Comment on "Cumulant mapping as the basis of multi-dimensional spectrometry" by Leszek J. Frasinski, Phys. Chem. Chem. Phys., 2022, 24, 20776-20787.

I state a general formula for the n-variate joint cumulant of the first order and prove that it satisfies the desired properties listed in Section 3.3 of Phys. Chem. Chem. Phys., 2022, 24, 20776-20787.

Indication of 310-Helix Structure in Gas-Phase Neutral Pentaalanine.

We investigate the gas-phase structure of the neutral pentaalanine peptide. The IR spectrum in the 340-1820 cm-1 frequency range is obtained by employing supersonic jet cooling, infrared multiphoton dissociation, and vacuum-ultraviolet action spectroscopy. Comparison with quantum chemical spectral calculations suggests that the molecule assumes multiple stable conformations, mainly of two structure types. In the most stable conformation theoretically found, the N-terminus forms a C5 ring and the backbone resembles that of an 310-helix with two ß-turns. Additionally, the conformational preferences of pentaalanine have been evaluated using Born-Oppenheimer molecular dynamics, showing that a nonzero simulation time step causes a systematic frequency shift.

IRMPD Spectroscopy of Homo- and Heterochiral Asparagine Proton-Bound Dimers in the Gas Phase.

We investigate gas-phase structures of homo- and heterochiral asparagine proton-bound dimers with infrared multiphoton dissociation (IRMPD) spectroscopy and quantum-chemical calculations. Their IRMPD spectra are recorded at room temperature in the range of 500-1875 and 3000-3600 cm-1. Both varieties of asparagine dimers are found to be charge-solvated based on their IRMPD spectra. The location of the principal intramolecular H-bond is discussed in light of harmonic frequency analyses using the B3LYP functional with GD3BJ empirical dispersion. Contrary to theoretical analyses, the two spectra are very similar.

Structure of Proton-Bound Methionine and Tryptophan Dimers in the Gas Phase Investigated with IRMPD Spectroscopy and Quantum Chemical Calculations.

The structures of three proton-bound dimers (Met2H+, MetTrpH+, and Trp2H+) are investigated in the gas phase with infrared multiple photon disassociation (IRMPD) spectroscopy in combination with quantum chemical calculations. Their IRMPD spectra in the range of 600-1850 cm-1 are obtained experimentally using an FT-ICR mass spectrometer and the CLIO free electron laser as an IR light source. The most abundant conformers are elucidated by comparing the IRMPD spectra with harmonic frequencies obtained at the B3LYP-GD3BJ/6-311++G** level of theory. Discrepancies between the experimental and theoretical data in the region of 1500-1700 cm-1 are attributed to the anharmonicity of the amino bending modes. We confirm the result of a previous IRMPD study that the structure of gas-phase Trp2H+ is charge-solvated but find that there are more stable structures than originally reported (Feng, R.; Yin, H.; Kong, X. Rapid Commun. Mass Spectrom. 2016, 30, 24-28). In addition, gas-phase Met2H+ and MetTrpH+ have been revealed to have charge-solvated structures. For all three dimers, the most stable conformer is found to be of type A. The spectrum of Met2H+, however, cannot be explained without some abundance of type B charge-solvated conformers as well as salt-bridged structures.

Commissioning and first-year operational results of the MAX†IV 3†GeV ring.

The MAX IV 3 GeV electron storage ring in Lund, Sweden, is the first of a new generation of light sources to make use of the multibend-achromat lattice (MBA) to achieve ultralow emitance and hence ultrahigh brightness and transverse coherence. The conceptual basis of the MAX IV 3 GeV ring project combines a robust lattice design with a number of innovative engineering choices: compact, multifunctional magnet blocks, narrow low-conductance NEG-coated copper vacuum chambers and a 100 MHz radio-frequency system with passively operated third-harmonic cavities for bunch lengthening. In this paper, commissioning and first-year operational results of the MAX IV 3 GeV ring are presented, highlighting those aspects that are believed to be most relevant for future MBA-based storage rings. The commissioning experience of the MAX IV 3 GeV ring offers in this way an opportunity for validation of concepts that are likely to be essential ingredients of future diffraction-limited light sources.

The MAX†IV storage ring project.

The MAX IV facility, currently under construction in Lund, Sweden, features two electron storage rings operated at 3 GeV and 1.5 GeV and optimized for the hard X-ray and soft X-ray/VUV spectral ranges, respectively. A 3 GeV linear accelerator serves as a full-energy injector into both rings as well as a driver for a short-pulse facility, in which undulators produce X-ray pulses as short as 100 fs. The 3 GeV ring employs a multibend achromat (MBA) lattice to achieve, in a relatively short circumference of 528 m, a bare lattice emittance of 0.33 nm rad, which reduces to 0.2 nm rad as insertion devices are added. The engineering implementation of the MBA lattice raises several technological problems. The large number of strong magnets per achromat calls for a compact design featuring small-gap combined-function magnets grouped into cells and sharing a common iron yoke. The small apertures lead to a low-conductance vacuum chamber design that relies on the chamber itself as a distributed copper absorber for the heat deposited by synchrotron radiation, while non-evaporable getter (NEG) coating provides for reduced photodesorption yields and distributed pumping. Finally, a low main frequency (100 MHz) is chosen for the RF system yielding long bunches, which are further elongated by passively operated third-harmonic Landau cavities, thus alleviating collective effects, both coherent (e.g. resistive wall instabilities) and incoherent (intrabeam scattering). In this paper, we focus on the MAX IV 3 GeV ring and present the lattice design as well as the engineering solutions to the challenges inherent to such a design. As the first realisation of a light source based on the MBA concept, the MAX IV 3 GeV ring offers an opportunity for validation of concepts that are likely to be essential ingredients of future diffraction-limited light sources.