Evaluation of the exothermicity of the chemi-ionization reaction Sm + O → SmO(+) + e(.)

The exothermicity of the chemi-ionization reaction Sm + O → SmO(+) + e(-) has been re-evaluated through the combination of several experimental methods. The thermal reactivity (300-650 K) of Sm(+) and SmO(+) with a range of species measured using a selected ion flow tube-mass spectrometer apparatus...

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Veröffentlicht in:The Journal of chemical physics 2015-04, Vol.142 (13), p.134307-134307
Hauptverfasser: Cox, Richard M, Kim, JungSoo, Armentrout, P B, Bartlett, Joshua, VanGundy, Robert A, Heaven, Michael C, Ard, Shaun G, Melko, Joshua J, Shuman, Nicholas S, Viggiano, Albert A
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Sprache:eng
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Zusammenfassung:The exothermicity of the chemi-ionization reaction Sm + O → SmO(+) + e(-) has been re-evaluated through the combination of several experimental methods. The thermal reactivity (300-650 K) of Sm(+) and SmO(+) with a range of species measured using a selected ion flow tube-mass spectrometer apparatus is reported and provides limits for the bond strength of SmO(+), 5.661 eV ≤ D0(Sm(+)-O) ≤ 6.500 eV. A more precise value is measured to be 5.725 ± 0.07 eV, bracketed by the observed reactivity of Sm(+) and SmO(+) with several species using a guided ion beam tandem mass spectrometer (GIBMS). Combined with the established Sm ionization energy (IE), this value indicates an exothermicity of the title reaction of 0.08 ± 0.07 eV, ∼0.2 eV smaller than previous determinations. In addition, the ionization energy of SmO has been measured by resonantly enhanced two-photon ionization and pulsed-field ionization zero kinetic energy photoelectron spectroscopy to be 5.7427 ± 0.0006 eV, significantly higher than the literature value. Combined with literature bond energies of SmO, this value indicates an exothermicity of the title reaction of 0.14 ± 0.17 eV, independent from and in agreement with the GIBMS result presented here. The evaluated thermochemistry also suggests that D0(SmO) = 5.83 ± 0.07 eV, consistent with but more precise than the literature values. Implications of these results for interpretation of chemical release experiments in the thermosphere are discussed.
ISSN:0021-9606
1089-7690
DOI:10.1063/1.4916396