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Protonated mixed pyrene-water clusters, (Py) m (H 2 O) n H + , where m=[1-3] and n=[1-10], are generated using a cryogenic molecular cluster source. Subsequently, the mass-selected mixed clusters undergo controlled collisions with rare gases, and the...
We report threshold collision induced dissociation experiments on protonated water clusters thermalized at low temperature for sizes n = 19–23. Fragmentation cross sections are recorded as a function of the collision energy and analyzed with a statistical model. This model allows us to account for dissociation cascades and provides values for the dissociation energies of each cluster. These values, averaging around 0.47 eV, are in good agreement with theoretical predictions at various levels of theory. Furthermore, the dissociation energies show a trend for the n = 21 magic and n = 22 anti-magic numbers relative to their neighbours, which is also in agreement with theory. These results provide further evidence to resolve the disagreement between previously published experimental values. A careful quantitative treatment of cascade dissociation in this model introduces interdependence between the dissociation energies of neighboring sizes, which reduces the number of free fitting parameters and improves both reliability and uncertainties on absolute dissociation energies deduced from experiments.
Entre 1849 et 1851, Hippolyte Fizeau a réalisé successivement trois expériences fondamentales relatives à la vitesse de la lumière. Ce sont toutes trois de véritables tours de force expérimentaux qui ont eu des conséquences majeures dans l’évolution de nos conceptions de la lumière et, comme l’a attesté Albert Einstein lui-même, dans l’avènement de la relativité restreinte. Nous présentons à la fois le contexte et les conséquences historiques ainsi que la réplique moderne que nous avons réalisée de l’expérience de 1851 dite « d’entraînement partiel de l’éther ».
PIRENEA and PIRENEA 2 are experimental setups dedicated to the study of fundamental molecular processes involving species of astrochemical interest. The coupling of a VUV source to PIRENEA has allowed us to study the fragmentation pathways and stability of polycyclic aromatic hydrocarbons (PAHs) containing aliphatic bonds under conditions relevant for astrophysical photodissociation regions. PIRE-NEA 2 will open the possibility to extend these studies to larger systems such as PAH clusters, and more generally to study gas-nanograin-photon interactions.
Sujets
DFT
CID
Collision Induced Dissociation
Agrégat
PAHs
Cross-sections
Cluster
Fonctionnelle
Time of flight mass spectrometry
Bromide
Thermodynamics of small systems
Vibrational states
Thermodynamics
Clusters
SCC-DFTB
Argent
Hydrogen bond
Ab-initio
Models
Bromure
Molecule-molecule collisions
Silver
VUV photoprocessing in PDRs
Polycyclic Aromatic Hydrocarbon Clusters
Collisions
Spectrométrie de masse
Fragmentation
Pyrene Dimer Cation
Phase transitions in clusters
Water
Ab initio
Agrégats
Collision
Molecular clusters
Cryogenic ion trap
Nanocalorimétrie
Mass spectrometry
PST
Heat capacities and heats of phase transitions
Molecular Dynamics
Nanocalorimetry
Thermodynamique
Sections efficaces
Modèle