Low Temperature Kinetics of the First Steps of Water Cluster Formation

Bourgalais, Jérémy; Roussel, Vivien; Capron, Michaël; Bénidar, Abdessamad; Jasper, Ahren W.; Klippenstein, Stephen J.; Biennier, Ludovic; Picard, Sébastien D. Le

doi:10.1103/physrevlett.116.113401

Cited by 29 publications

(43 citation statements)

References 43 publications

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“…These results, obtained by comparison of electron ionization and sodium doping (see below), have recently been confirmed by another type of experiment . Nevertheless, the assumption of only an OH evaporation upon (H 2 O) N ionization is sometimes extended to the electron ionization spectra . On the other hand, the minimum cluster fragmentation is apparently a good assumption in some cases of the mixed water clusters even upon the 70 eV electron ionization.…”

Section: Cluster Ionization For Mass Spectrometrysupporting

confidence: 52%

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Mass spectrometry of aerosol particle analogues in molecular beam experiments

Fárnı́k

Lengyel

2017

Mass Spectrometry Reviews

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Nanometer-size particles such as ultrafine aerosol particles, ice nanoparticles, water nanodroplets, etc, play an important, however, not yet fully understood role in the atmospheric chemistry and physics. These species are often composed of water with admixture of other atmospherically relevant molecules. To mimic and investigate such particles in laboratory experiments, mixed water clusters with atmospherically relevant molecules can be generated in molecular beams and studied by various mass spectrometric methods. The present review demonstrates that such experiments can provide unprecedented details of reaction mechanisms, and detailed insight into the photon-, electron-, and ion-induced processes relevant to the atmospheric chemistry. After a brief outline of the molecular beam preparation, cluster properties, and ionization methods, we focus on the mixed clusters with various atmospheric molecules, such as hydrated sulfuric acid and nitric acid clusters, N O and halogen-containing molecules with water. A special attention is paid to their reactivity and solvent effects of water molecules on the observed processes.

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Section: Cluster Ionization For Mass Spectrometrysupporting

confidence: 52%

“…[50][51][52] The aerosol probing can be performed by different techniques ranging from X-ray and neutron scattering 49,53 to VUV ionization mass spectrometry. 50,52,54 Such experiments enable direct experimental observation of the onset of the aerosol nucleation.…”

Section: Halogen Containing Molecules and Clustersmentioning

confidence: 99%

Mass spectrometry of aerosol particle analogues in molecular beam experiments

Fárnı́k

Lengyel

2017

Mass Spectrometry Reviews

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“…MS is extremely sensitive,but is usually not suitable (with an exception) [135] for distinguishing between conformers or molecules of the same mass,and lowresolution MS (which is typically used) is unable to distinguish between high-mass complex molecules.Afurther limitation on the LIF data is that, with afew exceptions,experiments on neutral-neutral reactions result in the changes in concentra- 2 30, 100 [130] 4.7 n-alcohols 200 [131] 10 D 2 O-nonane2 00 [132] 20 toluene 40 [133] 20 propane 40 [134] 5 H 2 O2 3-69 [111] tion being observed for only one species-the radical reagent. MS is extremely sensitive,but is usually not suitable (with an exception) [135] for distinguishing between conformers or molecules of the same mass,and lowresolution MS (which is typically used) is unable to distinguish between high-mass complex molecules.Afurther limitation on the LIF data is that, with afew exceptions,experiments on neutral-neutral reactions result in the changes in concentra- 2 30, 100 [130] 4.7 n-alcohols 200 [131] 10 D 2 O-nonane2 00 [132] 20 toluene 40 [133] 20 propane 40 [134] 5 H 2 O2 3-69 [111] tion being observed for only one species-the radical reagent.…”

Section: ''The Marriage'' Of Spectroscopy and Dynamicsmentioning

confidence: 99%

Uniform Supersonic Chemical Reactors: 30 Years of Astrochemical History and Future Challenges

et al. 2017

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The interstellar medium is of great interest to us as the place where stars and planets are born and from where, probably, the molecular precursors of life came to Earth. Astronomical observations, astrochemical modeling, and laboratory astrochemistry should go hand in hand to understand the chemical pathways to the formation of stars, planets, and biological molecules. We review here laboratory experiments devoted to investigations on the reaction dynamics of species of astrochemical interest at the temperatures of the interstellar medium and which were performed by using one of the most popular techniques in the field, CRESU. We discuss new technical developments and scientific ideas for CRESU, which, if realized, will bring us one step closer to understanding of the astrochemical history and the future of our universe.

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“…In molecular beam expansions, the cluster growth rate and internal temperature depend sensitively on the distance from the orifice (usually defined as a scaled distance relative to the orifice size), if other parameters such as the backing pressure, the source temperature, the carrier gas and the nozzle diameter are held constant. 32,33 The primary step in the cluster growth is the condensation of monomers to form dimers through "2+1" body collisions: two D2O molecules combine to form the energised dimer (D2O)2 * , which may then either dissociate or undergo a collision with a third body (Ar in the present case) that quenches the excess energy to form the stable dimer (D2O)2. 32 Additional monomers can condense onto the dimer or dimers can condense onto each other in similar collision processes, ultimately leading to the growth of the cluster.…”

Section: The Population Inversion Of Isomers I and Ii As A Function Omentioning

confidence: 99%

“…32,33 The primary step in the cluster growth is the condensation of monomers to form dimers through "2+1" body collisions: two D2O molecules combine to form the energised dimer (D2O)2 * , which may then either dissociate or undergo a collision with a third body (Ar in the present case) that quenches the excess energy to form the stable dimer (D2O)2. 32 Additional monomers can condense onto the dimer or dimers can condense onto each other in similar collision processes, ultimately leading to the growth of the cluster.…”

Section: The Population Inversion Of Isomers I and Ii As A Function Omentioning

confidence: 99%

Selectivity in Electron Attachment to Water Clusters

Lietard

Verlet

2019

J. Phys. Chem. Lett.

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The full-text may be used and/or reproduced, and given to third parties in any format or medium, without prior permission or charge, for personal research or study, educational, or not-for-prot purposes provided that:• a full bibliographic reference is made to the original source • a link is made to the metadata record in DRO • the full-text is not changed in any way The full-text must not be sold in any format or medium without the formal permission of the copyright holders.Please consult the full DRO policy for further details. ABSTRACTElectron attachment onto water clusters to form water cluster anions is studied by varying the point of electron attachment along a molecular beam axis and probing the produced cluster anions using photoelectron spectroscopy. The results show that the point of electron attachment has a clear effect on the final distribution of isomers for a cluster containing 78 water molecules, with isomer I formed preferentially near the start of the expansion and isomer II formed preferentially once the molecular beam has progressed for several millimetres. These changes can be accounted for by the cluster growth rate along the beam.Near the start of the expansion, cluster growth is proceeding rapidly with condensing water molecules solvating the electron, while further along the expansion, the growth has terminated and electrons are attached to large and cold preformed clusters, leading to the isomer associated with a loosely bound surface state.

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Low Temperature Kinetics of the First Steps of Water Cluster Formation

Cited by 29 publications

References 43 publications

Mass spectrometry of aerosol particle analogues in molecular beam experiments

Mass spectrometry of aerosol particle analogues in molecular beam experiments

Uniform Supersonic Chemical Reactors: 30 Years of Astrochemical History and Future Challenges

Selectivity in Electron Attachment to Water Clusters

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