On the dynamics of the reaction of positive hydrogen cluster ions (H5+ to H23+) with para and normal hydrogen at 10 K

Paul, William; Lucké, Balduin; Schlemmer, S.; Gerlich, D.

doi:10.1016/0168-1176(95)04269-q

Cited by 64 publications

(58 citation statements)

References 30 publications

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“…This result agrees with the experiments of Ref. [44], in which the most abundant cluster observed was the H + 19 one. …”

Section: The Clustering Process In Lowdensity Atmospheressupporting

confidence: 83%

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On the formation mechanisms of hydrogen ionic clusters

Barbatti¹,

Nascimento²

2003

Braz. J. Phys.

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Structural and thermodynamic properties of hydrogen molecular clusters formed around an atomic or molecular cation are examined. The shell distribution of H2 molecules and the size of the clusters are discussed. The Bloom-Margenau model for predicting the number of neutral molecules that could bind to a cation core is investigated and its limitations are illustrated using the Li + (H2) k clusters as test case. Finally, results for the entropy of the H + n clusters (n = 5 − 27, odd) and for the Gibbs free energy variations associated to the cluster formation are presented and the spontaneity of the clustering process in different conditions is examined. I IntroductionThe presence of a cation in a molecular hydrogen environment leads to the formation of molecular clusters around the ion. In the case of an H 2 homogeneous atmosphere, an H + 2 ion is quickly converted to the H + 3 molecule, which becomes the core for the clustering processwhere the exceeding H 2 molecule carries away the excess of energy, stabilizing the cluster. From these multiple-steps reactions, H + n clusters (n odd) are formed, and clusters as large as H + 99 have been observed [1]. Depending on the temperature and pressure conditions, the H + 15 and H + 17 clusters are the more abundant.One of the most interesting features of these species is that in the cluster, each H 2 molecule is strongly bound by the coulombian field of the cation. This may be very useful when dealing with hydrogen storage problems.In the last decade, ab initio calculations have been performed to clusters as large as H + 35 [2][3][4][5][6][7][8][9][10][11][12]. Recently, more attention has been dedicated to the H + 5 cluster. Its potential energy surface has been studied at high levels of calculation [13,14] and its presence in some interstellar environments in concentrations up two times higher than that of the H + 3 molecule has been investigated [15].Besides the H + 3 molecular ion, a large variety of atomic and molecular cations has been considered as a core for H 2 clustering: the first-column Li + , Na + and K + ions [16][17][18][19][20][21][22] Table I summarizes some properties of these X + (H 2 ) k hydrogen clusters.The experimental work on the hydrogen clusters has been concentrated on enthalpy variation measurements (∆H) [16,24,25,26,31,33] and collisional induced dissociation (CID) studies [34,35,36,37]. The ∆H measurements for the H + n clusters and for the most general X + (H 2 ) k clusters have been an important source of information about the cluster energetic properties and have guided the theoretical studies. On the other hand, the CID studies have revealed patterns for the cluster dissociation and their dependence on the shell structure of H 2 distribution. Hitherto, very few theoretical and experimental attention has been payed to the vibrational properties and the infrared spectra of the hydrogen clusters, these studies being basically restricted to the H + 5 species [38,39]. For clusters larger than the H + 5 one, only a few experimental results are...

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“…This result agrees with the experiments of Ref. [44], in which the most abundant cluster observed was the H + 19 one. …”

Section: The Clustering Process In Lowdensity Atmospheressupporting

confidence: 83%

“…[44], that is a density of 10 14 H 2 molecules/cm 3 (3 × 10 −16 atm) and a temperature of 10 K; b) the typical conditions found at DICs: H 2 density of 10 5 molecules/cm 3 (2 × 10 −15 atm) and a temperature of 30 K [45]. Figure 5a shows the entropy for the clusters with n = 5 − 27.…”

Section: The Clustering Process In Lowdensity Atmospheresmentioning

confidence: 99%

On the formation mechanisms of hydrogen ionic clusters

Barbatti¹,

Nascimento²

2003

Braz. J. Phys.

