X-ray Fourier transform holography with beam shaping optical elements.

Holography is a powerful method for achieving 3D images of objects. Extending this method to short wavelengths potentially offers significantly higher resolution than visible light holography. However, current X-ray holography setups employ nanoscale pinholes to form the reference wave. This approach is relatively inefficient and limited to very small sample size. Here, we propose a new setup for X-ray holography based on a binary diffractive optical element (DOE), which forms at the same time the object illumination and the reference wave. This optic is located separately from the sample plane, which permits investigation of larger sample areas. Using an extended test sample, we demonstrate a resolution of 90 nm (half-pitch) at an undulator beamline at BESSY II. The new holography setup can be directly transferred to free electron laser sources enabling time-resolved nanoscale imaging for ultra-fast processes.

Transverse Coherence Limited Coherent Diffraction Imaging using a Molybdenum Soft X-ray Laser Pumped at Moderate Pump Energies.

Coherent diffraction imaging (CDI) in the extreme ultraviolet has become an important tool for nanoscale investigations. Laser-driven high harmonic generation (HHG) sources allow for lab scale applications such as cancer cell classification and phase-resolved surface studies. HHG sources exhibit excellent coherence but limited photon flux due poor conversion efficiency. In contrast, table-top soft X-ray lasers (SXRL) feature excellent temporal coherence and extraordinary high flux at limited transverse coherence. Here, the performance of a SXRL pumped at moderate pump energies is evaluated for CDI and compared to a HHG source. For CDI, a lower bound for the required mutual coherence factor of |µ 12| ≥ 0.75 is found by comparing a reconstruction with fixed support to a conventional characterization using double slits. A comparison of the captured diffraction signals suggests that SXRLs have the potential for imaging micron scale objects with sub-20 nm resolution in orders of magnitude shorter integration time compared to a conventional HHG source. Here, the low transverse coherence diameter limits the resolution to approximately 180 nm. The extraordinary high photon flux per laser shot, scalability towards higher repetition rate and capability of seeding with a high harmonic source opens a route for higher performance nanoscale imaging systems based on SXRLs.

A laboratory 8 keV transmission full-field x-ray microscope with a polycapillary as condenser for bright and dark field imaging.

This article introduces a laboratory setup of a transmission full-field x-ray microscope at 8 keV photon energy. The microscope operates in bright and dark field imaging mode with a maximum field of view of 50 µm. Since the illumination geometry determines whether the sample is illuminated homogeneously and moreover, if different imaging methods can be applied, the condenser optic is one of the most significant parts. With a new type of x-ray condenser, a polycapillary optic, we realized bright field imaging and for the first time dark field imaging at 8 keV photon energy in a laboratory setup. A detector limited spatial resolution of 210 nm is measured on x-ray images of Siemens star test patterns.

Note: Thickness determination of freestanding ultra-thin foils using a table top laboratory extreme ultraviolet source.

We present a versatile and handy method allowing a thickness determination of freestanding thin plastic foils by its transmission characteristics in the extreme ultraviolet (EUV) spectrum. The method is based on a laser induced plasma source, emitting light in the EUV region, a compact double-mirror EUV monochromator operating at a fixed wavelength of 18.9 nm, and a CCD camera. The measurement delivers transmission values with a standard deviation of ΔT = 0.005 enabling foils thickness characterization with nm-accuracy at a given foil density and stoichiometric composition. Well characterized freestanding ultra-thin foils can be directly implemented in, e.g., high intensity laser matter experiments without further manipulation.

Speckle statistics and transverse coherence of an x-ray laser with fluctuations in its active medium.

It is shown that the statistics of the intensity distribution in the output beam of a collisional X-ray laser, analysed in terms of the degree of freedom or equivalently the number of the coherence modes in the beam cross-section, has non-Gaussian character. The non-Gaussian character seems to be caused by the small-scale plasma/medium fluctuations. It was assumed that these overlap the modal structure imposed by the geometry of the medium and considered as equivalent to a large-scale inhomogeneity. Thus, the fluctuations decide about the character of the output beam transverse coherence. It is also shown that the relevant to this model compound statistics of the intensity fluctuations in the output beam is well described by the m-m-distribution, a specific form of the K-distribution. The deviation from the Gaussian statistics was confirmed by the field correlation function at the laser exit plane, retrieved from the experimental data.

High average brightness water window source for short-exposure cryomicroscopy.

