Ion–Molecule Reactions in Helium Nanodroplets Doped with C<sub>60</sub> and Water Clusters

Denifl, Stephan; Zappa, Fábio; Mähr, Ingo; Silva, F. Ferreira da; Aleem, Abid; Mauracher, Andreas; Probst, Michael; Urban, Ján; Mach, Pavel; Bacher, A.; Echt, Olof; Märk, T.D.; Scheier, P.

doi:10.1002/anie.200904381

Cited by 43 publications

(45 citation statements)

References 29 publications

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“…However, theoretical studies leave no doubt that 32 helium atoms form a commensurate 1 × 1 phase on neutral or positively charged C 60 [11,13,14]. The same is true for adsorption of methane [24], ethylene [25], and xenon [28] but neither for neon, argon, and krypton [28] nor for polar molecules [29].…”

Section: Resultsmentioning

confidence: 99%

Adsorption of helium on isolated C₆₀and C₇₀anions

et al. 2015

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Adsorption of helium on free, negatively charged fullerenes is studied in this work. Helium nanodroplets have been doped with fullerenes and ionised by electron attachment. For suitable experimental conditions, C − 60 and C − 70 anions are found to be complexed with a large number of helium atoms. Prominent anomalies in the ion abundances indicate the high stability of the commensurate 1 × 1 phase in which all hollow adsorption sites are occupied by one atom each. The adsorption energy for an additional helium atom is about 40% less than for atoms in the commensurate layer, similar to our previous findings for fullerene cations and in agreement with theoretical dissociation energies. Similarly, an anomaly in the adsorption energy occurs when 60 helium atoms are attached to C − 60 or 65 to C − 70 . For C 60 , the anomaly coincides with the one observed for cationic complexes but for C 70 it does not. Implications of these features are discussed in light of several theoretical studies of neutral and positively charged helium-fullerene complexes.

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Section: Resultsmentioning

confidence: 99%

Adsorption of helium on isolated C₆₀and C₇₀anions

et al. 2015

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“…Very recently an FTIR experiment on water clusters generated under conditions very similar to ours (less than 1% of water seeded in argon with high backing pressure) suggest that small water clusters (n=2-5) were completely solvated by argon clusters composed of between [17][18][19][20][21][22] atoms. 33 This was based on comparison of the vibrational spectrum with ab-initio calculations.…”

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“…A process termed active parent ion cooling was coined, where argon atoms effectively carried away the excess energy upon evaporation. Electron impact ionization of water clusters embedded in helium nano-droplets have also shown evidence of water cluster ions (typically at the 10% level when compared to protonated ones), 18,19 as does ion bombardment of ice in a recent secondary ion emission experiment. 20 These studies suggest nondissociative ionization of small water clusters may be feasible only with an ultra-soft ionization method and here we show how an argon cluster can take the role of both electronic energy transport and a heat bath to achieve ultra-soft ionization.…”

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Ionization of Water Clusters Mediated by Exciton Energy Transfer from Argon Clusters

Golan

Ahmed

2012

J. Phys. Chem. Lett.

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The exciton energy deposited in an argon cluster (Ar n , ⟨n = 20⟩) using VUV radiation is transferred to softly ionize doped water clusters ((H2O) n , n = 1–9), leading to the formation of nonfragmented clusters. Following the initial excitation, electronic energy is channeled to ionize the doped water cluster while evaporating the Ar shell, allowing identification of fragmented and complete water cluster ions. Examination of the photoionization efficiency curve shows that cluster evaporation from excitons located above 12.6 eV is not enough to cool the energized water cluster ion and leads to their dissociation to (H2O) n−2H+ (protonated) clusters.

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“…[20] When different types of atoms/molecules are added to the droplets, aggregation into binary complexes is expected. [21][22][23][24][25][26][27][28][29][30] Here metal-organic complexes are formed by the co-addition of Au and H2TPyP to the droplets and any products are then deduced using mass spectrometry. Through these experiments we intend to show that different types of metal-organic compounds can be synthesized in helium nanodroplets by simply switching the order in which the dopants are added, i.e., the addition of Au to helium nanodroplets prior to or after the addition of H2TPyP.…”

Section: Introductionmentioning

confidence: 99%

“…An alternative explanation is the presence of doubly charged reaction intermediates, which can contribute to the H-loss in organic molecules and biomolecules. [41] The H-loss channel of the pyrrole ion at m/z 66 is as strong as the pyrrole ion signal at m/z 67. For the cluster centred at m/z 79, the protonated pyridine ion at m/z 80 is prominent and the H-loss product has nearly twice the abundance of the pyridine ion.…”

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Formation of Au and tetrapyridyl porphyrin complexes in superfluid helium

Cheng

Latimer

Spence

et al. 2015

Phys. Chem. Chem. Phys.

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Binary clusters containing a large organic molecule and metal atoms have been formed by the co-addition of 5,10,15,20-Tetra(4-pyridyl)porphyrin (H2TPyP) molecules and gold atoms to superfluid helium nanodroplets, and the resulting complexes were then investigated by electron impact mass spectrometry. In addition to the parent ion H2TPyP yields fragments mainly from pyrrole, pyridine and methylpyridine ions because of the stability of their ring structures. When Au is co-added to the droplets the mass spectra are dominated by H2TPyP fragment ions with one or more Au atoms attached. We also show that by switching the order in which Au and H2TPyP are added to the helium droplets, different types of H2TPyP/Au complexes are clearly evident from the mass spectra. This study suggests a new route for the control over the growth of metal-organic compounds inside superfluid helium nanodroplets.3

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Ion–Molecule Reactions in Helium Nanodroplets Doped with C₆₀ and Water Clusters

Cited by 43 publications

References 29 publications

Adsorption of helium on isolated C₆₀and C₇₀anions

Adsorption of helium on isolated C₆₀and C₇₀anions

Ionization of Water Clusters Mediated by Exciton Energy Transfer from Argon Clusters

Formation of Au and tetrapyridyl porphyrin complexes in superfluid helium

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Ion–Molecule Reactions in Helium Nanodroplets Doped with C60 and Water Clusters

Cited by 43 publications

References 29 publications

Adsorption of helium on isolated C60and C70anions

Adsorption of helium on isolated C60and C70anions

Ionization of Water Clusters Mediated by Exciton Energy Transfer from Argon Clusters

Formation of Au and tetrapyridyl porphyrin complexes in superfluid helium

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Ion–Molecule Reactions in Helium Nanodroplets Doped with C₆₀ and Water Clusters

Adsorption of helium on isolated C₆₀and C₇₀anions

Adsorption of helium on isolated C₆₀and C₇₀anions