J. Semaniak

An enhanced cosmic-ray flux towards ζ Persei inferred from a laboratory study of the H3+ – e- recombination rate

The H3+ molecular ion plays a fundamental role in interstellar chemistry, as it initiates a network of chemical reactions that produce many molecules. In dense interstellar clouds, the H3+ abundance is understood using a simple chemical model, from which observations of H3+ yield valuable estimates of cloud path length, density and temperature. But observations of diffuse clouds have suggested that H3+ is considerably more abundant than expected from the chemical models. Models of diffuse clouds have, however, been hampered by the uncertain values of three key parameters: the rate of H3+ destruction by electrons (e-), the electron fraction, and the cosmic-ray ionization rate. Here we report a direct experimental measurement of the H3+ destruction rate under nearly interstellar conditions. We also report the observation of H3+ in a diffuse cloud (towards ζ Persei) where the electron fraction is already known. From these, we find that the cosmic-ray ionization rate along this line of sight is 40 times faster than previously assumed. If such a high cosmic-ray flux is ubiquitous in diffuse clouds, the discrepancy between chemical models and the previous observations of H3+ can be resolved.

Enhanced cosmic-ray flux toward zeta Persei inferred from laboratory study of H3+ - e- recombination rate

The H3+ molecular ion plays a fundamental role in interstellar chemistry, as it initiates a network of chemical reactions that produce many molecules. In dense interstellar clouds, the H3+ abundance is understood using a simple chemical model, from which observations of H3+ yield valuable estimates of cloud path length, density and temperature. But observations of diffuse clouds have suggested that H3+ is considerably more abundant than expected from the chemical models. Models of diffuse clouds have, however, been hampered by the uncertain values of three key parameters: the rate of H3+ destruction by electrons (e-), the electron fraction, and the cosmic-ray ionization rate. Here we report a direct experimental measurement of the H3+ destruction rate under nearly interstellar conditions. We also report the observation of H3+ in a diffuse cloud (towards ζ Persei) where the electron fraction is already known. From these, we find that the cosmic-ray ionization rate along this line of sight is 40 times faster than previously assumed. If such a high cosmic-ray flux is ubiquitous in diffuse clouds, the discrepancy between chemical models and the previous observations of H3+ can be resolved.

Dissociative recombination of D3O+ and H3O+: Absolute cross sections and branching ratios

Dissociative recombination of the polyatomic ions D3O+ and H3O+ with electrons have been studied at the heavy-ion storage ring CRYRING (Manne Siegbahn Laboratory, Stockholm University). Absolute cross sections have been determined from 0.001 eV to 0.25 eV center-of-mass energy for D3O+ and from 0.001 eV to 28 eV for H3O+. The cross sections are large (7.3×10−13 cm2 for D3O+ and 3.3×10−12 cm2 for H3O+ at 0.001 eV). At low energies, the cross sections for D3O+ are E−1 energy dependent whereas it is slightly steeper for H3O+. A similar E−1 energy dependence was also observed by Mul et al. [J. Phys. B 16, 3099 (1983)] with a merged electron-ion beam technique for both H3O+ and D3O+ and by Vejby-Christensen et al. [Astrophys. J. 483, 531 (1997)] with the ASTRID storage ring in Denmark, who presented relative cross sections for H3O+. A resonance has been observed around 11 eV for H3O+. It reflects an electron capture to Rydberg states converging to an excited ionic core. A similar structure was reported by Vejb...

Dissociative recombination and excitation of O2+: Cross sections, product yields and implications for studies of ionospheric airglows

We present experimental data on the dissociative recombination (DR) and the dissociative excitation (DE) of O2+ in its electronic and vibrational ground state using a heavy ion storage ring. The absolute DR cross section has been determined over an electron collision energy range from 1 meV to 3 eV. The thermal DR rate coefficient is derived; α(Te)=2.4×10−7(300/Te)0.70±0.01 cm3 s−1, for T>200 K. The threshold for DE was observed near its energetic threshold of 6.7 eV. The DE cross section curve has a maximum of 3×10−16 cm2 near 15 eV. We have determined the branching fractions to the different dissociation limits and present atomic quantum yields for the DR process between 0 to 300 meV collision energy. The quantum yield of O(1D) is found to be 1.17±0.05, largely independent of the electron energy. Arguments are presented that the branching fraction to O(3P)+O(1S) is negligible. The branching fraction to the O(1S)+O(1D) is smaller than 0.06 and varies strongly as a function of collision energy. The O(1S) ...