Laboratory water window cryomicroscopy has recently demonstrated similar image quality as synchrotron-based microscopy but still with much longer exposure times, prohibiting the spread to a wider scientific community. Here we demonstrate high-resolution laboratory water window imaging of cryofrozen cells with 10 s range exposure times. The major improvement is the operation of a λ=2.48 nm, 2 kHz liquid nitrogen jet laser plasma source with high spatial and temporal stability at high average brightness >1.5×10(12) ph/(s×sr×µm(2)×line), i.e., close to that of early synchrotrons. Thus, this source enables not only biological x-ray microscopy in the home laboratory but potentially other applications previously only accessible at synchrotron facilities.

Compact x-ray microscope for the water window based on a high brightness laser plasma source.

We present a laser plasma based x-ray microscope for the water window employing a high-average power laser system for plasma generation. At 90 W laser power a brightness of 7.4 x 10(11) photons/(s x sr x µm(2)) was measured for the nitrogen Lyα line emission at 2.478 nm. Using a multilayer condenser mirror with 0.3 % reflectivity 10(6) photons/(µm(2) x s) were obtained in the object plane. Microscopy performed at a laser power of 60 W resolves 40 nm lines with an exposure time of 60 s. The exposure time can be further reduced to 20 s by the use of new multilayer condenser optics and operating the laser at its full power of 130 W.

Ethanol (C2H5OH) spray of sub-micron droplets for laser driven negative ion source.

Liquid ethanol (C(2)H(5)OH) was used to generate a spray of sub-micron droplets. Sprays with different nozzle geometries have been tested and characterised using Mie scattering to find scaling properties and to generate droplets with different diameters within the spray. Nozzles having throat diameters of 470 µm and 560 µm showed generation of ethanol spray with droplet diameters of (180 ± 10) nm and (140 ± 10) nm, respectively. These investigations were motivated by the observation of copious negative ions from these target systems, e.g., negative oxygen and carbon ions measured from water and ethanol sprays irradiated with ultra-intense (5 × 10(19) W/cm(2)), ultra short (40 fs) laser pulses. It is shown that the droplet diameter and the average atomic density of the spray have a significant effect on the numbers and energies of accelerated ions, both positive and negative. These targets open new possibilities for the creation of efficient and compact sources of different negative ion species.

Note: study of extreme ultraviolet and soft x-ray emission of metal targets produced by laser-plasma-interaction.

Different metal targets were investigated as possible source material for tailored laser-produced plasma-sources. In the wavelength range from 1 to 20 nm, x-ray spectra were collected with a calibrated spectrometer with a resolution of λ/Δλ = 150 at 1 nm up to λ/Δλ = 1100 at 15 nm. Intense line emission features of highly ionized species as well as continuum-like spectra from unresolved transitions are presented. With this knowledge, the optimal target material can be identified for the envisioned application of the source in x-ray spectrometry on the high energy side of the spectra at about 1 keV. This energy is aimed for because 1 keV-radiation is ideally suited for L-shell x-ray spectroscopy with nm-depth resolution.

Complementary ion and extreme ultra-violet spectrometer for laser-plasma diagnosis.

Simultaneous detection of extreme ultra-violet (XUV) and ion emission along the same line of sight provides comprehensive insight into the evolution of plasmas. This type of combined spectroscopy is applied to diagnose laser interaction with a spray target. The use of a micro-channel-plate detector assures reliable detection of both XUV and ion signals in a single laser shot. The qualitative analysis of the ion emission and XUV spectra allows to gain detailed information about the plasma conditions, and a correlation between the energetic proton emission and the XUV plasma emission can be suggested. The measured XUV emission spectrum from water spray shows efficient deceleration of laser accelerated electrons with energies up to keV in the initially cold background plasma and the collisional heating of the plasma.

High-repetition-rate chirped-pulse-amplification thin-disk laser system with joule-level pulse energy.

We are reporting on the development of a diode-pumped chirped-pulse-amplification (CPA) laser system based on Yb:YAG thin-disk technology with a repetition rate of 100 Hz and output pulse energy in the joule range. The focus lies with the first results of the preamplifier--a regenerative amplifier (RA) and a multipass amplifier (MP). The system consists of a front end including the CPA stretcher followed by an amplifier chain based on Yb:YAG thin-disk amplifiers and the CPA compressor. It is developed in the frame of our x-ray laser (XRL) program and fulfills all requirements for pumping a plasma-based XRL in grazing incidence pumping geometry. Of course it can also be used for other interesting applications. With the RA pulse energies of more than 165 mJ can be realized. At a repetition rate of 100 Hz a stability of 0.8% (1sigma) over a period of more than 45 min has been measured. The optical-to-optical efficiency is 14%. The following MP amplifier can increase the pulse energy to more than 300 mJ. A nearly bandwidth-limited recompression to less than 2 ps could be demonstrated.

