direct seeding with a high-harmonic generation (HHG) source can improve the spectral, temporal, and coherence properties of a free-electron laser (FEL) and shall reduce intensity and arrival-time fluctuations. In the seeding experiment sFLASH at the extreme ultraviolet FEL in Hamburg FLASH, which operates in the self-amplified spontaneous emission mode (SASE), the 21st harmonic of an 800 nm laser is refocused into a dedicated seeding undulator. For seeding, the external light field has to overcome the noise level of SASE; therefore, an efficient coupling between seed pulse and electron bunch is mandatory. Thus, an HHG beam with a proper divergence, width, beam quality, Rayleigh length, pointing stability, single-shot pulse energy, and stability in the 21st harmonic is needed. Here, we present the setup of the HHG source that seeds sFLASH at 38.1 nm, the optimization procedures, and the necessary diagnostics.

We report on soft X-ray scattering experiments on cryogenic hydrogen and simple metal samples. As a source of intense, ultrashort soft X-ray pulses we have used free-electron laser radiation at 92 eV photon energy from FLASH at DESY, Hamburg. X-ray pulses with energies up to 150 μJ and durations 15-50 fs provide interaction with the sample leading simultaneously to plasma formation and scattering. Experiments exploiting both of these interactions have been carried out, using the same experimental setup. Firstly, recording of soft X-ray inelastic scattering from near-solid density hydrogen plasmas at few electron volt temperatures confirms the feasibility of this diagnostics technique. Secondly, the soft X-ray excitation of few electron volt solid-density plasmas in bulk metal samples could be studied by recording soft X-ray line and continuum emission integrated over emission times from fs to ns. © 2009 Elsevier B.V.

We report on the x-ray absorption of Warm Dense Matter experiment at the FLASH Free Electron Laser (FEL) facility at DESY. The FEL beam is used to produce Warm Dense Matter with soft x-ray absorption as the probe of electronic structure. A multilayer-coated parabolic mirror focuses the FEL radiation, to spot sizes as small as 0.3μm in a ∼15fs pulse of containing >10 12 photons at 13.5 nm wavelength, onto a thin sample. Silicon photodiodes measure the transmitted and reflected beams, while spectroscopy provides detailed measurement of the temperature of the sample. The goal is to measure over a range of intensities approaching 10 18 W/cm 2. Experimental results will be presented along with theoretical calculations. A brief report on future FEL efforts will be given. © 2009 SPIE.

Unraveling and controlling chemical dynamics requires techniques to image structural changes of molecules with femtosecond temporal and picometer spatial resolution. Ultrashort-pulse x-ray free-electron lasers have significantly advanced the field by enabling advanced pump-probe schemes. There is an increasing interest in using table-top photon sources enabled by high-harmonic generation of ultrashort-pulse lasers for such studies. We present a novel high-harmonic source driven by a 100 kHz fiber laser system, which delivers 10sup11/supphotons/s in a single 1.3 eV bandwidth harmonic at 68.6 eV. The combination of record-high photon flux and high repetition rate paves the way for time-resolved studies of the dissociation dynamics of inner-shell ionized molecules in a coincidence detection scheme. First coincidence measurements on CHsub3/subI are shown and it is outlined how the anticipated advancement of fiber laser technology and improved sample delivery will, in the next step, allow pump-probe studies of ultrafast molecular dynamics with table-top XUV-photon sources. These table-top sources can provide significantly higher repetition rates than the currently operating free-electron lasers and they offer very high temporal resolution due to the intrinsically small timing jitter between pump and probe pulses.

We report a comprehensive investigation of the electronically excited states of helium clusters and droplets of sizes ranging from a few to several 10(7) atoms using time-resolved fluorescence excitation spectroscopy and quantum chemical ab initio calculations. We employ various approaches for our analysis considering the lifetime-dependence of the fluorescence intensity, spectral shifts, intensity scaling with cluster size, isotopic dependence, and density-dependence of the calculated electron wave function radii. A unique feature of helium clusters and droplets is their radially varying particle density. Our results show that short-lived fluorescence is sensitive to regions of increased density and probes excitations located in the bulk volume, whereas long-lived fluorescence is sensitive to regions of reduced density such as for small clusters or for the surface of large droplets. Spectra of (3)He droplets serve as a reference for low density, but are free from contributions of small clusters. This allows us to distinguish regions of reduced density as these can be due to both surface states or small clusters. Our analysis reveals a picture where spectral features are related to regions of different density due to isotopic composition, cluster size, and surface or bulk volume location of the excitations. The 2s and 2p related excitations appear as blue-shifted wings for small clusters or for excited atoms within the surface layer, whereas in the bulk-volume of large droplets, they appear as distinct bands with large intensities, dominating the entire spectrum. Excitations at energies higher than 23 eV are unambiguously assigned to regions of low and medium density location within the deeper parts of the surface layer but show no relation to the bulk volume. Our findings support the idea that in liquid helium high-lying states and, in particular, Rydberg states are quenched in favor of the 2s and 2p excitations.