Dissociative Recombination of N2H+: Evidence for Fracture of the N-N Bond

Branching ratios and absolute cross sections have been measured for the dissociative recombination of N2H+ using the CRYRING ion storage ring. It has been found that the channel N2H+ + e- → N2 + H accounts for only 36% of the total reaction and that the branching into the other exoergic pathway, N2H+ + e- → NH + N, consequently amounts to 64%. The cross section of the reaction could be fitted by the expression σ = (2.4 ± 0.4) × 10-16E-1.04±0.02 cm2, which leads to a thermal reaction rate of k(T) = (1.0 ± 0.2) × 10-7(T/300)-0.51±0.02 cm3 s-1, in favorable agreement with previous flowing afterglow Langmuir probe measurements at room temperature, although our temperature dependence is very different. The implications of these measurements for the chemistry of interstellar clouds are discussed. A standard model calculation for a dark cloud predicts a slight increase of N2H+ in the dark clouds but a five- to sevenfold increase of the NH concentration as steady state is reached.

Dissociative Recombination and Excitation of CH5+: Absolute Cross Sections and Branching Fractions

The heavy-ion storage ring CRYRING was used to measure the absolute dissociative recombination and dissociative excitation cross sections for collision energies below 50 eV. Deduced thermal rates coefficients are consistent with previous beams data but are lower by a factor of 3 than the rates measured by means of the flowing afterglow Langmuir probe technique. A resonant structure in dissociative recombination cross section was found at 9 eV. We have determined the branching fractions in DR of CH+5 below 0.2 eV. The branching is dominated by three-body CH3 + H + H and CH2 + H2 + H dissociation channels, which occur with branching ratios of ≈ 0.7 and ≈ 0.2, respectively; thus methane is a minor species among dissociation products. Both the measured absolute cross sections and branching in dissociative recombination of CH+5 can have important implications for the models of dense interstellar clouds and abundance of CH2, CH3 and CH4 in these media.

Branching Fractions in Dissociative Recombination of CH2

The absolute cross section and branching ratios for dissociative recombination of CH -->+2 with electrons have been measured by means of the heavy-ion storage ring CRYRING. Contrary to what has been previously believed, recombination of CH -->+2 is dominated by the three-body channel C + H + H (63%), whereas breakup into the CH + H and C + H2 channels occurs with branching ratios of 25% and 12%, respectively. The thermal rate coefficient for dissociative recombination at 300 K is 6.4 × 10-7 cm3 s-1, which is higher by a factor of 2.5 than the value used in modeling dark molecular clouds. The low CH production and the high production of energetic carbon atoms could be favorable factors for the turbulence model to explain the large abundance of interstellar CH+. The cross section for dissociative excitation was also measured and found to be in good agreement with results from a crossed electron-ion beam experiment.

Branching Fractions in Dissociative Recombination of CH{sup {plus}} {sub 2}

The absolute cross section and branching ratios for dissociative recombination of CH -->+2 with electrons have been measured by means of the heavy-ion storage ring CRYRING. Contrary to what has been previously believed, recombination of CH -->+2 is dominated by the three-body channel C + H + H (63%), whereas breakup into the CH + H and C + H2 channels occurs with branching ratios of 25% and 12%, respectively. The thermal rate coefficient for dissociative recombination at 300 K is 6.4 × 10-7 cm3 s-1, which is higher by a factor of 2.5 than the value used in modeling dark molecular clouds. The low CH production and the high production of energetic carbon atoms could be favorable factors for the turbulence model to explain the large abundance of interstellar CH+. The cross section for dissociative excitation was also measured and found to be in good agreement with results from a crossed electron-ion beam experiment.

Dissociative recombination of NH4+ and ND4+ ions: storage ring experiments and ab initio molecular dynamics.

The dissociative recombination (DR) process of NH4+ and ND4+ molecular ions with free electrons has been studied at the heavy-ion storage ring CRYRING (Manne Siegbahn Laboratory, Stockholm University). The absolute cross sections for DR of NH4+ and ND4+ in the collision energy range 0.001-1 eV are reported, and thermal rate coefficients for the temperature interval from 10 to 2000 K are calculated from the experimental data. The absolute cross section for NH4+ agrees well with earlier work and is about a factor of 2 larger than the cross section for ND4+. The dissociative recombination of NH4+ is dominated by the product channels NH3+H (0.85+/-0.04) and NH2+2H (0.13+/-0.01), while the DR of ND4+ mainly results in ND3+D (0.94+/-0.03). Ab initio direct dynamics simulations, based on the assumption that the dissociation dynamics is governed by the neutral ground-state potential energy surface, suggest that the primary product formed in the DR process is NH3+H. The ejection of the H atom is direct and leaves the NH3 molecule highly vibrationally excited. A fraction of the excited ammonia molecules may subsequently undergo secondary fragmentation forming NH2+H. It is concluded that the model results are consistent with gross features of the experimental results, including the sensitivity of the branching ratio for the three-body channel NH2+2H to isotopic exchange.

DISSOCIATIVE RECOMBINATION OF NITRILE IONS: DCCCN + AND DCCCND +

Branching ratios and absolute cross sections have been measured for the dissociative recombination of DCCCN+ and DCCCND+ using the CRYRING ion storage ring. In the case of DCCCN+ the dissociation y ...