High spectral resolution x-ray optics with highly oriented pyrolytic graphite.

Thin films of highly oriented pyrolytic graphite (HOPG) give the opportunity to realize crystal optics with arbitrary geometry by mounting it on a mould of any shape. A specific feature of HOPG is its mosaicity accompanied by a high integral reflectivity, which is by an order of magnitude higher than that of all other known crystals in an energy range between 2 keV up to several 10 keV. These characteristics make it possible to realize highly efficient collecting optics, which could be also relevant for compact x-ray diagnostic tools and spectrometers. For these applications the achievable spectral resolution of the crystal optics is of interest. In this article measurements with a spectral resolution of E/DeltaE=2900 in the second order reflection and E/DeltaE=1800 in the first order reflection obtained with HOPG crystals are presented. These are by far the highest spectral resolutions reported for HOPG crystals. The integral reflectivity of these very thin films is still comparable with that of ideal Ge crystals. The trade-off between energy resolution and high integral reflectivity for HOPG is demonstrated by determining these parameters for HOPG films of different thickness.

Towards elucidating the energy of the first excited singlet state of xanthophyll cycle pigments by X-ray absorption spectroscopy.

The first excited singlet state (S(1)) of carotenoids (also termed 2A(g)(-)) plays a key role in photosynthetic excitation energy transfer due to its close proximity to the S(1) (Q(y)) level of chlorophylls. The determination of carotenoid 2A(g)(-) energies by optical techniques is difficult; transitions from the ground state (S(0), 1A(g)(-)) to the 2A(g)(-) state are forbidden ("optically dark") due to parity (g <-- //--> g) as well as pseudo-parity selection rules (- <-- //--> -). Of particular interest are S(1) energies of the so-called xanthophyll-cycle pigments (violaxanthin, antheraxanthin and zeaxanthin) due to their involvement in photoprotection in plants. Previous determinations of S(1) energies of violaxanthin and zeaxanthin by different spectroscopic techniques vary considerably. Here we present an alternative approach towards elucidation of the optically dark states of xanthophylls by near-edge X-ray absorption fine structure spectroscopy (NEXAFS). The indication of at least one pi* energy level (about 0.5 eV below the lowest 1B(u)(+) vibronic sublevel) has been found for zeaxanthin. Present limitations and future improvements of NEXAFS to study optically dark states of carotenoids are discussed. NEXAFS combined with simultaneous optical pumping will further aid the investigation of these otherwise hardly accessible states.

Explosion characteristics of intense femtosecond-laser-driven water droplets.

An efficient acceleration of energetic ions is observed when small heavy-water droplets of approximately 20 microm diameter are exposed to ultrafast (approximately 40 fs) Ti:sapphire laser pulses of up to 10(19) W/cm2 intensity. Quantitative measurements of deuteron and neutron spectra were done, allowing one to analyze the outward and inward directed deuteron acceleration from the droplet. Neutron spectroscopy based on the D (d,n) fusion reaction was accomplished in four different spatial directions. The energy shifts of those fusion neutrons produced inside the exploding droplet reflect a remaining deuteron acceleration inside the irradiated droplet along the axis of the incident laser beam. The overall neutron yield of the microdroplets is relatively small as a result of the dominant outward directed acceleration of the deuterons with 1200 neutrons/shot. Relying on the "explosion-like" acceleration of such spherical droplet targets we have developed a spray target consisting of heavy-water microspheres with diameters of 150 nm . Both the high deuteron energies of up to 1 MeV resulting from the irradiation intensity of approximately 10(19) W/cm2 as well as the collisions between the deuterons and the surrounding spray delivered about one order of magnitude more neutrons than the single-droplet system. The approximately 6 x 10(3) neutrons per laser pulse from the spray can be attributed to an efficient deuteron release from a significantly smaller laser excited volume as from deuterium-cluster targets.

Absolute extreme ultraviolet yield from femtosecond-laser-excited Xe clusters.

Large Xe clusters (10(5)-10(6) atoms per cluster) have been irradiated with ultrashort (50 fs) and high-intensity ( approximately 2 x 10(18) W/cm(2)) pulses from a Ti:sapphire multi-TW laser at 800 nm wavelength. Scaling and absolute yield measurements of extreme ultraviolet (EUV) emission in a wavelength range between 7 and 15 nm in combination with cluster target characterization have been used for yield optimization. Maximum emission as a function of the backing pressure and a spatial emission anisotropy covering a factor of two at optimized yields is discussed with a simple model of the source geometry and EUV-radiation absorption. Circularly polarized laser light instead of linear polarization results in a factor of 2.5 higher emission in the 11 to 15 nm wavelength range. This indicates the initial influence of optical-field ionization for the interaction parameter range used and contrasts to collisional heating that seems to influence preferentially higher ionization. Absolute emission efficiency at 13.4 nm of up to 0.5% in 2pi sr and 2.2% bandwidth has been obtained.