New journal of physics 20, 013010 (2017). doi:10.1088/1367-2630/aa9b4c, We report on a direct time-domain measurement of the temporal properties of a seeded free-electron laser pulse in the extreme ultraviolet spectral range. Utilizing the oscillating electromagnetic field of terahertz radiation, a single-shot THz streak-camera was applied for measuring the duration as well as spectral phase of the generated intense XUV pulses. The experiment was conducted at FLASH, the free electron laser user facility at DESY in Hamburg, Germany. In contrast to indirect methods, this approach directly resolves and visualizes the frequency chirp of a seeded FEL pulse. The reported diagnostic capability is a prerequisite to tailor amplitude, phase and frequency distributions of FEL beams on demand. In particular, it opens up a new window of opportunities for advanced coherent spectroscopic studies making use of the high degree of temporal coherence expected from a seeded FEL pulse., Published by IOP Publ., [Bad Honnef]

Measurements of the longitudinal phase-space distribution of electron bunches seeded with an external laser were done in order to study the impact of collective effects on seeded microbunches in free-electron lasers. Velocity bunching of a seeded microbunch appears to be a viable alternative to compression with a magnetic chicane under high-gain harmonic generation seeding conditions when the collective effects of Coulomb forces in a drift space and coherent synchrotron radiation in a chicane are considered. Measurements of these effects on seeded electron microbunches were performed with an RF deflecting structure and a dipole magnet which streak out the electron bunch for single-shot images of the longitudinal phase-space distribution. Particle tracking simulations in 3D predicted the compression dynamics of the seeded microbunches with collective effects., Proceedings of the 37th International Free Electron Laser Conference, FEL2015, Daejeon, Republic of Korea

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 $11+$.

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. (Less)

Femtosecond x-ray laser flashes with power densities of up to ${10}^{14}\text{ }\text{ }\mathrm{W}/{\mathrm{cm}}^{2}$ 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 ${\mathrm{Xe}}^{4+}$. 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.

FLASH has been a user facility since 2005, delivering radiation in the wavelength range between 7 and 47 nm using the SASE principle. After the present upgrade, the wavelength range is extended to 4.45 nm. With the third harmonic accelerating module in place to linearize the longitudinal phase space, the stability and reproducibility of the machine is substantially improved. The user requests for beam time by far exceeds the time available. In order to increase user beam time and to improve the radiation properties delivered to users, a major extension of the user facility called FLASH II has been proposed by DESY in collaboration with the HZB. FLASH II is a seeded FEL in the parameter range of FLASH. As logical continuation, the seeding with HHG which started with sFLASH will result in direct seeding. Because in the foreseeable future there will probably not be HHG seed lasers available at high repetition rates down to wavelengths of 4 nm, a cascaded HGHG scheme is proposed to produce short wavelengths. After a first design report, the project now enters its technical design phase. During this time, the FLASH beam parameters after the present upgrade 2009/2010 will be characterized and the present design will be re-evaluated and adjusted. In addition, start-to-end simulations will complete the simulations which have been performed so far, including a design of the extraction area.

Tampering of a sample with a layer of another material is a promising technique to slow down the expansion dynamics within laser irradiated samples, with sound implications for single-particle diffraction imaging. Ideally, if an imaged object is covered by a layer of another material, during the irradiation this layer will be primarily ionized and will expand fast due to Coulomb repulsion, whereas the object located within the net neutral core will expand more slowly (hydrodynamically). We investigate the details of the electronic damage within the tampered samples during their irradiation with an intense extreme ultraviolet (EUV) pulse. We study heterogeneous clusters composed of noble gas atoms, Xe and Ar, for which chemical-bond effects can be neglected. Using a fully nonequilibrium kinetic equation code, we demonstrate the influence of cluster composition on ionization dynamics; in particular, on the electronic damage. The results are obtained for the wavelength of 32 nm, which is available at the free-electron laser in Hamburg (FLASH) facility, but our conclusions can also have implications for samples with a more complex structure and irradiated at a much shorter wavelength.

