Vacuum Ultraviolet Free Electron Laser Research Articles

Infrared spectroscopy of neutral water clusters at finite temperature: Evidence for a noncyclic pentamer

Infrared spectroscopic study of neutral water clusters is crucial to understanding of the hydrogen-bonding networks in liquid water and ice. Here we report infrared spectra of size-selected neutral water clusters, (H2O) n (n = 3-6), in the OH stretching vibration region, based on threshold photoionization using a tunable vacuum ultraviolet free-electron laser. Distinct OH stretch vibrational fundamentals observed in the 3,500-3,600-cm-1 region of (H2O)5 provide unique spectral signatures for the formation of a noncyclic pentamer, which coexists with the global-minimum cyclic structure previously identified in the gas phase. The main features of infrared spectra of the pentamer and hexamer, (H2O) n (n = 5 and 6), span the entire OH stretching band of liquid water, suggesting that they start to exhibit the richness and diversity of hydrogen-bonding networks in bulk water.

Vacuum-Ultraviolet Photon Detections.

Vacuum-ultraviolet (VUV) photon detection technology is an effective means for the exploration in the field of space science (monitoring the formation and evolution of solar storms), high-energy physics (dark matter detection), large-scale scientific facility (VUV free electron lasers) and electronic industry (high-resolution lithography). The advancement of this technology mainly depends on the performance optimization of VUV photodetectors. In this review, we introduced the research progress on the typical VUV photodetectors based on scintillator, photomultiplier tube, semiconductor, and gas, with their unique advantages and optimal performance indicators in different applications summarized. In particular, during recent years, thanks to the advances in ultra-wide bandgap semiconductors, economical VUV photodetectors with low power consumption and small size have been encouragingly developed. Finally, we pointed out the remaining challenges for each type of VUV detector, with the aim of maximizing the performance in a variety of applications in the future.

Application of laser dispersion method in apparatus combining H atom Rydberg tagging time-of-flight technique with vacuum ultraviolet free electron laser

Photodissociation of H2S in the VUV region plays an important role in the atmospheric chemistry and interstellar chemistry. To date, however, few studies have been focused on this topic. In this article, we have described a laser dispersion method applied in the apparatus combining the high-n H atom Rydberg tagging time-of-flight technique with the vacuum ultraviolet free electron laser (VUV FEL). The Lyman-α laser beam (121.6 nm) used in the H-atom detection was generated by the difference frequency four-wave mixing schemes in a Kr/Ar gas cell. After passing through an off-axis biconvex LiF lens, the 121.6 nm beam was dispersed from the 212.6 nm and 845 nm beams due to the different deflection angles experienced by these laser beams at the surfaces of the biconvex lens. This method can eliminate the background signal from the 212.6 nm photolysis. Combined with the VUV FEL, photodissociation of H2S at 122.95 nm was studied successfully. The TOF spectrum was measured and the derived total kinetic energy release spectrum was displayed. The results suggest that the experimental setup is a powerful tool for investigating photodissociation dynamics of molecules in the VUV region which involves the H-atom elimination processes.

Infrared + vacuum ultraviolet two-color ionization spectroscopy of neutral metal complexes based on a tunable vacuum ultraviolet free-electron laser.

This paper describes an experimental technique for studying neutral metal complexes using infrared + vacuum ultraviolet (IR+VUV) two-color ionization spectroscopy based on a tunable VUV free-electron laser (VUV-FEL). The preliminary IR spectroscopy results of mass-selected nickel tetracarbonyl are reported in this work. The results demonstrate that the tunable VUV-FEL light allows the selective ionization of a given neutral cluster free of confinement along with the recording of well-resolved IR spectra. As the ionization energies of many neutral clusters are accessible by a broadly tunable VUV-FEL (50-150 nm) and near-threshold ionization can be readily achieved, the proposed experimental method offers unique possibilities for the size-specific study of a wide variety of confinement-free neutral clusters.

Infrared Spectroscopy of Neutral Water Dimer Based on a Tunable Vacuum Ultraviolet Free Electron Laser

Infrared (IR) spectroscopy provides detailed structural and dynamical information on clusters at the fingerprint level. Herein, we demonstrate the capability of a tunable vacuum ultraviolet free electron laser (VUV-FEL) for selective detection of a wide variety of neutral water clusters and for recording the size-dependent IR spectra. The present technique does not require the presence of an ultraviolet chromophore or a dipole moment and is generally applicable for IR spectroscopy of neutral clusters free from confinement. To show the features of our technique, we report here the IR spectra of neutral water dimer in the OH stretch region, providing benchmarks for theoretical study of the accurate description of hydrogen bonding structures involved in liquid water and ice. Quantum mechanical calculations on a 12-dimensional ab initio potential energy surface are utilized to simulate the anharmonic vibrational spectra of water dimer. These results help to resolve the controversy of the exact vibrational assignment of each band feature of the water dimer.

