Pickup and reactions of molecules on clusters relevant for atmospheric and interstellar processes

Fárnı́k, Michal; Fedor, Juraj; Kočišek, Jaroslav; Lengyel, Jozef; Pluhařová, Eva; Poterya, Viktoriya; Pysanenko, Andriy

doi:10.1039/d0cp06127a

Cited by 39 publications

(53 citation statements)

References 268 publications

(368 reference statements)

Supporting

Mentioning

Contrasting

Order By: Relevance

“…The supersonic expansion + pickup principle has proved efficient for the production of mixed water clusters with dopant species and their subsequent characterization in the gas phase. 10 It has recently been applied to study alkali halides in water clusters 11 , 12 as well as anhydrous alkali halide clusters 12 − 15 with X-ray photoelectron spectroscopy (XPS). It was reported that the binding energies (BEs) of nanosolvated alkali and halide ions are insensitive to the counterions in water clusters with a few hundred water molecules, 11 similar to what has been observed in bulk solutions.…”

Section: Introductionmentioning

confidence: 99%

Core and Valence Level Photoelectron Spectroscopy of Nanosolvated KCl

et al. 2021

View full text Add to dashboard Cite

The solvation of alkali and halide ions in the aqueous environment has been a subject of intense experimental and theoretical research with multidisciplinary interests; yet, a comprehensive molecular-level understanding has still not been obtained. In recent years, electron spectroscopy has been increasingly applied to study the electronic and structural properties of aqueous ions with implications, especially in atmospheric chemistry. In this work, we report core and valence level (Cl 2p, Cl 3p, and K 3p) photoelectron spectra of the common alkali halide, KCl, doped in gas-phase water clusters in the size range of a few hundred water molecules. The results indicate that the electronic structure of these nanosolutions shows a distinct character from that observed at the liquid–vapor interface in liquid microjets and ambient pressure setups. Insights are provided into the unique solvation properties of ions in a nanoaqueous environment, emerging properties of bulk electrolyte solutions with growing cluster size, and sensitivity of the electronic structure to varying solvation configurations.

show abstract

Section: Introductionmentioning

confidence: 99%

Core and Valence Level Photoelectron Spectroscopy of Nanosolvated KCl

et al. 2021

View full text Add to dashboard Cite

show abstract

“…Then, the clusters enter a time-of-flight mass spectrometer (TOF), where the mass spectra after electron ionization are recorded. The experimental setup is described elsewhere, 23 , 24 and more details are given in the Supporting Information . We should mention that due to cluster fragmentation and the limited discrimination-free mass range of our TOF spectrometer, the mean cluster size has been derived from the Poisson distribution of the adsorbed molecular clusters rather than from the mass spectra, as detailed in the Supporting Information .…”

mentioning

confidence: 99%

Uptake of Hydrogen Bonding Molecules by Benzene Nanoparticles

Vinklárek

Pysanenko

Pluhařová

et al. 2022

J. Phys. Chem. Lett.

Self Cite

View full text Add to dashboard Cite

The uptake of molecules on nanometer-size clusters of polyaromatic hydrocarbons (PAHs) is important for the condensation of water on PAH aerosols in the atmosphere and for ice mantle growth on nanoparticles in the interstellar medium. We generate benzene clusters Bz N of mean size N̅ ≈ 300 (radius R̅ ≈ 2.2 Å) as a model system for the PAH nanoparticles. Using molecular beams and mass spectrometry detection, we investigate the uptake of water, methanol, and ethanol by these clusters. All picked up molecules are highly mobile on Bz N and generate clusters within <3 ms. The relative uptakes for the different investigated molecules can be directly compared and quantified. Water molecules exhibit the lowest relative pickup probability that is ∼30% lower than those for methanol and ethanol, which are approximately the same.

show abstract

“…Trends as well as dimensionless sphericity are comparable between both approaches. 4 ■ RESULTS AND DISCUSSION Implementation Overview. The development of the custom-built software that actively utilizes the power of GPU for higher precision simulation has posed multiple challenges.…”

Section: ■ Theoretical Overviewmentioning

confidence: 99%

“…These clusters are similar to atmospheric aerosol particles; therefore, their properties have a great meaning in the chemistry of atmosphere. 2 The cross section of water clusters can be estimated 3,4 by their capability to pick up other particles on their surface. After considering polarization and other phenomena which cause the pickup cross section to be larger than the geometric cross section, it has been deduced that there is still an unexplained increase for large clusters, which has been attributed to the clusters of irregular shape 4,5 rather than spherical.…”

Section: ■ Introductionmentioning

confidence: 99%

“…2 The cross section of water clusters can be estimated 3,4 by their capability to pick up other particles on their surface. After considering polarization and other phenomena which cause the pickup cross section to be larger than the geometric cross section, it has been deduced that there is still an unexplained increase for large clusters, which has been attributed to the clusters of irregular shape 4,5 rather than spherical. This is to some extent counter-intuitive and witnesses about complex phenomena that may take place here, as aggregation of frozen smaller clusters later in the apparatus as a consequence of turbulent flow and/or sonic boom.…”

Section: ■ Introductionmentioning

confidence: 99%

See 1 more Smart Citation

Molecular Dynamics of Heterogeneous Systems on GPUs and Their Application to Nucleation in Gas Expanding to a Vacuum

Celný

Klíma

Kolafa

2021

J. Chem. Theory Comput.

View full text Add to dashboard Cite

Expansion of water vapor through a small orifice to a vacuum produces liquid or frozen clusters which in the experiment serve as model particles for atmospheric aerosols. Yet, there are controversies about the shape of these clusters, suggesting that the nucleation process is not fully understood. Such questions can be answered by molecular dynamics simulations; however, they require microsecond-scale runs with thousands of molecules and accurate energy conservation. The available highly parallel codes typically utilize domain decomposition and are inefficient for heterogeneous systems as clusters in a dilute gas. In this work, we present an implementation of molecular dynamics on graphics processing units based on the Verlet list and apply it to several systems for which experimental data are available. We reproduce sufficiently sized clusters but not the experimentally observed clusters of irregular shape.

show abstract

Pickup and reactions of molecules on clusters relevant for atmospheric and interstellar processes

Abstract: In this perspective, we review experiments with molecules picked up on clusters in molecular beams with the focus on the processes in atmospheric and interstellar chemistry.

Cited by 39 publications

References 268 publications

Core and Valence Level Photoelectron Spectroscopy of Nanosolvated KCl

Core and Valence Level Photoelectron Spectroscopy of Nanosolvated KCl

Uptake of Hydrogen Bonding Molecules by Benzene Nanoparticles

Molecular Dynamics of Heterogeneous Systems on GPUs and Their Application to Nucleation in Gas Expanding to a Vacuum

Contact Info

Product

Resources

About