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“…The feature is critically important for experiments conducted at lower temperatures for larger and/or less strongly bound clusters. 10 Lovejoy and Bianco 29 have examined the effect of the applied trap driving voltage on the measured decomposition rate constants for H + (H 2 O) 4 and other cluster ion systems. Their results show that the RF heating effect is nonnegligible at the parameter q z > 0.3 when using the quadrupole ion trap as a storage cell.…”

Section: Experimental and Computational Sectionsmentioning

confidence: 99%

“…Temperature control of the storage cell can therefore be performed to change the ion temperature. In the 1980s, Gerlich and co-workers [8][9][10] developed multipole radio frequency (RF) ion traps, which serve as ion storage cells and can easily be combined with lasers. 8 Integration of the trap to a refrigeration system enables active temperature control of the storage cell, thereby allowing studies of the temperature dependence of ionmolecule interactions 9 as well as the thermodynamic and kinetic properties of gas-phase ions and cluster ions.…”

Section: Introductionmentioning

confidence: 99%

“…8 Integration of the trap to a refrigeration system enables active temperature control of the storage cell, thereby allowing studies of the temperature dependence of ionmolecule interactions 9 as well as the thermodynamic and kinetic properties of gas-phase ions and cluster ions. 10 In this paper, a temperature-variable 22-pole ion trap integrated into a tandem mass spectrometer is used for investigation of charged water clusters, in both protonated [H + (H 2 O) n ] and deprotonated [OH -(H 2 O) m ] forms, produced from a supersonic expansion. These cluster ions are chosen because water is not only of general interest in physical chemistry but also plays important roles in interstellar space 11 and in the atmosphere.…”

Section: Introductionmentioning

confidence: 99%

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Investigations of Protonated and Deprotonated Water Clusters Using a Low-Temperature 22-Pole Ion Trap

Wang¹,

Tsai²,

Lee³

et al. 2003

J. Phys. Chem. A

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121

103

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A new tandem mass spectrometer, containing a temperature-variable 22-pole ion trap, has been constructed. It is applied, as a first application, to kinetic and spectroscopic investigation of charged water clusters produced from a supersonic expansion. Using low-pressure He or H 2 as buffer gas for collisional thermalization, refrigeration of the ion trap allows a good control of the cluster temperature over the range 77-350 K. It provides an accurate means of determining the dissociation energies of both protonated and deprotonated water cluster ions [H + (H 2 O) n and OH -(H 2 O) m ] by measuring the dissociation rates at various temperatures along with their internal energies calculated from vibrational frequencies provided by density functional theory calculations. In this report, results of the thermochemical measurements for H + (H 2 O) 4-10 and OH -(H 2 O) 3-7 at well-defined cluster temperatures are presented. The feasibility of using this ion trap to acquire temperaturedependent infrared spectra of charged water clusters is also demonstrated with H + (H 2 O) 6 .

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Collisions of FeO⁺ with H₂ and He in a Cryogenic Ion Trap

et al. 2016

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The nominal temperature range of cryogenic radio-frequency ion traps has recently been extended down to T=2.3 K. Whereas in situ He tagging of mass-selected ions embedded in dense helium buffer gas is becoming common for recording IR spectra through photofragmentation of small and large ions, much less activity is devoted to the field of cold chemistry, which in this contribution means the two orders of magnitude extending from 300 to below 3 K. The importance of this temperature range for understanding the dynamics of bi- and termolecular reactions is illustrated with new results for the time-honored reaction of FeO with H obtained with the cryogenic ion trap ISORI in Prague. The rate coefficient for forming Fe +H O increases steeply with decreasing temperature. In addition more product channels open up, such as the stabilized reaction-intermediate complexes H FeO and He -FeO formed by ternary association with He. For the FeOH +H channel only a minor signal is observed. The rate coefficients provide deep insight into lifetimes, bottlenecks, and barriers impeding almost completely the exothermic, but spin-forbidden, reaction at room temperature. For some of the He-tagged ions, IR predissociation spectra are recorded. A breakthrough is obtaining the first spectrum of [(H )FeO] , synthesized and tagged in situ with He. These results pave the way to study the structures of reaction intermediates stabilized in the gas phase by means of collisions with helium.

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On the dynamics of the reaction of positive hydrogen cluster ions (H5+ to H23+) with para and normal hydrogen at 10 K

Cited by 64 publications

References 30 publications

On the formation mechanisms of hydrogen ionic clusters

On the formation mechanisms of hydrogen ionic clusters

Investigations of Protonated and Deprotonated Water Clusters Using a Low-Temperature 22-Pole Ion Trap

Collisions of FeO⁺ with H₂ and He in a Cryogenic Ion Trap

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On the dynamics of the reaction of positive hydrogen cluster ions (H5+ to H23+) with para and normal hydrogen at 10 K

Cited by 64 publications

References 30 publications

On the formation mechanisms of hydrogen ionic clusters

On the formation mechanisms of hydrogen ionic clusters

Investigations of Protonated and Deprotonated Water Clusters Using a Low-Temperature 22-Pole Ion Trap

Collisions of FeO+ with H2 and He in a Cryogenic Ion Trap

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Collisions of FeO⁺ with H₂ and He in a Cryogenic Ion Trap