Time-resolved site-selective imaging of predissociation and charge transfer dynamics: The CH3I B-band

The predissociation dynamics of the 6s (B2E) Rydberg state of gas-phase CH3I were investigated by time-resolved Coulomb-explosion imaging using extreme ultraviolet (XUV) free-electron laser pulses. Inner-shell ionization at the iodine 4d edge was utilized to provide a site-specific probe of the ensuing dynamics. The combination of a velocity-map imaging (VMI) spectrometer coupled with the pixel imaging mass spectrometry (PImMS) camera permitted three-dimensional ionic fragment momenta to be recorded simultaneously for a wide range of iodine charge states. In accord with previous studies, initial excitation at 201.2 nm results in internal conversion and subsequent dissociation on the lower-lying A-state surface on a picosecond time scale. Examination of the time-dependent yield of low kinetic energy iodine fragments yields mechanistic insights into the predissociation and subsequent charge transfer following multiple ionization of the iodine products. The effect of charge transfer was observed through differing delay-dependencies of the various iodine charge states, from which critical internuclear distances for charge transfer could be inferred and compared to a classical over-the-barrier model. Time-dependent photofragment angular anisotropy parameters were extracted from the central slice of the Newton sphere, without Abel inversion, and highlight the effect of rotation of the parent molecule before dissociation, as observed in previous © 2020 The Author(s). Published by IOP Publishing Ltd Printed in the U

Simulation of Optical Transport Beamlines for High-quality Optical Beams for Accelerator Applications

High-quality optical beams play already an important role in the field of particle accelerators which will most probably become even more prominent in the view of laser-driven particle accelerators. Nowadays, optical transport systems are needed for particle generation in photo injectors, for particle acceleration in laser-driven plasma wakefield accelerators, for particle beam diagnostics such as synchrotron radiation monitoring systems, or for particle manipulation schemes e.g. for external seeding of free-electron lasers. For the latter case, also the photon beam transport to the user end-stations requires dedicated optical transport system. The utilized wavelengths range from the hard x-ray up to the far-infrared spectral range. Parameters like surface quality, polarization effects, damage thresholds in- and out-of-vacuum, mechanical stability, dispersion effect etc. need to be studied for the variaty of applications. Here, we present the simulation results of the optical transport beamline for the seeding setup at FLASH and give a comparision to our measurement results

Indirect Measurements of NIR and UV Ultrashort Seed Laser Pulses Using a Transverse Deflecting RF-structure

Seeding of free-electron lasers (FELs) using external coherent optical pulses recently became an area of interest as users demand spectrally and temporally coherent FEL radiation which is not achievable in traditional self-amplified spontaneous emission operation mode. Since temporal and spectral properties of the seed laser pulses are directly imprinted on the electron bunch, a proper characterization of these seed pulses is needed. However, the lack of any measurement technique capable of characterizing ultrashort seed laser pulses at the laser-electron interaction region is a primary drawback. In thispaper we report indirect measurements of seed laser pulses in an undulator section using a transverse deflecting RF-structure (TDS) at the free-electron laser FLASH at DESY. Temporally chirped and unchirped seed pulse length measurements will be compared with second-harmonic generation frequency-resolved optical gating measurements and theoretical simulations. Using this technique we will demonstrate that pulse artifacts such as pre- and post-pulses in the seed pulse in the femtosecond and picosecond timescales can be identified without any temporal ambiguity

Indirect Measurements of NIR and UV Ultrashort Seed Laser Pulses Using a Transverse Deflecting RF-Structure

Seeding of free-electron lasers (FELs) using external coherent optical pulses recently became an area of interest as users demand spectrally and temporally coherent FEL radiation which is not achievable in traditional self-amplified spontaneous emission operation mode. Since temporal and spectral properties of the seed laser pulses are directly imprinted on the electron bunch, a proper characterization of these seed pulses is needed. However, the lack of any measurement technique capable of characterizing ultrashort seed laser pulses at the laser-electron interaction region is a primary drawback. In thispaper we report indirect measurements of seed laser pulses in an undulator section using a transverse deflecting RF-structure (TDS) at the free-electron laser FLASH at DESY. Temporally chirped and unchirped seed pulse length measurements will be compared with second-harmonic generation frequency-resolved optical gating measurements and theoretical simulations. Using this technique we will demonstrate that pulse artifacts such as pre- and post-pulses in the seed pulse in the femtosecond and picosecond timescales can be identified without any temporal ambiguity

Mapping few-femtosecond slices of ultra-relativistic electron bunches

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

Extraction of the Longitudinal Profile of the Transverse Emittance From Single-Shot RF Deflector Measurements at sFLASH

The gain length of the free-electron laser (FEL) process strongly depends on the slice energy spread, slice emittance, and current of the electron bunch. At an FEL with only moderately compressed electron bunches, the slice energy spread is mainly determined by the compression process. In this regime, single-shot measurements using a transverse deflecting rf cavity enable the extraction of the longitudinal profile of the transverse emittance. At the free-electron laser FLASH at DESY, this technique was used to determine the slice properties of the electron bunch set up for seeded operation in the sFLASH experiment. Thereby, the performance of the seeded FEL process as a function of laser-electron timing can be predicted from these slice properties with the semi-analytical Ming-Xie model where only confined fractions of the electron bunch are stimulated to lase. The prediction is well in line with the FEL peak power observed during an experimental laser-electron timing scan. The power profiles of the FEL pulses were reconstructed from the longitudinal phase-space measurements of the seeded electron bunch that was measured with the rf deflector

Operation of a seeded XUV free electron laser at DESY with high-gain harmonic generation seeding

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

Probing electron and hole co-localization by resonant four-wave mixing in the extreme-ultraviolet

The extension of nonlinear spectroscopic techniques into the x-ray domain is in its infancy but holds the promise to provide unique insight into the dynamics of charges in photoexcited processes, which are of fundamental as well as applied interest. We report on the observation of a third order nonlinear process in lithium fluoride at a free-electron laser. Exploring the yield of four wave mixing (FWM) in resonance with transitions to strongly localized core exciton states vs. delocalized Bloch states, we find resonant FWM to be a sensitive probe for the degree of charge localization: substantial sum- and difference-frequency generation is observed exclusively when in a one- or three-photon resonance with a LiF core exciton, with a dipole forbidden transition affecting details of the nonlinear response. Our reflection-geometry-based approach to detect FWM signals enables the study of a wide variety of condensed matter sample systems, provides atomic selectivity via resonant transitions and can be easily scaled to shorter wavelengths at free electron x-ray lasers

Free-Electron Laser Multiplex Driven by a Superconducting Linear Accelerator

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

Probing electron and hole co-localization by resonant four-wave mixing in the extreme-ultraviolet

The extension of nonlinear spectroscopic techniques into the x-ray domain is in its infancy but holds the promise to provide unique insight into the dynamics of charges in photoexcited processes, which are of fundamental as well as applied interest. We report on the observation of a third order nonlinear process in lithium fluoride at a free-electron laser. Exploring the yield of four wave mixing (FWM) in resonance with transitions to strongly localized core exciton states vs. delocalized Bloch states, we find resonant FWM to be a sensitive probe for the degree of charge localization: substantial sum- and difference-frequency generation is observed exclusively when in a one- or three-photon resonance with a LiF core exciton, with a dipole forbidden transition affecting details of the nonlinear response. Our reflection-geometry-based approach to detect FWM signals enables the study of a wide variety of condensed matter sample systems, provides atomic selectivity via resonant transitions and can be easily scaled to shorter wavelengths at free electron x-ray lasers