Velocity- and mass-resolved REMPI spectroscopy of van der Waals molecules. A technique for determining the cluster size responsible for spectral features

Sampson, Rebecca K; Bellm, Susan; Gascooke, Jason R.; Lawrance, Warren D.

doi:10.1016/s0009-2614(03)00154-4

Cited by 16 publications

(33 citation statements)

References 11 publications

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“…26 We have shown previously 26 that one can easily distinguish parent from offspring ions in such an experiment because the parent ions only appear at the image center, since they have no orthogonal momentum component as occurs for dissociation products. This provides a means to assign whether the signal observed at the NO-Ar mass originates from NO-Ar or from higher clusters that have undergone dissociation.…”

Section: E Spectral Observation Of High-lying No-ar X Statesmentioning

confidence: 99%

The dissociation of NO–Ar(Ã) from around threshold to 200 cm−1 above threshold

Holmes-Ross

Lawrance

2010

The Journal of Chemical Physics

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We report an investigation of the dissociation of Ã state NO-Ar at energies from 23 cm −1 below the dissociation energy to 200 cm −1 above. The NO product rotational distributions show population in states that are not accessible with the energy available for excitation from the NO ground state. This effect is observed at photon energies from below the dissociation energy up to approximately 100 cm −1 above it. Translational energy distributions, extracted from velocity map images of individual rotational levels of the NO product, reveal contributions from excitation of high energy NO-Ar X states at all the excess energies probed, although this diminishes with increasing photon energy and is quite small at 200 cm −1 , the highest energy studied. These translational energy distributions show that there are contributions arising from population in vibrational levels up to the X state dissociation energy. We propose that the reason such sparsely populated levels contribute to the observed dissociation is a considerable increase in the transition moment, via the FranckCondon factor associated with these highly excited states, which arises because of the quite different geometries in the NO-Ar X and Ã states. This effect is likely to arise in other systems with similarly large geometry changes.

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Section: E Spectral Observation Of High-lying No-ar X Statesmentioning

confidence: 99%

The dissociation of NO–Ar(Ã) from around threshold to 200 cm−1 above threshold

Holmes-Ross

Lawrance

2010

The Journal of Chemical Physics

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“…In Überschallexpansionen existiert BA 2 in zwei isomeren Formen, von denen aber bisher nur eine mithilfe von IR-Spektroskopie charakterisiert werden konnte. [7,8] Hier präsentieren wir erstmalig das IRSpektrum des anderen Isomers. Dieses Isomer hat eine doppelt T-förmige Struktur, wie sie sich auch im Cokristall entlang der c-Achse findet (Abbildung 1).…”

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“…Mithilfe der resonanten Zweiphotonenionisationsspektroskopie (R2PI) [7,8,12,13] [14] bei 38 606 cm À1 nachgewiesen werden. Die Blauverschiebung in den UV-Spektren deutet auf eine verminderte Clusterstabilität im elektronisch angeregten Zustand hin, die durch eine aus der pp*-Anregung resultierende, niedrigere Elektronendichte im Benzolring zustandekommt, wie es bei anderen Clustern mit Wasserstoffbrücken zum aromatischen p-System beobachtet wurde.…”

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Isomerenselektive IR‐Spektroskopie von Benzol‐Acetylen‐Clustern: Vergleich mit der Struktur des Benzol‐Acetylen‐Cokristalls

et al. 2008

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“…17 Here, the center of each image and a surrounding annulus are integrated separately. DFB ions originating from dissociation of the complex gain kinetic energy and contribute intensity away from the center of the image, i.e., in the annulus.…”

Section: Methodsmentioning

confidence: 99%

“…10 Through the use of velocity and mass resolved REMPI, 17 we identified a weak feature at 0 0 0 + 823 cm −1 as the first band from which dissociation was detected. The truncated distribution gave a maximum excess energy of 37Ϯ 4 cm −1 ; the corresponding binding energies are given in Table II.…”

Section: A Dfb-water Binding Energiesmentioning

confidence: 96%

A velocity map ion imaging study of difluorobenzene-water complexes: Binding energies and recoil distributions

Bellm

Leeuwen

Lawrance

2008

The Journal of Chemical Physics

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The binding energies of the p-, m-, and o-difluorobenzene-H2O complexes have been measured by velocity map ion imaging to be 922±10, 945±10, and 891±4cm−1, respectively. The lack of variation provides circumstantial evidence for water binding to the three isomers via the same interaction, viz. an in-plane O–H⋯F hydrogen bond to one of the fluorine atoms on the ring, with a second, weaker interaction of the water O atom with an ortho hydrogen, as determined previously for the p-difluorobenzene-H2O complex [Kang et al., J. Phys. Chem. A 109, 767 (2005)]. The ground state binding energies for the difluorobenzene-H2O complexes are ∼5%–11% larger than that for benzene-H2O, where binding occurs to the π electrons out-of-plane. However, in the S1 state the binding energies of the o- and p-difluorobenzene-H2O complexes are smaller than the benzene-H2O value, raising an interesting question about whether the geometry at the global energy minimum remains in-plane in the excited electronic states of these two complexes. Recoil energy distributions for dissociation of p-difluorobenzene-H2O have been measured from the 31¯, 52¯, and 3151¯ levels of the excited electronic state. These levels are 490, 880, and 1304cm−1, respectively, above the dissociation threshold. Within the experimental uncertainty, the recoil energy distributions are the same for dissociation from these three states, with average recoil energies of ∼100cm−1. These recoil energies are 60% larger than was observed for the dissociation of p-difluorobenzene-Ar, which is a substantially smaller increase than the 400% seen in a comparable study of dissociation within the triplet state for pyrazine-Ar, -H2O complexes. The majority of the available energy is partitioned into vibration and rotation of the fragments.

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Velocity- and mass-resolved REMPI spectroscopy of van der Waals molecules. A technique for determining the cluster size responsible for spectral features

Cited by 16 publications

References 11 publications

The dissociation of NO–Ar(Ã) from around threshold to 200 cm−1 above threshold

The dissociation of NO–Ar(Ã) from around threshold to 200 cm−1 above threshold

Isomerenselektive IR‐Spektroskopie von Benzol‐Acetylen‐Clustern: Vergleich mit der Struktur des Benzol‐Acetylen‐Cokristalls

A velocity map ion imaging study of difluorobenzene-water complexes: Binding energies and recoil distributions

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