The SwissFEL soft X-ray free-electron laser beamline: Athos.

The SwissFEL soft X-ray free-electron laser (FEL) beamline Athos will be ready for user operation in 2021. Its design includes a novel layout of alternating magnetic chicanes and short undulator segments. Together with the APPLE X architecture of undulators, the Athos branch can be operated in different modes producing FEL beams with unique characteristics ranging from attosecond pulse length to high-power modes. Further space has been reserved for upgrades including modulators and an external seeding laser for better timing control. All of these schemes rely on state-of-the-art technologies described in this overview. The optical transport line distributing the FEL beam to the experimental stations was designed with the whole range of beam parameters in mind. Currently two experimental stations, one for condensed matter and quantum materials research and a second one for atomic, molecular and optical physics, chemical sciences and ultrafast single-particle imaging, are being laid out such that they can profit from the unique soft X-ray pulses produced in the Athos branch in an optimal way.

Pulse-shaping assisted multidimensional coherent electronic spectroscopy.

Understanding nuclear and electronic dynamics of molecular systems has advanced considerably by probing their nonlinear responses with a suitable sequence of pulses. Moreover, the ability to control crucial parameters of the excitation pulses, such as duration, sequence, frequency, polarization, slowly varying envelope, or carrier phase, has led to a variety of advanced time-resolved spectroscopic methodologies. Recently, two-dimensional electronic spectroscopy with ultrashort pulses has become a more and more popular tool since it allows to obtain information on energy and coherence transfer phenomena, line broadening mechanisms, or the presence of quantum coherences in molecular complexes. Here, we present a high fidelity two-dimensional electronic spectroscopy setup designed for molecular systems in solution. It incorporates the versatility of pulse-shaping methods to achieve full control on the amplitude and phase of the individual exciting and probing pulses. Selective and precise amplitude- and phase-modulation is shown and applied to investigate electronic dynamics in several reference molecular systems.

Metrology for advanced radiotherapy using particle beams with ultra-high dose rates.

Dosimetry of ultra-high dose rate beams is one of the critical components which is required for safe implementation of FLASH radiotherapy (RT) into clinical practice. In the past years several national and international programmes have emerged with the aim to address some of the needs that are required for translation of this modality to clinics. These involve the establishment of dosimetry standards as well as the validation of protocols and dosimetry procedures. This review provides an overview of recent developments in the field of dosimetry for FLASH RT, with particular focus on primary and secondary standard instruments, and provides a brief outlook on the future work which is required to enable clinical implementation of FLASH RT.

Charge collection efficiency of commercially available parallel-plate ionisation chambers in ultra-high dose-per-pulse electron beams.

Objective. This investigation aims to experimentally determine the charge collection efficiency (CCE) of six commercially available parallel-plate ionisation chamber (PPIC) models in ultra-high dose-per-pulse (UHDPP) electron beams.Approach. The CCE of 22 PPICs has been measured in UHDPP electron beams at the National Metrology Institution of Germany (PTB). The CCE was determined for a dose per pulse (DPP) range between 0.1 and 6.4 Gy (pulse duration of 2.5µs). The results obtained with the different PPICs were compared to evaluate the reproducibility, intra- and inter-model variation, and the performance of a CCE empirical model.Main results. The intra-model variation was, on average, 4.0%, which is more than three times the total combined relative standard uncertainty and was found to be greater at higher DPP (up to 20%). The inter-model variation for the PPIC with 2 mm electrode spacing, which was found to be, on average, 10%, was also significant compared to the relative uncertainty and the intra-model variation. The observed CCE variation could not be explained only by the expected deviation of the electrode spacing from the nominal value within the manufacturing tolerance. It should also be noted that a substantial polarity effect, between 0.914(5) and 1.201(3), was observed, and significant intra- and inter-model variation was observed on this effect.Significance. For research and pre-clinical study, the commercially available PPIC with a well-known CCE (directly measured for the specific chamber) and with a small electrode spacing could be used for relative and absolute dosimetry with a lower-limit uncertainty of 1.6% (k= 1) in the best case. However, to use a PPIC as a secondary standard in UHDPP electron beams for clinical purposes would require new model development to reduce the ion recombination, the polarity effect, and the total standard uncertainty on the dose measurement.

Influence of finite spatial resolution on single- and double-pass femtosecond pulse shapers.

We investigate the influence of the finite spatial resolution of a typical 4f pulse-shaping setup in a single- and double-pass configuration on the shaped waveforms. Specifically, we calculate and measure the space-frequency distribution at the focal plane of a lens following the shaping setup and show that steep amplitude or phase jumps, as they appear with pixelated spatial light modulators, are affected by a finite spatial resolution.

Ultrafast electronic and vibrational relaxations in mixed-ligand dithione-dithiolato Ni, Pd, and Pt complexes.

Ultrafast excited-state dynamics of planar Pt, Pd, and Ni dithione-dithiolato complexes were investigated by transient absorption spectroscopy on the femtosecond-picosecond timescale. All studied complexes show a common photobehaviour, although individual kinetics parameters and quantum yields vary with the metal, the dithione ligand and, namely the solvent (DMF, MeCN). Laser pulse irradiation at 800 nm populates the lowest singlet excited state of a dithiolato → dithione charge transfer character, (1)LL'CT. The optically excited state undergoes a solvation-driven sub-picosecond electronic relaxation that enhances the dithione/dithiolato charge separation. The (1)LL'CT state decays with a 1.9-4.5 ps lifetime by two simultaneous pathways: intersystem crossing (ISC) to the lowest triplet state (3)LL'CT and non-radiative decay to the ground state. ISC occurs on a ∼6 ps timescale, virtually independent of the metal, whereas the rate of the non-radiative decay to the ground state decreases on going from Ni (2 ps) to Pd (3 ps) and Pt (∼10 ps). (3)LL'CT is initially formed as a vibrationally excited state. Its equilibration (cooling) takes place on a picosecond timescale and is accompanied by a competitive decay to the ground state. Equilibrated (3)LL'CT is populated with a quantum yield of less than 50%, depending on the metal: Pt > Pd > Ni. (3)LL'CT is long-lived for Pt and Pd (≫500 ps) and short-lived for Ni (∼15 ps). Some of the investigated complexes also exhibit spectral changes due to vibrational cooling of the singlet (2-3 ps, depending on the solvent). Rotational diffusion occurs with lifetimes in the 120-200 ps range. Changing the dithione (Bz2pipdt/(i)Pr2pipdt) as well as dithiolate/diselenolate (dmit/dsit) ligands has only small effects on the photobehavior. It is proposed that the investigated dithione-dithiolato complexes could act as photooxidants (*E(o) ≈ +1.2 V vs. NHE) utilizing their lowest excited singlet ((1)LL'CT), provided that the excited-state electron transfer is ultrafast, competitive with the picosecond decay. On the other hand, the efficiency of any triplet-based processes would be severely limited by the low quantum yield of the triplet population.