Ultra-fast laser sources have revolutionized many fields in science. As technology improves, new applications can be made accessible. The OPCPA technique has shown potential to be the key technology for future amplifier systems, but hasn’t achieved a breakthrough such as Ti:Sapphire laser technology, mostly due to the complex pump amplifier design. We present an operationally stable OPCPA system that might turn the tide for OPCPA technology. This first prototype system will be used in the accelerator environment at the FLASH free electron laser at DESY in Hamburg. The envisioned key parameters for this amplifier are >1 mJ pulse energy with a repetition rate of 100 kHz and a pulse duration of

International audience; X-ray scattering using highly brilliant X-ray free-electron laser (FEL) radiation provides a new access to probe free electron density, temperature and ionization in near-solid density plasmas. First experiments at the soft X-ray FEL FLASH at DESY, Hamburg, show the capabilities of this technique. The ultrashort FEL pulses in particular can probe equilibration phenomena occurring after excitation of the plasma using ultrashort optical laser pumping. We have investigated liquid hydrogen and find that the interaction of very intense soft X-ray FEL radiation alone heats the sample volume. As the plasma establishes, photons from the same pulse undergo scattering, thus probing the transient, warm dense matter state. We find a free electron density of (2.6 ± 0.2) · 10 20 cm −3 and an electron temperature of 14 ± 3.5 eV. In pump-probe experiments, using intense optical laser pulses to generate more extreme states of matter, this interaction of the probe pulse has to be considered in the interpretation of scattering data. In this paper we present details of the experimental setup at FLASH and the diagnostic methods used to quantitatively analyze the data. Probing near-solid density plasmas using soft X-ray scattering 2 Plasma production and heating by laser beams Probing near-solid density plasmas using soft X-ray scattering 3

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.

26th International Conference on Photonic, Electronic and Atomic Collisions, ICPEAC 2009, Kalamazoo, Michigan, USA, 22 Jul 2009 - 28 Jul 2009; Journal of physics / Conference Series 194, 032066 (2009). doi:10.1088/1742-6596/194/3/032066, Charge recombination in a nanoplasma produced by a short soft x-ray pulse from the FLASH freeelectron laser has been observed. XeAr core-shell clusters have been used to follow charge migration and frag-mentation dynamics. After multiple ionization of the Xe core, the charge is transferred to the outer Ar shells.While the shells explode the inner nanoplasma expands and recombines slowly. This delayed expansion of thecore could be of major importance for future imaging experiments at x-ray FELs., Published by IOP Publ., Bristol

We present the attempt to diagnose electron temperature and density of a plasma via Thomson Scattering in the Warm Dense Matter Regimew using soft x-ray Free Electron Laser radiation. A preliminary Self Thomson Scattering experiment has already been conducted. In a current pump-probe experiment, together with an optical heating laser, we will record the temporal evolution of the plasma achieving a resolution of approximately 250fs.

We present collective Thomson scattering with soft x-ray free electron laser radiation as a method to track the evolution of warm dense matter plasmas with ∼200 fs time resolution. In a pump-probe scheme an 800 nm laser heats a 20 ∼m hydrogen droplet to the plasma state. After a variable time delay in the order of ps the plasma is probed by an x-ray ultra violet (XUV) pulse which scatters from the target and is recorded spectrally. Alternatively, in a self-Thomson scattering experiment, a single XUV pulse heats the target while a portion of its photons are being scattered probing the target. From such inelastic x-ray scattering spectra free electron temperature and density can be inferred giving insight on relaxation time scales in plasmas as well as the equation of state. We prove the feasibility of this method in the XUV range utilizing the free electron laser facility in Hamburg, FLASH. We recorded Thomson scattering spectra for hydrogen plasma, both in the self-scattering and in the pump-probe mode using optical laser heating. © 2009 SPIE-.

We report the creation of solid-density aluminum plasma using free-electron laser (FEL) radiation at $13.5\phantom{\rule{0.3em}{0ex}}\mathrm{nm}$ wavelength. Ultrashort pulses were focused on a bulk Al target, yielding an intensity of $2\ifmmode\times\else\texttimes\fi{}{10}^{14}\phantom{\rule{0.3em}{0ex}}\mathrm{W}∕{\mathrm{cm}}^{2}$. The radiation emitted from the plasma was measured using an xuv spectrometer. Bremsstrahlung and line intensity ratios yield consistent electron temperatures of about $38\phantom{\rule{0.3em}{0ex}}\mathrm{eV}$, 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.

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.

