arXiv subjects

Ivo S. Vinklárek

Publications and source records attributed to Ivo S. Vinklárek.

4 recordsLinked to original sources

arXiv2026

Proton transfer and hydronium formation in ionized water

Aqueous radiation chemistry emerges through ultrafast proton transfer and ion-radical formation with unexplored energy-redistribution dynamics steering the subsequent reactions. We performed a time-resolved disruptive-probing experiment on pure water dimer, (H$_2$O)$_2$, to disentangle the elementary post-ionization reactions. Through kinetic-energy-resolved ion imaging, we unraveled the dynamics in the (H$_2$O)$_2^+$ ground state: at low-energy ($\sim$0.05~eV) ultrafast proton transfer ($\sim$19~fs) is followed by H$_3$O$^+$+OH fragmentation ($\sim$360~fs). At higher energies, proton transfer becomes hindered ($\sim$60~fs) while the subsequent fragmentation becomes faster ($\sim$210~fs), eventually ($>0.15$~eV) merging into coupled dynamics ($\sim$100~fs). Additionally, we observed H$_2$O)$_2^+$ stabilization proceeding through a Zundel-like structure. These timescales and product energies reveal how ion-radical formation in ionized hydrogen-bonded networks shapes reactivity in aqueous dynamics.

physics.chem-ph↗

arXiv2026

Rotational-state-controlled dissociative ionization dynamics in $\mathrm{CF_2I_2}$

We investigated strong-field dissociative ionization of $\mathrm{CF_2I_2}$ ensembles prepared in different initial rotational-state distributions using an electrostatic deflector. Pronounced changes in ion-channel branching ratios revealed a strong dependence of the fragmentation dynamics on the initial rotational excitation. Analysis of fragment yields and their laser-power dependences identifies resonance-enhanced multiphoton ionization through an intermediate excited state, $\mathrm{CF_2I_2^{\ast}}$. The measured branching behavior indicates competition between stabilization into bound ionic states and dissociative channels, driven by near-threshold non-adiabatic Coriolis-type coupling. Tuning the rotational energy by only a few $μ$eV is sufficient to significantly alter the ionization dynamics and to redistribute the reaction products. These findings demonstrate the key role of rotational excitation in controlling non-adiabatic dynamics following strong-field ionization of $\mathrm{CF_2I_2}$.

physics.chem-ph↗

arXiv2024

A versatile and transportable endstation for controlled molecule experiments

We report on a new versatile transportable endstation for controlled molecule (eCOMO) experiments providing a combination of molecular beam purification by electrostatic deflection and simultaneous ion and electron detection using velocity-map imaging (VMI). The $b$-type electrostatic deflector provides spatial dispersion of species based on their effective-dipole-moment-to-mass ratio. This enables selective investigation of molecular rotational quantum states, conformers, and molecular clusters. Furthermore, the double-sided VMI spectrometer equipped with two high-temporal-resolution event-driven Timepix3 cameras provides detection of all generated ions independently of their mass-over-charge ratio and electrons. To demonstrate the potential of this novel apparatus, we present experimental results from our investigation of carbonyl sulfide (OCS) after ionization. Specifically, we provide the characterization of the molecular beam, electrostatic deflector, and electron- and ion-VMI spectrometer. The eCOMO endstation delivers a platform for ultrafast dynamics studies using a wide range of light sources from table-top lasers to free-electron-laser and synchrotron-radiation facilities. This makes it suitable for research activities spanning from atomic, molecular, and cluster physics, over energy science and chemistry, to structural biology.

physics.chem-ph↗

arXiv2024

Reaction Pathways of Water Dimer Following Single Ionization

Water dimer $(\text{H}_2\text{O})_2$ -- a vital component of the earth's atmosphere -- is an important prototypical hydrogen-bonded system. It provides direct insight into fundamental chemical and biochemical processes, e.g., proton transfer and ionic supramolecular dynamics occurring in astro- and atmospheric chemistry. Exploiting a purified molecular beam of water dimer and multi-mass ion imaging, we report the simultaneous detection of all generated ion products of $(\text{H}_2\text{O})^{+}_2$-fragmentation following single ionization. Detailed information about ion yields and reaction energetics of 13 ion-radical pathways, 6 of which are new, of $(\text{H}_2\text{O})^{+}_2$ are presented, including strong ${}^{18}\text{O}$-isotope effects.

physics.atm-clus↗