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Register a new userCarbon isotopic fractionation in molecular clouds
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C-fractionation has been studied from a theoretical point of view with different models of time-dependent chemistry, including both isotope-selective photodissociation and low-temperature isotopic exchange reactions. Recent chemical models predict that the latter may lead to a depletion of $^{13}$C in nitrile-bearing species, with $^{12}$C/$^{13}$C ratios two times higher than the elemental abundance ratio of 68 in the local ISM. Since the carbon isotopic ratio is commonly used to evaluate the $^{14}$N/$^{15}$N ratios with the double-isotope method, it is important to study C-fractionation in detail to avoid incorrect assumptions. In this work we implemented a gas-grain chemical model with new isotopic exchange reactions and investigated their introduction in the context of dense and cold molecular gas. In particular, we investigated the $^{12}$C/$^{13}$C ratios of HNC, HCN, and CN using a grid of models, with temperatures and densities ranging from 10 to 50 K and 2$times$10$^{3}$ to 2$times$10$^{7}$ cm$^{-3}$, respectively. We suggest a possible $^{13}$C exchange through the $^{13}$C + C$_{3}$ $rightarrow$ $^{12}$C +$^{13}$CC$_{2}$ reaction, which does not result in dilution, but rather in $^{13}$C enhancement, for molecules formed starting from atomic carbon. This effect is efficient in a range of time between the formation of CO and its freeze-out on grains. Furthermore, we show that the $^{12}$C/$^{13}$C ratios of nitriles are predicted to be a factor 0.8-1.9 different from the local value of 68 for massive star-forming regions. This result also affects the $^{14}$N/$^{15}$N ratio: a value of 330 obtained with the double-isotope method is predicted to be 260-1150, depending on the physical conditions. Finally, we studied the $^{12}$C/$^{13}$C ratios by varying the cosmic-ray ionization rate: the ratios increase with it because of secondary photons and cosmic-ray reactions.
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We have developed the first gas-grain chemical model for oxygen fractionation (also including sulphur fractionation) in dense molecular clouds, demonstrating that gas-phase chemistry generates variable oxygen fractionation levels, with a particularly strong effect for NO, SO, O2, and SO2. This large effect is due to the efficiency of the neutral 18O + NO, 18O + SO, and 18O + O2 exchange reactions. The modeling results were compared to new and existing observed isotopic ratios in a selection of cold cores. The good agreement between model and observations requires that the gas-phase abundance of neutral oxygen atoms is large in the observed regions. The S16O/S18O ratio is predicted to vary substantially over time showing that it can be used as a sensitive chemical proxy for matter evolution in dense molecular clouds.
Context. The increased sensitivity and high spectral resolution of millimeter telescopes allow the detection of an increasing number of isotopically substituted molecules in the interstellar medium. The 14N/ 15N ratio is difficult to measure directly for carbon containing molecules. Aims. We want to check the underlying hypothesis that the 13C/ 12C ratio of nitriles and isonitriles is equal to the elemental value via a chemical time dependent gas phase chemical model. Methods. We have built a chemical network containing D, 13C and 15N molecular species after a careful check of the possible fractionation reactions at work in the gas phase. Results. Model results obtained for 2 different physical conditions corresponding respectively to a moderately dense cloud in an early evolutionary stage and a dense depleted pre-stellar core tend to show that ammonia and its singly deuterated form are somewhat enriched in 15N, in agreement with observations. The 14N/ 15N ratio in N2H+ is found to be close to the elemental value, in contrast to previous models which obtain a significant enrichment, as we found that the fractionation reaction between 15N and N2H+ has a barrier in the entrance channel. The large values of the N2H+/15NNH+ and N2H+/ N15NH+ ratios derived in L1544 cannot be reproduced in our model. Finally we find that nitriles and isonitriles are in fact significantly depleted in 13C, questioning previous interpretations of observed C15N, HC15N and H15NC abundances from 13C containing isotopologues.
