Mass spectrometry and its role in advancing cluster science

Jena, P.; Castleman, A. W.

doi:10.1016/j.ijms.2014.08.033

Cited by 15 publications

(12 citation statements)

References 93 publications

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“…Atomically precise metal clusters can be generated both in solution and in the gas phase. Mass spectrometry (MS) is a critical tool for preparing and understanding the unique properties of metal clusters both in the gas phase 7,8 and when deposited onto surfaces. 2,9,10 The production of gas-phase metal clusters has been demonstrated using a variety of ionization sources, including magnetron sputtering, 11 laser ablation, [12][13][14][15] gas aggregation, 16,17 cold reflux discharge 18 , pulsed arc cluster ion sources, 19,20 and electrospray ionization (ESI).…”

Section: Introductionmentioning

confidence: 99%

Ambient preparation and reactions of gas phase silver cluster cations and anions

Wleklinski

Sarkar

Hollerbach

et al. 2015

Phys. Chem. Chem. Phys.

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Electrospray ionization of metal salt solutions followed by ambient heating transforms the resulting salt clusters into new species, primarily naked ionic metal clusters. The experiment is done by passing the clusters through a heated coiled loop outside the mass spectrometer which releases the counter-anion while generating the anionic or cationic naked metal cluster. The nature of the anion in the starting salt determines the type of metal cluster observed. For example, silver acetate upon heating generates only positive silver clusters, Ag(n)(+), but silver fluoride generates both positive and negative silver clusters, Ag(n)(+/-) (3 < n < 20). Both unheated and heated metal salt sprays yield ions with characteristic geometric and electronic magic numbers. There is also a strong odd/even effect in the cationic and anionic silver clusters. Thermochemical control is suggested as the basis for favored formation of the observed clusters, with anhydride elimination occurring from the acetates and fluorine elimination from the fluorides to give cationic and anionic clusters, respectively. Data on the intermediates observed as the temperature is ramped support this. The naked metal clusters react with gaseous reagents in the open air, including methyl substituted pyridines, hydrocarbons, common organic solvents, ozone, ethylene, and propylene. Argentation of hydrocarbons, including saturated hydrocarbons, is shown to occur and serves as a useful analytical ionization method. The new cluster formation methodology allows investigation of ligand-metal binding including in reactions of industrial importance, such as olefin epoxidation. These reactions provide insight into the physicochemical properties of silver cluster anions and cations. The potential use of the ion source in ion soft landing is demonstrated by reproducing the mass spectra of salts heated in air using a custom surface science instrument.

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Section: Introductionmentioning

confidence: 99%

Ambient preparation and reactions of gas phase silver cluster cations and anions

Wleklinski

Sarkar

Hollerbach

et al. 2015

Phys. Chem. Chem. Phys.

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“…This process is called Coulomb explosion or fission of the cluster. The importance of the subject is due to several applications. − For example, a significant part of the experimental research in atomic clusters is carried out with mass spectrometers . The clusters must be ionized before entering into the mass spectrometer. , The other interesting, relatively new application is the study of the reactivity of alkaline metals with water. , …”

Section: Introductionmentioning

confidence: 99%

Coulomb Explosion of Multi-charged Atomic Alkaline Metal Clusters

2021

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In the present work, a computational study of the Coulomb explosions of atomic metal clusters of the type X 8 2+ was carried out, X = (Li−Cs). The work was done within the Kohn−Sham methodology using the Born−Oppenheimer molecular dynamics approximation. The dominant fission channels were established and the electron bonding patterns were analyzed with the help of the Electron Localization Function (ELF). A simple theoretical model was developed to understand and describe, in a qualitatively way, the main physical mechanism involved in the fission of these multicharged clusters. It has been found that the most possible fragments after explosion are the same considering the dynamics or the thermodynamics results. The bonds breaking and formation are well depicted by the ELF, and the main physical effects are well described by the developed model.

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“…Laser vaporization cluster growth and various mass spectrometry techniques have been employed to investigate oxide clusters of many different metals. − Mass-selected photodissociation experiments reveal the decomposition pathways of these systems and the survival of the most stable cluster units, while oxide stoichiometries reveal the metal oxidation states. − ,,, In some systems the preferred stoichiometry indicates a cluster oxidation state that is the same as that found in the bulk metal oxide. This was the case for lanthanum and cerium oxides. , Oxide clusters of other metals were found to fragment preferentially into stoichiometries not common for the bulk material.…”

Section: Introductionmentioning

confidence: 99%

Photodissociation and Theory to Investigate Uranium Oxide Cluster Cations

et al. 2020

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Uranium oxide cluster cations of the form U n O m + are produced by laser vaporization of a depleted uranium rod in a pulsed supersonic expansion. Ions are mass-analyzed and mass-selected with a time-of-flight spectrometer and studied with UV laser multiphoton dissociation. Cations of the stoichiometry UO 2 (UO 3 ) n + were observed as photofragments from all photodissociated cluster cations. (UO 3 ) n + clusters were also observed to result from dissociation of larger (UO 3 ) n + clusters, with UO 3 neutral as a common leaving group. Electronic structure calculations were used to investigate the stability of the prominent uranium oxide cluster cations using density functional theory (DFT) with the hybrid B3LYP exchange-correlation functional and at the CCSD(T) level with cc-pVnZ-PP basis sets (n = D,T), including diffuse orbitals as computational expense and availability permitted. Clustering energies, relative energies and dissociation energies of the cations are reported. The lowest energy neutral (UO 3 ) n clusters up to n = 3 are rings, n = 4 and 5 are chains with very low energy rings, and n = 6 is 3D. The lowest energy structures for UO 2 (UO 3 ) n + are composed of uranyl-like UO 2 + units bound by bridging oxygens to other UO 2 2+ units for n = 2 and 3, and for n = 4 a more complex 3D structure is predicted.

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Mass spectrometry and its role in advancing cluster science

Cited by 15 publications

References 93 publications

Ambient preparation and reactions of gas phase silver cluster cations and anions

Ambient preparation and reactions of gas phase silver cluster cations and anions

Coulomb Explosion of Multi-charged Atomic Alkaline Metal Clusters

Photodissociation and Theory to Investigate Uranium Oxide Cluster Cations

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