Intense VUV–xenon-cluster interaction revisited

During the inaugural experiment at FLASH, the first vacuum ultraviolet (VUV) free-electron laser facility, Wabnitz et al. [Nature 420, 482 (2002)] irradiated xenon clusters and sparked a concerted theoretical and experimental effort to understand how dense, finite plasmas behave under intense irradiation. In this work, we revisit this experiment with a model that is based only on well-established atomic processes. We find that the experimental results can be explained by hybrid quantum-classical molecular-dynamics simulations if collisional excitation, recombination, and a sufficiently deep soft-core potential is used. Our recent theoretical model for inverse bremsstrahlung heating (IBH) is used to show that the measured energy absorbed by the cluster in the experiment is well predicted by our model.

Tunable VUV photochemistry using vacuum ultraviolet free electron laser combined with H-atom Rydberg tagging time-of-flight spectroscopy.

In this article, we describe an experimental setup for studying tunable vacuum ultraviolet photochemistry using the H-atom Rydberg tagging time-of-flight technique. In this apparatus, two vacuum ultraviolet laser beams were used: one is generated by using a nonlinear four-wave mixing scheme in a Kr gas cell and fixed at 121.6 nm wavelength to probe the H-atom product through the Lyman α transition and the other beam, produced by a seeded free electron laser facility, can be continuously tunable for photodissociating molecules in the wavelength range of 50-150 nm with extremely high brightness. Preliminary results on the H2O photodissociation in the 4d (000) Rydberg state are reported here. These results suggest that the experimental setup is a powerful tool for investigating photodissociation dynamics in the vacuum ultraviolet region for molecules involving H-atom elimination processes.

Photodissociation dynamics of H2O at 111.5 nm by a vacuum ultraviolet free electron laser.

Photodissociation dynamics of H2O via the F̃ state at 111.5 nm were investigated using the high resolution H-atom Rydberg "tagging" time-of-flight (TOF) technique, in combination with the tunable vacuum ultraviolet free electron laser at the Dalian Coherent Light Source. The product translational energy distributions and angular distributions in both parallel and perpendicular directions were derived from the recorded TOF spectra. Based on these distributions, the quantum state distributions and angular anisotropy parameters of OH (X) and OH (A) products have been determined. For the OH (A) + H channel, highly rotationally excited OH (A) products have been observed. These products are ascribed to a fast direct dissociation on the B̃1A1 state surface after multi-step internal conversions from the initial excited F̃ state to the B̃ state. While for the OH (X) + H channel, very highly rotationally excited OH (X) products with moderate vibrational excitation are revealed and attributed to the dissociation via a nonadiabatic pathway through the well-known two conical intersections between the B̃-state and the X̃-state surfaces.

VUV and X-ray free-electron lasers: The technology and its scientific promise

Currently available, fully coherent (laser) light sources emit radiation only in a limited range of wavelengths in the infrared, visible and near-ultraviolet range, excluding their use in all the measurements needing tunable photons of energy higher than a few eV. Consequentially, the strong scientific need for tunable, coherent radiation sources from the vacuum ultraviolet (VUV) to the X-ray in the femtosecond and picosecond time domain has spurred international research efforts to develop a new generation of research facilities. Laser-driven light sources that use non-linear processes to create very high harmonics and the interaction between an ultra-short laser pulse and an electron bunch in a storage ring are both able to produce radiation pulses in the femtosecond time domain and in the soft EUV and X-ray region, but with a relatively low useful photon flux on the sample. In contrast Free-Electron Lasers (FELs) can produce light pulses with peak brilliance as much as ten orders of magnitude higher than the pulses generated in present third-generation synchrotron light sources and with photon energies ranging from the VUV to the hard X-rays, i.e. from about 10eV (120nm) to 10keV (0.12nm). This manuscript reviews the scientific fields that can be opened or extended by the new techniques along with the progress of FEL physics and the supporting accelerator physics and technology.

Spectrometer for shot-to-shot photon energy characterization in the multi-bunch mode of the free electron laser at Hamburg.

