The photofragmentation dynamics of 1,1,1,2-tetrafluoroethane (R134a) with photon energies from 12 eV up to 320 eV, surrounding the C 1s edge is discussed. The ionic moieties were measured in coincidence with the ejected electrons (PEPICO mode), and detected as a function of the photon energy. Around the C K core edge, the fragmentation profiles are examined regarding the site specific excitation of the CH2FCF3 molecule. In the present case, site-selectivity is favored by the distinct chemical environments surrounding both C atoms. NEXAFS spectrum at the C 1s edge simulation has been obtained at the TDDFT level and excited state geometry optimization calculations have been performed at the inner-shell multiconfigurational self-consistent field level. Our observations indicate that the C(H2F) 1s excitation to a highly repulsive potential expels a fluorine atom leaving the heavier radical fragment C2F3H2* which relaxes to the fundamental state of the ion C2F3H2 +. On the other hand, the excitation from the C(F3) 1s carbon to a repulsive state in the C–C bond, leads to a C–C bond cleavage, explaining the observed site specific fragmentation.
We have performed an experimental investigation into the interaction of vacuum-ultraviolet synchrotron radiation with pyridine molecules in the gas phase. Specifically, a double-ion chamber spectrometer was used to measure the absolute photoabsorption cross sections and the photoionization quantum yields from the ionization threshold to 21.5 eV. Moreover, photoionization and neutral-decay cross sections in absolute scale were derived from these data. In addition, the fragmentation pattern was investigated as a function of the photon energy by using a time-of-flight mass spectrometer and the photoelectron-photoion coincidence technique. Thus, the absolute partial ionization cross sections for each ionic fragment were obtained. Comparisons are made with experimental data available in the literature.
We discuss the use of a region of uniform and constant magnetic field in order to implement a two-state atomic polarizer for an H(2S) beam. We have observed that a device with such field configuration is capable of achieving an efficient polarization for a wide range of magnetic field intensities and atomic velocities. In addition, we establish a criterion that must be met to confirm a successful polarization. That is possible due to a specific beating pattern for the Lyman-α radiation expected for the outgoing two-state atomic beam.
An experimental investigation of the processes leading tothe fragmentation of the singly ionized 1,1,1,2-tetrafluoroethane (HFC-134a, CH2FCF3) by EUV and soft X-rays is presented. HFC-134ais taken into consideration as the most convenient replacement for CFC-12 in refrigeration applications due to the fact that it has null ozone depletion factor. Dissociation of the singly ionized HFC-134amolecule was induced by valence, direct and indirect C 1s core photoionization or photoexcitation and the ionic fragments were detected in coincidence (PEPICO mode) with the ejected electrons without energy analysis. The singly ionized parent ion CF4CH2+can be detected even at photon energies above the C 1s threshold.
In this work we investigate the single-photon double ionization of the SUVA 134a (1,1,1,2-tetrafluoroethane) molecule in the energy range from 21.21 to 320 eV. Our experimental data are supported by Thomas' and Samson's models. It is shown that the double photoionization of the SUVA 134a can be expressed as a sum of the so-called shake-off (SO) and the knockout (KO) processes. Methods:The experiments were executed at the TGM beamline at Laborat orio Nacional de Luz Síncrotron in Campinas, Brazil. The source of EUV and X-ray radiation was a bending magnet that enabled us to work in the photon energy range of 21.21 to 320 eV. The spectrometer was devised to collect 100% of the ions with kinetic energies up to 30 eV. The photoelectron-photoion (PEPICO) and photoelectron-photoion-photoion (PE2PICO) coincidence techniques were used in the present work. Results:The ratio of double-to-total photoionization as a function of the photon energy for the SUVA molecule exhibits remarkably similar behavior with other atomic and molecular systems. SO depends on large excess energy above the ionization threshold, enabling the photoelectron to leave the interaction region rather speedily to yield a sudden change in the Coulomb field that the shaken electron feels. The measured asymptotic SO probability is P SO (∞) = 0.09. Conclusions:The present analysis shows that the separation of SO and KO processes relies on the experimental evidence that there is no significant interference between SO and KO. The analysis also shows that the separate formulation of KO and SO presents a factual portrayal of double photoionization.Despite having 50 electrons, SUVA has lower double-to-total photoionization fraction (9%) in comparison, for instance, to argon atoms ($20%), which has 18 electrons. This lower e-e correlation could be attributed to its larger volume, that is, lower electron density. | INTRODUCTIONAt low photon energies (EUV), photo-double ionization of atoms and molecules is a rare event, corresponding to only a small percentage when compared to single ionization. It can take place either directly or indirectly. Photo-double ionization of atoms and molecules by a single photon is a central many-body process. Direct double ionization is portrayed by a single photon absorption by the target followed by the sudden ejection of two electrons, as opposed to sequential or indirect core ionization or excitation followed by a series of Auger decays, or
We show that two-particle interferences can be used to probe the nuclear motion in a doublyexcited hydrogen molecule. The dissociation of molecular hydrogen by electron impact involves several decay channels, associated to different molecular rotational states, which produce quantum interferences in the detection of the atomic fragments. Thanks to the correlations between the angular momentum and vibrational states of the molecule, the fragments arising from each dissociation channel carry out a phase-shift which is a signature of the molecule rotation. These phase-shifts, which cannot be observed in a single-atom detection scheme, may be witnessed in realistic experimental conditions in a time-of-flight coincidence measurement. We analyse the interferences arising from the two lowest-energy rotational states of a para-hydrogen molecule. Our result shows the relevance of two-fragments correlations to track the molecular rotation.
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