Recent progress in the understanding of the primary excitation mechanisms of the C60 fullerene in intense laser pulses is reported. By analyzing mass spectra as a function of pulse duration, laser intensity and time delay between pump- and probe pulse insight into fundamental photoinduced processes such as ionization and fragmentation is obtained. Using ultrashort sub-10fs pulses excitation times are addressed which lie well below the characteristic time scales for electron–electron and electron–phonon coupling. The measured saturation intensities of multiply charged parent ions indicate that for higher charge states the well known C60 giant plasmon resonance is involved in creating ions and a significant amount of large fragments through a non-adiabatic multi-electron dynamics. To enhance the formation of large fragments femtosecond laser pulses tailored with closed-loop, optimal control feedback were used. A characteristic pulse sequence excites oscillations in C60 with large amplitude by coherent heating of nuclear motion. Again, the experimental findings can be understood by a laser-induced multi-electron excitation via the electronically excited resonance followed by efficient coupling to the radial symmetric breathing vibration of C60.

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.

We performed time-of-flight (TOF) spectroscopy on a jet of rare gas clusters using light pulses at λFEL = 32 nm produced by the FLASH VUV freeelectron-laser (Hamburg, Germany) with a maximum peak power density of about 3 × 1013 W/cm2 at the sample. Energy deposition on the clusters was found to be strongly dependent on lambda and much more efficient in the VUV than in the IR and visible spectral range. We observed multiple ionization of rare gas atoms coming from clusters; the latter fragment completely upon absorption of a single pulse. We have also measured high quality photoelectron spectra. Small angle soft X-ray scattering (SAXS) from a single light pulse (λFEL = 32 nm), was recorded with high signal to noise ratio for very large (Natoms 3 × 106) Argon clusters.

Dense cryogenic hydrogen is heated by intense femtosecond infrared laser pulses at intensities of 1015-1016 Wcm-2. Three-dimensional particle-in-cell (PIC) simulations predict that this heating is limited to the skin depth, causing an inhomogeneously heated outer shell with a cold core and two prominent temperatures of about 25 and 40 eV for simulated delay times up to +70 fs after the laser pulse maximum. Experimentally, the time-integrated emitted bremsstrahlung in the spectral range of 8-18 nm was corrected for the wavelength-dependent instrument efficiency. The resulting spectrum cannot be fit with a single temperature bremsstrahlung model, and the best fit is obtained using two temperatures of about 13 and 30 eV. The lower temperatures in the experiment can be explained by missing energy-loss channels in the simulations, as well as the inclusion of hot, non- Maxwellian electrons in the temperature calculation. We resolved the time-scale for laser-heating of hydrogen, and PIC results for laser-matter interaction were successfully tested against the experiment data.

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.

Physical review / A 74(2), 027402 (2006). doi:10.1103/PhysRevA.74.027402, Published by APS, College Park, Md.

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.

Publisher Summary This chapter presents notions, facts, and findings on C60 and the fullerenes. The chapter discusses basic terminology and concepts from the area of atoms and molecules in strong fields. Some experimental aspects of studying molecules in intense, short pulse laser fields are addressed. The chapter also explains the ionization process, charge states, and fragmentation after short pulse laser interaction with C60 as observed by mass spectroscopy. The intensity dependence of these processes and compares saturation intensities for the ionization processes with simple atomic systems is addressed in the chapter. Further, the above threshold ionization (ATI) observed in photoelectron spectra at various short pulse laser intensities are discussed and compared with the recent theoretical results. Theoretical comparison leads to a critical discussion of the primary excitation mechanism in an intense laser pulse. The chapter also discusses the band structure model in condensed matter, that is, for a semiconductor in the case of C60. The chapter illustrates this with an example: the non-resonant excitation of Rydberg states in C60. Further, the fast fragmentation processes of C60 beyond the established statistical fragmentation processes known to occur on the ns to μs time scale are addressed.

Physical review letters 95, 063402 (2005). doi:10.1103/PhysRevLett.95.063402, Published by APS, College Park, Md.

Intense radiation from lasers has opened up many new areas of research in physics and chemistry, and has revolutionized optical technology. So far, most work in the field of nonlinear processes has been restricted to infrared, visible and ultraviolet light, although progress in the development of X-ray lasers has been made recently. With the advent of a free-electron laser in the soft-X-ray regime below 100 nm wavelength, a new light source is now available for experiments with intense, short-wavelength radiation that could be used to obtain deeper insights into the structure of matter. Other free-electron sources with even shorter wavelengths are planned for the future. Here we present initial results from a study of the interaction of soft X-ray radiation, generated by a free-electron laser, with Xe atoms and clusters. We find that, whereas Xe atoms become only singly ionized by the absorption of single photons, absorption in clusters is strongly enhanced. On average, each atom in large clusters absorbs up to 400 eV, corresponding to 30 photons. We suggest that the clusters are heated up and electrons are emitted after acquiring sufficient energy. The clusters finally disintegrate completely by Coulomb explosion.