The setup and first results from commissioning of a fast online photon energy spectrometer for the vacuum ultraviolet free electron laser at Hamburg (FLASH) at DESY are presented. With the use of the latest advances in detector development, the presented spectrometer reaches readout frequencies up to 1 MHz. In this paper, we demonstrate the ability to record online photon energy spectra on a shot-to-shot base in the multi-bunch mode of FLASH. Clearly resolved shifts in the mean wavelength over the pulse train as well as shot-to-shot wavelength fluctuations arising from the statistical nature of the photon generating self-amplified spontaneous emission process have been observed. In addition to an online tool for beam calibration and photon diagnostics, the spectrometer enables the determination and selection of spectral data taken with a transparent experiment up front over the photon energy of every shot. This leads to higher spectral resolutions without the loss of efficiency or photon flux by using single-bunch mode or monochromators.

Ultrafast Internal Conversion of Aromatic Molecules Studied by Photoelectron Spectroscopy using Sub-20 fs Laser Pulses

This article describes our recent experimental studies on internal conversion via a conical intersection using photoelectron spectroscopy. Ultrafast S2(ππ*)–S1(nπ*) internal conversion in pyrazine is observed in real time using sub-20 fs deep ultraviolet pulses (264 and 198 nm). While the photoelectron kinetic energy distribution does not exhibit a clear signature of internal conversion, the photoelectron angular anisotropy unambiguously reveals the sudden change of electron configuration upon internal conversion. An explanation is presented as to why these two observables have different sensitivities to internal conversion. The 198 nm probe photon energy is insufficient for covering the entire Franck-Condon envelopes upon photoionization from S2/S1 to D1/D0. A vacuum ultraviolet free electron laser (SCSS) producing 161 nm radiation is employed to solve this problem, while its pulse-to-pulse timing jitter limits the time resolution to about 1 ps. The S2–S1 internal conversion is revisited using the sub-20 fs 159 nm pulse created by filamentation four-wave mixing. Conical intersections between D1(π−1) and D0(n−1) and also between the Rydberg state with a D1 ion core and that with a D0 ion core of pyrazine are studied by He(I) photoelectron spectroscopy, pulsed field ionization photoelectron spectroscopy and one-color resonance-enhanced multiphoton ionization spectroscopy. Finally, ultrafast S2(ππ*)–S1(ππ*) internal conversion in benzene and toluene are compared with pyrazine.

Simulation of cross-correlation method for temporal characterization of VUV free-electron-lasers

The cross-correlation method for temporal characterization is investigated using simulations of the twocolor above threshold ionization (ATI) on He induced by a vacuum ultraviolet (VUV) free-electron laser (FEL) in the presence of an infrared (IR) field. Non-linear dependencies of the sideband structure produced in the two-color ATI process are expressed as a function of IR laser intensity by considering the spatial distributions and temporal jitter of both lasers. The temporal properties of the FEL pulse can be characterized accurately using the cross-correlation method at a low IR laser intensity of ~3 \times 10^{10} W/cm2 but with low cross-correlation signals. When the dynamic range of sidebands is increased to high IR intensity, the accuracy of the cross-correlation method becomes crucially dependent on the actual nonlinear index. An approach of determining this index is proposed here to improve the accuracy of temporal characterizations.

Rate equation for intense core-level photoexcitation and relaxation in metals

A dynamical equation for intense core–valence photoexcitation and collisional relaxation in a metal is derived by combining cluster-model electronic-structure calculations and the equation of motion for density matrices. By invoking the Markov approximation, it can be reduced to a generalized rate equation, where the rate coefficients for collisional and radiative transitions are derived from the cluster Hamiltonian in a self-contained fashion; they incorporate energy-level shifts due to electron–hole interactions as well as modification of dipole transition matrix elements due to induced polarization. Numerical examples are shown for K-edge excitation of lithium metal by a laser pulse with the photon energy of 60 eV and the intensity of 1014 W cm−2. It is found that creation of multiple core holes gives rise to a shift of the absorption edge towards the high-energy side, leading to a reduction of the absorption coefficient within 10 fs timescale. Such an ultrafast switching mechanism may have relevance to recently demonstrated nonlinear transmission of soft x-ray and vacuum ultraviolet free-electron laser pulses through metallic targets.

Time-resolved photoelectron imaging using a femtosecond UV laser and a VUV free-electron laser

A time-resolved photoelectron imaging using a femtosecond ultraviolet (UV) laser and a vacuum UV free-electron laser is presented. Ultrafast internal conversion and intersystem crossing in pyrazine in a supersonic molecular beam were clearly observed in the time profiles of photoioinzation intensity and time-dependent photoelectron images.