Towards time-resolved, coupled structure-function information on carotenoid excited state processes: X-ray and optical short-pulse double resonance spectroscopy.

A novel soft X-ray and optical short-pulse double resonance spectroscopic technique tailor-made to elucidate processes involving the optically forbidden S1 (2(1)A(g)) state of carotenoids in native biological samples (e.g., photosynthetic antenna complexes) is described. The principle relies on probing the near carbon K-edge absorption of the optically excited sample with soft X-rays generated by a laser-induced plasma. A first application concerns location of the 2(1)A(g) state of beta-carotene in vitro. Further applications are proposed.

Evaluation of the energetic position of the lowest excited singlet state of beta-carotene by NEXAFS and photoemission spectroscopy.

In carotenoids the lowest energetic optical transition belonging to the pi-electron system is forbidden by symmetry, therefore the energetic position of the S(1) (2(1)A(g)) level can hardly be assessed by optical spectroscopy. We introduce a novel experimental approach: For molecules with pi-electron systems the transition C1s-->2p(pi*) from inner-atomic to the lowest unoccupied molecular orbital (LUMO) appears in X-ray absorption near edge spectra (NEXAFS) as an intense, sharp peak a few eV below the carbon K-edge. Whereas the peak position reflects the energy of the first excited singlet state in relation to the ionization potential of the molecule, intensity and width of the transition depend on hybridization and bonding partners of the selected atom. Complementary information can be obtained from ultraviolet photoelectron spectroscopy (UPS): At the low binding energy site of the spectrum a peak related to the highest occupied molecular orbital (HOMO) appears. We have measured NEXAFS and UPS of beta-carotene. Based on these measurements and quantum chemical calculations the HOMO and LUMO energies can be derived.

Pigment-protein architecture in the light-harvesting antenna complexes of purple bacteria: does the crystal structure reflect the native pigment-protein arrangement?

Structural analysis of crystallized peripheral (LH2) and core antenna complexes (LH1) of purple bacteria has revealed circular aggregates of high rotational symmetry (C8, C9 and C16, respectively). Quantum-chemical calculations indicate that in particular the waterwheel-like arrangements of pigments should show characteristic structure-sensitive spectroscopic behavior in the near infrared absorption region. Laser-spectroscopic data obtained with non-crystallized, isolated LH2 of Rhodospirillum molischianum are in line with a highly symmetric (C8) circular aggregate, but deviations have been found for LH2 of Rhodobacter sphaeroides and Rhodopseudomonas acidophila. For both the latter, C-shaped incomplete circular aggregates (as seen only recently in electron micrographs of crystallized LH1-reaction center complexes) may be a suitable preliminary model.

Photophysical consequences of coupling bacteriochlorophyll a with serine and its resulting solubility in water.

We investigated the dependence on solvents of optical absorption and emission of the bacteriochlorophyll a-serine (BChl-ser), a water soluble bacteriochlorophyll (BChl) derivative. Comparison between the experimental data and those collected for BChl in nonaqueous solvents shows that only a minor interaction takes place between serine and the macrocycle's pi-electron system. Nevertheless, the coupling with serine results in a small enhancement of the nonradiative relaxation rate from the first excited singlet state S1. In buffered aqueous solution (pH = 7.4), the Stokes shift of the BChl-ser fluorescence and its nonradiative relaxation rate are enhanced compared with those in nonaqueous solutions (Scherz, A., S. Katz, Y. Vakrat, V. Brumfeld, E. Gabelmann, D. Leupold, J. R. Norris, H. Scheer and Y. Salomon (1998) Photosynthesis: Mechanisms and Effects, Vol. V (Edited by G. Garab), pp. 4207-4212. Kluwer Academic, Dordrecht.), probably as a result of a hydrogen bonding between the BChl macrocycle and the water molecules. In aprotic solvents, without hydrogen bonds, the permanent dipole moment of the first excited singlet state in both BChl and BChl-ser is increased compared with the ground state by at least 2.5 Debye.

Photophysical studies of the pheophorbide a dimer.

This work reports on a monomer-dimer equilibrium state of pheophorbide a in solution. A methodology for controlling the equilibrium constant by use of temperature and solvent variation is described. The absorption spectrum of the dimer is calculated, using different prepared equilibria of monomer and dimer in solution. We propose that these aggregates provide a good model for understanding the dimerization process in tetrapyrroles.