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Physical chemistry, chemical physics 24, 23096 - 23105 (2022). doi:10.1039/D2CP02252D special issue: "Ions, electrons, coincidences and dynamics: Festschrift for John H.D. Eland", We investigated the dissociation of dications and trications of three polycyclic aromatic hydrocarbons (PAHs), fluorene, phenanthrene, and pyrene. PAHs are a family of molecules ubiquitous in space and involved in much of the chemistry of the interstellar medium. Ions are formed by ionization with 30.3 nm extreme ultraviolet (XUV) photons, and their velocity map images are recorded using a PImMS multi-mass imaging sensor. Application of recoil-frame covariance analysis allows the total kinetic energy release (TKER) associated with multiple fragmentation channels to be determined to high precision. Experimental measurements are supported by Born-Oppenheimer molecular dynamics (BOMD) molecular dynamics simulations., Published by RSC Publ., Cambridge

New clinical radiotherapy dosimetry systems need comprehensive demonstration of measurement quality. Practicality and reliability are other important aspects for clinical dosimeters. In this work the performance of an optical CT scanner for true 3D dosimetry is assessed using a radiochromic gel dosimeter. The fluid-less scanner utilised dual lasers to avoid the necessity for pre-irradiation scans and give greater robustness of image quality, enhancing practicality. Calibration methods using both cuvettes and reconstructed volumes were developed. Dosimetric accuracy was similar for dual and single wavelength measurements, except that cuvette calibration reliability was reduced for dual wavelength without pre-irradiation scanning. Detailed performance parameters were specified for the dosimetry system indicating the suitability for clinical use. The most significant limitations of the system were due to the gel dosimeter rather than the optical CT scanner. Quality assurance guidelines were developed to maintain dosimetry system performance in routine use.

Extreme ultraviolet (XUV) and X-ray free-electron lasers enable new scientific opportunities. Their ultra-intense coherent femtosecond pulses give unprecedented access to the structure of undepositable nanoscale objects and to transient states of highly excited matter. In order to probe the ultrafast complex light-induced dynamics on the relevant time scales, the multi-purpose end-station CAMP at the free-electron laser FLASH has been complemented by the novel multilayer-mirror-based split-and-delay unit DESC (DElay Stage for CAMP) for time-resolved experiments. XUV double-pulses with delays adjustable from zero femtoseconds up to 650 picoseconds are generated by reflecting under near-normal incidence, exceeding the time range accessible with existing XUV split-and-delay units. Procedures to establish temporal and spatial overlap of the two pulses in CAMP are presented, with emphasis on the optimization of the spatial overlap at long time-delays via time-dependent features, for example in ion spectra of atomic clusters.

Synopsis In the interstellar medium polycyclic aromatic hydrocarbon molecules (PAH) are exposed to strong ionizing radation leading to complex organic photochemistry. We investigated these ultrafast fragmentation reactions after ionization of the PAHs phenanthrene, fluorene and pyrene at a wavelength of 30.3 nm using pump probe spectroscopy at a free electron laser. We observe double ionization and afterwards hydrogen abstraction and acetylene loss with characteristic time scales for the reaction processes below one hundred femtoseconds.

Laser-based higher-order harmonic generation has been investigated extensively in the past two decades. The current manuscript deals with the high harmonic generation (HHG) outputs from a gas-filled waveguide when using mixtures of two rare gases (Ar and Ne) as nonlinear media. We find that the efficiency of the HHG process can be optimized by changing the pressure or alternatively the mixing ratio of the two gases. This is attributed to the fact that both of these parameters have an effect on the phase-matching in the waveguide. These observations are especially useful when phase matching in a gas jet is concerned, where the absolute local pressure of the gas media cannot be controlled as readily as in a capillary-based HHG setup.

Three dimensional dosimetry by optical CT readout of radiosensitive gels or solids has previously been indicated as a solution for measurement of radiotherapy 3D dose distributions. The clinical uptake of these dosimetry methods has been limited, partly due to impracticalities of the optical readout such as the expertise and labour required for refractive index fluid matching. In this work a fast laser beam optical CT scanner is described, featuring fluid-less and dual wavelength operation. A second laser with a different wavelength is used to provide an alternative reference scan to the commonly used pre-irradiation scan. Transmission data for both wavelengths is effectively acquired simultaneously, giving a single scan process. Together with the elimination of refractive index fluid matching issues, scanning practicality is substantially improved. Image quality and quantitative accuracy were assessed for both dual and single wavelength methods. The dual wavelength scan technique gave improvements in uniformity of reconstructed optical attenuation coefficients in the sample 3D volume. This was due to a reduction of artefacts caused by scan to scan changes. Optical attenuation measurement accuracy was similar for both dual and single wavelength modes of operation. These results established the basis for further work on dosimetric performance.

Optical CT scanners for a 3D readout of externally irradiated radiosensitive hydrogels currently require the use of a refractive index (RI) matching liquid bath to obtain suitable optical ray paths through the gel sample to the detector. The requirement for a RI matching liquid bath has been negated by the design of a plastic cylindrical gel container that provides parallel beam geometry through the gel sample for the majority of the projection. The design method can be used for various hydrogels. Preliminary test results for the prototype laser beam scanner with ferrous xylenol-orange gel show geometric distortion of 0.2 mm maximum, spatial resolution limited to beam spot size of about 0.4 mm and 0.8% noise (1 SD) for a uniform irradiation. Reconstruction of a star pattern irradiated through the cylinder walls demonstrates the suitability for external beam applications. The extremely simple and cost-effective construction of this optical CT scanner, together with the simplicity of scanning gel samples without RI matching fluid increases the feasibility of using 3D gel dosimetry for clinical external beam dose verifications. Refereed/Peer-reviewed