A5071983526- Spectroscopy and Quantum Chemical Studies
- Advanced Chemical Physics Studies
- Laser-Matter Interactions and Applications
- Mass Spectrometry Techniques and Applications
- Spectroscopy and Laser Applications
- Photochemistry and Electron Transfer Studies
- Electron and X-Ray Spectroscopy Techniques
- Quantum, superfluid, helium dynamics
- X-ray Spectroscopy and Fluorescence Analysis
- Nuclear Physics and Applications
- Radiation Therapy and Dosimetry
- Luminescence Properties of Advanced Materials
- Atomic and Molecular Physics
ETH Zurich
2020-2022
Attosecond science in liquid phase Many physical properties of water remain unresolved due to the very fast dynamics involved phase. Using attosecond time-resolved photoelectron spectroscopy, Jordan et al. found that photoemission electrons from shows a time delay about 50 70 attoseconds compared with gas This difference was attributed solvation effects and validated by analysis various contributions measured delays using theoretical simulations clusters different sizes. Science , this issue p. 974
We report the first observation of intermolecular Coulombic decay (ICD) in liquid water following inner-valence ionization. By combining a monochromatized tabletop high-harmonic source with microjet, we record electron-electron coincidence spectra at two photon energies that identify ICD electrons, together photoelectrons originating from 2a_{1} band water. Our results confirm importance as low-energy electrons bulk and provide quantitative for modeling velocity distribution slow are thought...
The ionization energy of liquid water is one its most fundamental properties, an important benchmark for first-principles electronic-structure calculations and a crucial reference in the growing field liquid-phase photoelectron spectroscopy. Despite this significance, consensus on value appears to be missing literature. Therefore, we use monochromatized high-harmonic light source perform detailed measurements presence tunable bias voltage applied jet. Our results suggest that simple method...
This study reports fully angle- and state-resolved measurement of time delays in molecular photoionization.
Mean free paths of low-energy electrons in liquid water are importance for modeling many physicochemical processes, but neither theoretical predictions nor experimental results have converged these parameters. We therefore introduce an approach to determine elastic and inelastic mean (EMFP, IMFP) based on data. show that ab initio calculations electron scattering with clusters converge cluster size, thus providing access condensed-phase scattering. The used Monte Carlo simulations extract...
We present the experimental observation of two-center interference in ionization time delays Kr_{2}. Using attosecond electron-ion-coincidence spectroscopy, we simultaneously measure photoionization krypton monomer and dimer. The relative delay is found to oscillate as a function electron kinetic energy, an effect that traced back constructive destructive photoelectron wave packets are emitted or scattered from two atomic centers. Our interpretation results supported by solving...
We report the first systematic photoelectron measurements of three outer-valence bands liquid water as a function ionizing photon energy in near-threshold region. use extreme-ultraviolet (XUV) radiation tunable between ∼17.1 and 35.6 eV, obtained through monochromatization high-harmonic source. show that absolute values apparent vertical ionization energies their respective peak widths decreasing trend magnitudes with increasing close to threshold. find observed effects do not only depend on...
Attosecond photoionization delays have mostly been interpreted within the single-particle approximation of multi-electron systems. The strong electron correlation between channels associated with 3p and 3s orbitals argon presents an interesting arena where this breaks down. Around photon energies 42~eV, channel experiences a ``Cooper-like" minimum, which is exclusively result inter-electronic correlations shell. Photoionization around minimum predicted theoretically, but experimental...
Attosecond science is well developed for atoms and promising results have been obtained molecules solids. Here, we review the first steps in developing attosecond time-resolved measurements liquids. These advances provide access to time-domain studies of electronic dynamics natural environment chemical reactions biological processes. We concentrate on two techniques that are representative main branches science: pump-probe using pulses high-harmonic spectroscopy (HHS). In part, discuss...
Intermolecular Coulombic decay has been observed in liquid water for the first time. This was achieved using monochromatized high-harmonic radiation coupled to a microjet and an electron-electron coincidence spectrometer.
Electron dynamics in water are of fundamental importance for a broad range phenomena, but their real-time study faces numerous conceptual and methodological challenges. Here, we introduce attosecond size-resolved cluster spectroscopy build up molecular-level understanding the electron water. We measure effect that addition single molecules has on photoionization time delays clusters. find continuous increase delay clusters containing to 4-5 little change towards larger show these...
Measuring time-resolved photoelectron spectra of liquids, and achieving photon energies to probe electronic ground states is challenging. We present gas- liquid-phase XUV-TRPES cis- stilbene, providing new insight into this prototype molecular photoisomerisation dynamics.
In a recent comment, Ruth Signorell raises number of issues that she considers to question the validity our approach determine mean free paths for electron scattering in liquid water and comparison with results on amorphous ice by Michaud, Wen, Sanche. Here, we show these critiques are unjustified, being either unfounded or based misconceptions author comment. We nevertheless welcome opportunity further clarify certain aspects work did not discuss detail letter.