Following excited-state chemical shifts in molecular ultrafast x-ray photoelectron spectroscopy

Mayer, D. T.; Lever, Fabiano; Picconi, David; Metje, Jan; Ališauskas, Skirmantas; Calegari, Francesca; Düsterer, S.; Ehlert, Christopher; Feifel, Raimund; Niebuhr, Mario; Manschwetus, Bastian; Kuhlmann, Marion; Mazza, Tommaso; Robinson, M. S.; Squibb, Richard J.; Trabattoni, Andrea; Wallner, M.; Saalfrank, Peter; Wolf, Thomas; Gühr, Markus

doi:10.1038/s41467-021-27908-y

Cited by 47 publications

(34 citation statements)

References 56 publications

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“…In the following sections, we compare experimental results with 3D simulations performed for a chirped electron beam. The energy chirp along the lasing fraction of the bunch was set to 150 keV/fs (Figure 2), leading to a spectral width of about 1% for the XUV pulse, in agreement with several spectral measurements performed at FLASH [5,[22][23][24]. The chirp in the electron bunch leads to a chirp of 30 meV/fs in the 13.5 nm XUV pulse, or, expressed as second-order dispersion, it yields a value of 25 fs 2 , which is comparable to the measurements described in Ref.…”

Section: Sase Fel Amplification Processsupporting

confidence: 80%

FEL Pulse Duration Evolution along Undulators at FLASH

Bidhendi¹,

Macias²,

Ivanov³

et al. 2022

Applied Sciences

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Self-amplified spontaneous-emission (SASE) free-electron lasers (FELs) deliver ultrashort pulses with femtosecond durations. Due to the fluctuating nature of the radiation properties of SASE FELs, characterizing FEL pulses on a single-shot basis is necessary. Therefore, we use terahertz streaking to characterize the temporal properties of ultrashort extreme ultraviolet pulses from the free-electron laser in Hamburg (FLASH). In this study, pulse duration as well as pulse energy are measured in a wavelength range from 8 to 34 nm as functions of undulators contributing to the lasing process. The results are compared to one-dimensional and three-dimensional, time-dependent FEL simulations.

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Section: Sase Fel Amplification Processsupporting

confidence: 80%

FEL Pulse Duration Evolution along Undulators at FLASH

Bidhendi¹,

Macias²,

Ivanov³

et al. 2022

Applied Sciences

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“…Experimental data confirmed that a soft X-ray FEL source is very effective in timeresolved PECD for studying dissociating chiral cations [34] and for time-resolved photoelectron spectroscopy (XPS) applied to site-specific analysis suitable to distinguish the contributions of different atoms of the same chemical element simultaneously probed [35]. Following these promising results, Faccialà et al investigated at the C K-edge the chirality of fenchone, a prototypical organic molecule, using both time-resolved XPS and PECD [36].…”

Section: -3 the Electronic Structure Of Photo-excited Chiral Moleculesmentioning

confidence: 69%

Progress and Perspectives of Spectroscopic Studies at Carbon K-edge Using Novel Soft X-ray Pulsed Sources

Ebrahimpour¹,

Coreno²,

Giannessi³

et al. 2022

Preprint

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The development of novel coherent and brilliant sources, such as soft X-ray Free Electron Laser (FEL) and High Harmonic Generation (HHG) enables new ultrafast analysis of the electronic and structural dynamics of a wide variety of materials. Soft X-ray FEL delivers high brilliance beams with short pulse duration, high spatial coherence and photon energy tunability. In com-parison with FELs, HHG X-ray sources are characterized by a wide spectral bandwidth and few to sub-femtosecond pulses. The approach will lead to time-resolved reconstruction of molecular dynamics, shedding light on different photochemical pathways. The high peak brilliance of soft X-ray FELs facilitates investigations in nonlinear regime, while the broader spectral bandwidth of the HHG sources may provide the simultaneous probing of multiple components. Significant technical breakthroughs in these novel sources are under way to improve brilliance, pulse dura-tion, and to control spectral bandwidth, spot size, and energy resolution. Therefore, in the next few years, the new generation of soft X-ray sources combined with novel experimental tech-niques, new detectors, and computing capabilities will allow the study of several extremely-fast dynamics, such as vibronic dynamics. In the present review, we shortly discuss recent devel-opments in experiments, performed with soft X-ray FELs and HHG sources, operating near car-bon K-absorption edge, being a key atomic component in biosystems and soft materials. Differ-ent spectroscopy methods such as time-resolved pump-probe techniques, nonlinear spectrosco-pies and photoelectron spectroscopy studies have been addressed in an attempt of a better un-derstanding of fundamental physico-chemical processes

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“… 10–12 A prerequisite for any control of electronic and nuclear dynamics toward specific molecular reaction pathways is a detailed analysis of structural properties, when the molecule is driven out of equilibrium and here, in particular, the analysis of the time-dependent electronic structure defining the potential energy landscape in which the nuclei move. 13 X-ray photoelectron spectroscopy (XPS) is a well-established technique sensitive to the electronic structure. Applied in a time-resolved pump-probe scheme, it allows us to unambiguously monitor electronic coherences and vibronic coupling long before fragmentation sets in, i.e., while the electronic wave packet propagates.…”

Section: Introductionmentioning

confidence: 99%

Charge-induced chemical dynamics in glycine probed with time-resolved Auger electron spectroscopy

Schwickert

Ruberti

Kolorenč

et al. 2022

Structural Dynamics

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In the present contribution, we use x-rays to monitor charge-induced chemical dynamics in the photoionized amino acid glycine with femtosecond time resolution. The outgoing photoelectron leaves behind the cation in a coherent superposition of quantum mechanical eigenstates. Delayed x-ray pulses track the induced coherence through resonant x-ray absorption that induces Auger decay. Temporal modulation of the Auger electron signal correlated with specific ions is observed, which is governed by the initial electronic coherence and subsequent vibronic coupling to nuclear degrees of freedom. In the time-resolved x-ray absorption measurement, we monitor the time-frequency spectra of the resulting many-body quantum wave packets for a period of 175 fs along different reaction coordinates. Our experiment proves that by measuring specific fragments associated with the glycine dication as a function of the pump-probe delay, one can selectively probe electronic coherences at early times associated with a few distinguishable components of the broad electronic wave packet created initially by the pump pulse in the cation. The corresponding coherent superpositions formed by subsets of electronic eigenstates and evolving along parallel dynamical pathways show different phases and time periods in the range of [Formula: see text] and [Formula: see text] fs. Furthermore, for long delays, the data allow us to pinpoint the driving vibrational modes of chemical dynamics mediating charge-induced bond cleavage along different reaction coordinates.

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Following excited-state chemical shifts in molecular ultrafast x-ray photoelectron spectroscopy

Cited by 47 publications

References 56 publications

FEL Pulse Duration Evolution along Undulators at FLASH

FEL Pulse Duration Evolution along Undulators at FLASH

Progress and Perspectives of Spectroscopic Studies at Carbon K-edge Using Novel Soft X-ray Pulsed Sources

Charge-induced chemical dynamics in glycine probed with time-resolved Auger electron spectroscopy

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