Using the Green Bank Telescope (GBT), we have obtained accurate measurements of the $^{14}$N/$^{15}$N isotopic ratio in ammonia in two nearby cold, dense molecular clouds, Barnard~1 and NGC 1333. The $^{14}$N/$^{15}$N ratio in Barnard~1, $334 pm 50$ (3$sigma$), is particularly well constrained and falls in between the local interstellar medium/proto-solar value of $sim 450$ and the terrestrial atmospheric value of 272. The NGC 1333 measurement is consistent with the Barnard~1 result, but has a larger uncertainty. We do not see evidence for the very high $^{15}$N enhancements seen in cometary CN. Sensitive observations of a larger, carefully selected sample of prestellar cores with varying temperatures and gas densities can significantly improve our understanding of the nitrogen fractionation in the local interstellar medium and its relation to the isotopic ratios measured in various solar system reservoirs.
We have carried out observations of CCH and its two $^{13}$C isotopologues, $^{13}$CCH and C$^{13}$CH, in the 84 - 88 GHz band toward two starless cores, L1521B and L134N (L183), using the Nobeyama 45 m radio telescope. We have detected C$^{13}$CH with a signal-to-noise (S/N) ratio of 4, whereas no line of $^{13}$CCH was detected in either the dark clouds. The column densities of the normal species were derived to be ($1.66 pm 0.18$)$times 10^{14}$ cm$^{-2}$ and ($7.3 pm 0.9$)$times 10^{13}$ cm$^{-2}$ ($1 sigma$) in L1521B and L134N, respectively. The column density ratios of $N$(C$^{13}$CH)/$N$($^{13}$CCH) were calculated to be $>1.1$ and $>1.4$ in L1521B and L134N, respectively. The characteristic that $^{13}$CCH is less abundant than C$^{13}$CH is likely common for dark clouds. Moreover, we find that the $^{12}$C/$^{13}$C ratios of CCH are much higher than those of HC$_{3}$N in L1521B by more than a factor of 2, as well as in Taurus Molecular Cloud-1 (TMC-1). In L134N, the differences in the $^{12}$C/$^{13}$C ratios between CCH and HC$_{3}$N seem to be smaller than those in L1521B and TMC-1. We discuss the origins of the $^{13}$C isotopic fractionation of CCH and investigate possible routes that cause the significantly high $^{12}$C/$^{13}$C ratio of CCH especially in young dark clouds, with the help of chemical simulations. The high $^{12}$C/$^{13}$C ratios of CCH seem to be caused by reactions between hydrocarbons (e.g., CCH, C$_{2}$H$_{2}$, $l,c$-C$_{3}$H) and C$^{+}$.
We upgraded the chemical network from the UMIST Database for Astrochemistry 2006 to include isotopes such as ^{13}C and ^{18}O. This includes all corresponding isotopologues, their chemical reactions and the properly scaled reaction rate coefficients. We study the fractionation behavior of astrochemically relevant species over a wide range of model parameters, relevant for modelling of photo-dissociation regions (PDRs). We separately analyze the fractionation of the local abundances, fractionation of the total column densities, and fractionation visible in the emission line ratios. We find that strong C^+ fractionation is possible in cool C^+ gas. Optical thickness as well as excitation effects produce intensity ratios between 40 and 400. The fractionation of CO in PDRs is significantly different from the diffuse interstellar medium. PDR model results never show a fractionation ratio of the CO column density larger than the elemental ratio. Isotope-selective photo-dissociation is always dominated by the isotope-selective chemistry in dense PDR gas. The fractionation of C, CH, CH^+, and HCO^+ is studied in detail, showing that the fractionation of C, CH and CH^+ is dominated by the fractionation of their parental species. The light hydrides chemically derive from C^+, and, consequently, their fractionation state is coupled to that of C^+. The fractionation of C is a mixed case depending on whether formation from CO or HCO^+ dominates. Ratios of the emission lines of [C II], [C I], ^{13}CO, and H^{13}CO^+ provide individual diagnostics to the fractionation status of C^+, C, and CO.
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