Proton transfer dynamics following strong-field ionization of the water dimer

Zhang, C.; Lu, Juwei; Feng, Tianli; Rottke, H.

doi:10.1103/physreva.99.053408

Cited by 6 publications

(9 citation statements)

References 28 publications

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“…In a previous ion coincidence experiment on water dimers, where a single strong-field 800-nm laser pulse was used to double ionize the dimers, the measured yield of H 3 O + + OH + ion pairs was found to be consistent with a PT time of ∼30 fs (8). The difference to our result is relatively small, especially considering error bars in both experiments.…”

Section: Discussioncontrasting

confidence: 90%

“…The molecular fragments can then be directly detected, and the dynamics can be investigated simultaneously in the time and energy domains. Water clusters provide a test bed for experiments [e.g., (6)(7)(8)(9)] and theory [e.g., (10)(11)(12)(13)] to study the photoionization and, in turn, PT dynamics of water in unprecedented detail for different target size (14). PT manifests as the almost exclusive formation of protonated water clusters following valence ionization, which was experimentally confirmed in clusters of various sizes using time-of-flight measurements (15)(16)(17).…”

Section: Introductionmentioning

confidence: 99%

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Direct tracking of ultrafast proton transfer in water dimers

et al. 2023

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Upon ionization, water forms a highly acidic radical cation H 2 O +· that undergoes ultrafast proton transfer (PT)—a pivotal step in water radiation chemistry, initiating the production of reactive H 3 O + , OH ⋅ radicals, and a (hydrated) electron. Until recently, the time scales, mechanisms, and state-dependent reactivity of ultrafast PT could not be directly traced. Here, we investigate PT in water dimers using time-resolved ion coincidence spectroscopy applying a free-electron laser. An extreme ultraviolet (XUV) pump photon initiates PT, and only dimers that have undergone PT at the instance of the ionizing XUV probe photon result in distinct H 3 O + + OH + pairs. By tracking the delay-dependent yield and kinetic energy release of these ion pairs, we measure a PT time of (55 ± 20) femtoseconds and image the geometrical rearrangement of the dimer cations during and after PT. Our direct measurement shows good agreement with nonadiabatic dynamics simulations for the initial PT and allows us to benchmark nonadiabatic theory.

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Section: Discussioncontrasting

confidence: 90%

Section: Introductionmentioning

confidence: 99%

Direct tracking of ultrafast proton transfer in water dimers

et al. 2023

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“…E ver denotes the first excitation energy of (H 2 O) 2 2+ . These results are consistent with those mentioned in the Introduction [40,41]; it is theoretically predicted that (H 2 O) [40]. The time-scale is consistent with the present calculation.…”

Section: Distribution Of Translational Energies Of Dissociation Productssupporting

confidence: 93%

“…The latter case, the formation of H 3 O + + OH + via a proton-transferred intermediate, includes the influence of the laser pulse duration because the time-scale of the proton transfer and the laser pulse width are comparable. Zhang et al suggested that possible ways to exclude the influence of pulse duration are the use of an extremely short laser pulse width and successive ionization using the pump-probe method [41]. The dynamics calculation of stepwise ionization in this work started from geometrically optimized H 3 O + -OH radical-ion pair as an initial structure.…”

Section: Distribution Of Translational Energies Of Dissociation Productsmentioning

confidence: 99%

“…They calculated the population of reaction products as a function of time on the basis of the dynamics of doubly ionized (H 2 O) 2 at the lowest electronic state and found that the dominant reaction channel was separated into two H 2 O + . Recently, Zhang et al experimentally investigated the proton transfer dynamics of (H 2 O) 2 following strong-field ionization using ultrashort laser pulses [41]. The first and second ionizations occurred within the same laser pulse under the conditions applied.…”

Section: Introductionmentioning

confidence: 99%

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Direct ab initio molecular dynamics study on the reactions of multi-valence ionized states of water dimer

Takada¹,

Tachikawa²

2021

J. Phys. B: At. Mol. Opt. Phys.

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We investigated the reaction of multi-valence (+2) ionization states of water dimer (H2O)2 using direct ab initio molecular dynamics method. The following multi-valence ionization states were considered. In the direct two-electron ionization state, (H2O)2 was ionized to form (H2O)2 2+ in one step; in the stepwise two-electron ionization state, (H2O)2 was first converted to (H2O)2 + and further ionized after structural relaxation. The (H2O)2 2+ from direct ionization dissociated into two H2O+ ions, while (H2O)2 2+ in stepwise ionization generated H3O+ and OH+ ions from H3O+–OH radical-ion pairs. Additionally, we performed dynamics calculations for the excited state of (H2O)2 2+ generated through direct ionization. The excited (H2O)2 2+ ions also dissociated to form H3O+ and OH+ ions. The reaction mechanism of multi-valence ionization states of (H2O)2 is discussed on the basis of calculation results.

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Reaction Pathways of Water Dimer Following Single Ionization

Vinklárek,

Bromberger,

Vadassery

et al. 2024

J. Phys. Chem. A

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Water dimer (H 2 O) 2 �a vital component of the earth's atmosphere�is an important prototypical hydrogen-bonded system. It provides direct insights 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 multimass ion imaging, we report the simultaneous detection of all generated ion products of (H 2 O) 2 + fragmentation following single ionization. Detailed information about ion yields and reaction energetics of 13 ionradical pathways, 6 of which are new, of (H 2 O) 2 + are presented, including strong 18 Oisotope effects.

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Proton transfer dynamics following strong-field ionization of the water dimer

Cited by 6 publications

References 28 publications

Direct tracking of ultrafast proton transfer in water dimers

Direct tracking of ultrafast proton transfer in water dimers

Direct ab initio molecular dynamics study on the reactions of multi-valence ionized states of water dimer

Reaction Pathways of Water Dimer Following Single Ionization

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