Note: Measurement of saturable absorption by intense vacuum ultraviolet free electron laser using fluorescent material

Advances in free electron lasers (FELs) which generate high energy photons are expected to open novel nonlinear optics in the x-ray and vacuum ultraviolet (VUV) regions. In this paper, we report a new method for performing VUV-FEL focusing experiments. A VUV-FEL was focused with Kirkpatrick-Baez optics on a multilayer target, which contains fused silica as a fluorescent material. By measuring the fluorescence, a 5.6x4.9 microm(2) focal spot was observed in situ. Fluorescence was used to measure the saturable absorption of VUV pulses in the tin layer. The transmission increases nonlinearly higher with increasing laser intensity.

Photodissociation of theHeH+ion into excited fragments(n=2,3)by time-dependent methods

The total and partial photodissociation cross sections of the molecular ion ${\text{HeH}}^{+}$ are computed by time-dependent methods for fragmentation into the excited shells $n=1,2,3$ up to a photon energy of 40 eV. ${^{1}\ensuremath{\Sigma}}^{+}$ and $^{1}\ensuremath{\Pi}$ states are considered for parallel and perpendicular transitions for different initial rotational or vibrational excitations. Nonadiabatic radial and rotational couplings are taken into account. The results from coupled-channel equations are compared with the Born-Oppenheimer approximation. A time-dependent calculation with a femtosecond laser pulse is carried out to simulate a recent crossed beam photodissociation imaging experiment with vacuum ultraviolet free-electron laser [H. B. Pedersen et al., Phys. Rev. Lett. 98, 223202 (2007)]. The dominance of photodissociation perpendicular to the photon polarization is confirmed.

New infrared undulator beamline at FLASH

At the vacuum ultraviolet (VUV) free electron laser in Hamburg (FLASH) an infrared (IR) beamline is being built to allow novel pump-and-probe experiments combining coherent IR pulses with the FEL radiation in the VUV spectral range. It will provide useful IR radiation generated by a purpose built undulator over the wavelength range from 200μm to 10μm and possibly even shorter. The commissioning of the beamline has started this summer and first light will be delivered to the experimental hall by autumn 2007. Another important application of the beamline will be electron diagnostics of the longitudinal charge distribution of the electron bunches.

Measurement of static force at liquid helium temperature

The multilayer piezostacks which are integrated into a cold tuning electromechanical system are used for the compensation of the Lorentz force and damping of microphonics. Cold tuning systems are tested in the CHECHIA horizontal test stand and in the vacuum ultraviolet free electron laser VUV-FEL, both built at DESY-Hamburg. One of the most important issues for the used active element's lifetime is a correct initial preloading force. The commonly used method for measuring preload is based on a strain gauge and requires an additional sensor and wiring. The authors propose an alternative method where the piezostacks are used as force sensors. More precisely, the capacitance and the impedance change of the piezostacks were investigated. The resonance peaks, which are visible on the impedance versus frequency curve, shift when the static force is applied to piezostacks. Moreover, the value of the piezostacks capacitance increases with applied static force. A measurement performed at room and at LHe temperature (T < 4.2 K) showed that this behaviour (frequency shift and capacitance increase) might be used for the precise measurement of static force in the temperature range 1.8 K–300 K. Using this method it is possible to estimate in situ the preload force applied to the piezoelectric element.

Performance of the monochromator beamline at FLASH

The performance of the high-resolution monochromator at FLASH, the vacuum ultra-violet free-electron laser at DESY in Hamburg, was investigated. Using different techniques we measured the relative and absolute transmission of the monochromator beamline for FLASH radiation in the fundamental and higher (up to third) harmonics. The focal spot size of the soft x-ray beam at the output of the beamline was determined as well. In addition, a new way of acquiring the resolving power of the monochromator is discussed. This method has also been applied to calibrate the energy scale of the monochromator system with an accuracy of 5 meV at 48 eV photon energy.

Space-time characterization of laser plasma interactions in the warm dense matter regime

Laser plasma interaction experiments have been performed using an fs Titanium Sapphire laser. Plasmas have been generated from planar PMMA targets using single laser pulses with 3.3 mJ pulse energy, 50 fs pulse duration at 800 nm wavelength. The electron density distributions of the plasmas in different delay times have been characterized by means of Nomarski Interferometry. Experimental data were compared with hydrodynamic simulation. First results to characterize the plasma density and temperature as a function of space and time are obtained. This work aims to generate plasmas in the warm dense matter (WDM) regime at near solid-density in an ultra-fast laser target interaction process. Plasmas under these conditions can serve as targets to develop X-ray Thomson scattering as a plasma diagnostic tool, e.g., using the Vacuum ultraviolet (VUV) free-electron laser (FLASH) at Dentsches Elektronen-Synchrotron (DESY) Hamburg.