An Ultrafast Glimpse of Cluster Solvation Effects on Reaction Dynamics

Zhong, Qun; Aw, Castleman

doi:10.1021/cr990056f

Cited by 58 publications

(35 citation statements)

References 202 publications

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“…This is the case for neutron halos in neutron rich nuclei, close to the neutron drip line (23,24), which marks the boundary for the existence of these nuclei (e.g., 6 He, 11 Li, and 11 Be), where a diffuse neutron cloud is induced by short-range nuclear forces (23,24). Another example is the formation of diffuse surface states of an excess electron on (He) n (n Ͼ 4⅐10 5 ) clusters, which are induced by strong short-range repulsive pseudopotential and weak longrange attractive polarization interactions (25).…”

Section: Discussionmentioning

confidence: 93%

Regular multicharged transient soft matter in Coulomb explosion of heteroclusters

Last

Jortner

2005

Proc. Natl. Acad. Sci. U.S.A.

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Nanointerfaces of mobile, thin spherical shells of light ions that expand on the femtosecond time scale, can be produced by Coulomb explosion of extremely ionized molecular heteroclusters consisting of light and heavy ions, e.g., (D ؉ I q؉ ) n (q ‫؍‬ 7-35), which are generated in ultraintense laser fields (intensity, I, ‫؍‬ 10 16 to 10 20 W⅐cm ؊2 ). Modeling, together with molecular dynamics simulations, reveals the expansion of 2D monolayers with high energies and narrow energy distributions [e.g., Eav Ӎ 23 keV and ⌬E͞Eav ‫؍‬ 0.16 for D ؉ from (D ؉ I 25؉ )2171] arising from kinematic run-over effects. The expanding regular, monoionic, spherical nanointerfaces manifest the attainment of transient self-organization in complex systems driven by repulsive Coulomb interactions. molecular heteroclusters ͉ extreme ionization ͉ Coulomb instability ͉ expanding nanointerfaces ͉ transient self-organization R igid and soft interfaces between different forms of macroscopic matter play a central role in surface, polymer, and soft matter science (1). Nanointerfaces in finite systems, i.e., clusters and nanostructures, that are characterized by a large surfaceto-volume ratio (2), can also be subdivided into two analogous categories: (i) Rigid nanointerfaces, involving the surfaces of metallic, ionic, molecular, semiconductor, or van der Waals clusters at sufficiently low temperatures (2), as well as monomolecular layers of fullerenes or of nanotubes (3), and (ii) soft nanointerfaces involving surfaces of liquid clusters above the (smeared out) phase transition temperature (4) or of helium clusters at zero temperature (2). We propose that nanointerfaces consisting of multicharged soft matter with radially expanding monomolecular mobile boundaries can be realized by Coulomb explosion (5-7) of some highly ionized molecular heteroclusters, whose constituents consist of light few-electron and heavy many-electron atoms, e.g., hydroiodic acid (AI) n clusters or methyl iodide (CA 3 I) n clusters (with A ϭ H, D, or T). Extreme multielectron heterocluster ionization in ultraintense laser fields (peak I ϭ 10 16 to 10 20 W⅐cm Ϫ2 ) results in spectacular ionic clusters, e.g., (D ϩ I qϩ ) n (with an iodine heavy ion charge of q ϭ 7-35). Such extreme ionization levels can be accomplished by the barrier suppression ionization mechanism (8) for a single molecule (Fig. 1). In the intensity domain I ϭ 10 17 to 10 18 W⅐cm Ϫ2 , a further increase of the ionization level in the cluster is induced by the ignition mechanism (8, 9), whereas at the highest-intensity domain, I ϭ 10 19 to 10 20 W⅐cm Ϫ2 , which is of interest herein, the charges on individual cluster molecules are identical to the single-molecule q (Fig. 1 Inset). We demonstrate the formation of unique regular nanostructures (spatial dimensions of ϳ100-500 Å) in the Coulomb explosion of light-heavy ionic heteroclusters, which gives rise to extremely mobile, transient, expanding boundary monolayers of A ϩ (H ϩ , D ϩ , or T ϩ ) ions. These transient spherical shells provide a case of soft m...

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Section: Discussionmentioning

confidence: 93%

Regular multicharged transient soft matter in Coulomb explosion of heteroclusters

Last

Jortner

2005

Proc. Natl. Acad. Sci. U.S.A.

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“…The interaction of ions with their chemical environment plays an important role in many areas of chemistry, from atmospheric chemistry and astrochemistry to electrochemistry, catalysis and biochemistry [12][13][14][15][16][17][18][19][20][21][22][23][24][25]. For example, solvation has an important mediating role in chemistry, e.g.…”

Section: Introductionmentioning

confidence: 99%

The interaction of negative charge with carbon dioxide – insight into solvation, speciation and reductive activation from cluster studies

Weber

2014

International Reviews in Physical Chemistry

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The interaction of CO 2 with negative charge is of high importance in many natural and industrial processes, since reductive activation is one of the most common and convenient ways to chemically unlock this robust molecule. While free CO 2 does not form stable anions, the accessibility of low-lying molecular orbitals is critical for its chemical versatility and allows CO 2 to act as solvent as well as a reaction partner for negative ions. Experiments on mass selected cluster ions are highly suitable for the study of the fundamental properties of CO 2 and its interaction with excess electrons and anions, since they circumvent many problems associated with experiments in the condensed phase. The combination of mass spectrometry, laser spectroscopy and quantum chemical calculations results in a powerful tool set to address questions of reactivity, ion speciation and solvation, and they can provide key information to understanding the ion chemistry of CO 2 .

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“…[8][9][10][11][12][13] Such bond dissociations are mainly of "chemical" nature and are characterized by electron redistribution [14][15][16][17] through availability of more favorable bonding partners or through external driving forces such as environmental conditions (solvent or temperature). [18][19][20] Furthermore, many atmospheric reactions are also of this type. Ozone depletion through the presence of chlorofluorocarbon in the stratosphere is an example for one of these reactions.…”

Section: Introductionmentioning

confidence: 99%

Photodissociation Dynamics of ClCN at Different Wavelengths

Lütz¹,

Meuwly²

2011

ChemPhysChem

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The photodissociation dynamics of small molecules in the gas and condensed phase is an important source of information for better characterizing intermolecular interactions. Herein, classical molecular dynamics simulations with provisions to follow reactive processes between different electronic states are used to probe the wavelength dependence of product state distributions after laser excitation of ClCN. It is found that the maximum of the rotational excitation distribution P(j) of the CN product shifts to lower j-values with increasing wavelength and the width of the distribution narrows. Both observations are in accord with earlier experiments and provide improvements over previous theoretical treatments of the process with the same interaction potentials. For the reaction in a water droplet, strong quenching of rotational excitation is found.

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An Ultrafast Glimpse of Cluster Solvation Effects on Reaction Dynamics

Cited by 58 publications

References 202 publications

Regular multicharged transient soft matter in Coulomb explosion of heteroclusters

Regular multicharged transient soft matter in Coulomb explosion of heteroclusters

The interaction of negative charge with carbon dioxide – insight into solvation, speciation and reductive activation from cluster studies

Photodissociation Dynamics of ClCN at Different Wavelengths

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