A key feature of extreme ultraviolet (XUV) radiation from free-electron lasers (FELs) is its spatial and temporal coherence. We measured the spatio-temporal coherence properties of monochromatized FEL pulses at 13.5 nm using a Michelson interferometer. A temporal coherence time of (59±8) fs has been determined, which is in good agreement with the spectral bandwidth given by the monochromator. Moreover, the spatial coherence in vertical direction amounts to about 15% of the beam diameter and about 12% in horizontal direction. The feasibility of measuring spatio-temporal coherence properties of XUV FEL radiation using interferometric techniques advances machine operation and experimental studies significantly.

We have developed an easy-to-use and reliable timing tool to determine the arrival time of an optical laser and a free electron laser (FEL) pulses within the jitter limitation. This timing tool can be used from XUV to X-rays and exploits high FELs intensities. It uses a shadowgraph technique where we optically (at 800 nm) image a plasma created by an intense XUV or X-ray FEL pulse on a transparent sample (glass slide) directly placed at the pump - probe sample position. It is based on the physical principle that the optical properties of the material are drastically changed when its free electron density reaches the critical density. At this point the excited glass sample becomes opaque to the optical laser pulse. The ultra-short and intense XUV or X-ray FEL pulse ensures that a critical electron density can be reached via photoionization and subsequent collisional ionization within the XUV or X-ray FEL pulse duration or even faster. This technique allows to determine the relative arrival time between the optical laser and the FEL pulses in only few single shots with an accuracy mainly limited by the optical laser pulse duration and the jitter between the FEL and the optical laser. Considering the major interest in pump-probe experiments at FEL facilities in general, such a femtosecond resolution timing tool is of utmost importance. © 2012 IOP Publishing Ltd and Sissa Medialab srl.

The ionization and charge separation processes of nanoplasmas created by resonant excitation of atomic clusters in intense soft x-ray pulses have been investigated. Through irradiation with femtosecond pulses from the FLASH free electron laser (FEL) at ? = 13.7 nm and power densities exceeding 1014 W cm?2 the clusters are highly ionized with transient atomic charge states up to 9+. Variation of the cluster composition from pristine to doped and core?shell systems allows tracking of the spatial origin and charge states of the fragments yielding insight into the nanoplasma dynamics. The data give evidence for efficient charge redistribution processes leading to a Coulomb explosion of the cluster outer part and recombination of the nanoplasma core. The experiments show qualitatively different processes for (soft) x-ray produced nanoplasmas from the optical (IR) strong-field regime where the clusters disintegrate completely in a Coulomb explosion.

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.

The interaction of C60 fullerenes with 765-797 nm laser pulses as short as 9 fs at intensities of up to 3.7 x 10(14) W cm(-2) is investigated with photoion spectroscopy. The excitation time thus addressed lies well below the characteristic time scales for electron-electron and electron-phonon couplings. Thus, energy deposition into the system is separated from energy redistribution among the various electronic and nuclear degrees of freedom. Insight into fundamental photoinduced processes such as ionization and fragmentation is obtained from the analysis of the resulting mass spectra as a function of pulse duration, laser intensity, and time delay between pump and probe pulses, the latter revealing a memory effect for storing electronic energy in the system with a relaxation time of about 50 fs. Saturation intensities and relative abundances of (multiply charged) parent and fragment ions (C60(q+), q=1-6) are fingerprints for the ionization and fragmentation mechanisms. The observations indicate that for final charge states q1 the well known C60 giant plasmon resonance is involved in creating ions and a significant amount of large fragments even with 9 fs pulses through a nonadiabatic multielectron dynamics. In contrast, for energetic reasons singly charged ions are generated by an essentially adiabatic single active electron mechanism and negligible fragmentation is found when 9 fs pulses are used. These findings promise to unravel a long standing puzzle in understanding C60 mass spectra generated by intense femtosecond laser pulses.

A review of the thermal parameters of Li-based nonlinear crystals is presented and preliminary results demonstrate a 8 µm laser system with 2 µJ at 200 kHz supporting a Fourier limit of under 100 fs.