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Register a new userDirect measurement of desorption and diffusion energies of O and N atoms physisorbed on amorphous surfaces
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Physisorbed atoms on the surface of interstellar dust grains play a central role in solid state astrochemistry. Their surface reactivity is one source of the observed molecular complexity in space. In experimental astrophysics, the high reactivity of atoms also constitutes an obstacle to measuring two of the fundamental properties in surface physics, namely desorption and diffusion energies, and so far direct measurements are non-existent for O and N atoms. We investigated the diffusion and desorption processes of O and N atoms on cold surfaces in order to give boundary conditions to astrochemical models. Here we propose a new technique for directly measuring the N- and O-atom mass signals. Including the experimental results in a simple model allows us to almost directly derive the desorption and diffusion barriers of N atoms on amorphous solid water ice (ASW) and O atoms on ASW and oxidized graphite. We find a strong constraint on the values of desorption and thermal diffusion energy barriers. The measured barriers for O atoms are consistent with recent independent estimations and prove to be much higher than previously believed (E$_{des}=1410_{-160}^{+290}$; E$_{dif}=990_{-360}^{+530}$ K on ASW). As for oxygen atoms, we propose that the combination E$_{des}$-E$_{dif}$=1320-750 K is a sensible choice among the possible pairs of solutions. Also, we managed to measure the desorption and diffusion energy of N atoms for the first time (E$_{des}=720_{-80}^{+160}$; E$_{dif}=525_{-200}^{+260}$ K on ASW) in the thermal hopping regime and propose that the combination E$_{des}$-E$_{dif}$=720-400 K can be reasonably adopted in models. The value of E$_{dif}$ for N atoms is slightly lower than previously suggested, which implies that the N chemistry on dust grains might be richer.
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The abundance of interstellar ice constituents is usually expressed with respect to the water ice because, in denser regions, a significant portion of the interstellar grain surface would be covered by water ice. The binding energy (BE), or adsorption energy of the interstellar species regulates the chemical complexity of the interstellar grain mantle. Due to the high abundance of water ice, the BE of surface species with the water is usually provided and widely used in astrochemical modeling. However, the hydrogen molecules would cover some part of the grain mantle in the denser and colder part of the interstellar medium. Even at around ~ 10K, few atoms and simple molecules with lower adsorption energies can migrate through the surface. The BE of the surface species with H2 substrate would be very different from that of a water substrate. However, adequate information regarding these differences is lacking. Here, we employ the quantum chemical calculation to provide the BE of 95 interstellar species with H2 substrate. These are representative of the BEs of species to a H2 overlayer on a grain surface. On average, we notice that the BE with the H2 monomer substrate is almost ten times lower than the BE of these species reported earlier with the H2 O c-tetramer configuration. The encounter desorption of H and H2 was introduced (with ED (H, H2 ) =45 K and ED (H2 , H2 ) =23 K) to have a realistic estimation of the abundances of the surface species in the colder and denser region. Our quantum chemical calculations yield higher adsorption energy of H2 than that of H (ED (H, H2 ) = 23 - 25 K and ED (H2, H2 ) =67 - 79 K). We further implement an astrochemical model to study the effect of encounter desorption with the resent realistic estimation. The encounter desorption of the N atom (calculations yield ED (N, H2 ) =83 K) is introduced to study the differences with its inclusion.
Any evolving system can change of state via thermal mechanisms (hopping a barrier) or via quantum tunneling. Most of the time, efficient classical mechanisms dominate at high temperatures. This is why an increase of the temperature can initiate the chemistry. We present here an experimental investigation of O-atom diffusion and reactivity on water ice. We explore the 6-25 K temperature range at sub-monolayer surface coverages. We derive the diffusion temperature law and observe the transition from quantum to classical diffusion. Despite of the high mass of O, quantum tunneling is efficient even at 6 K. As a consequence, the solid-state astrochemistry of cold regions should be reconsidered and should include the possibility of forming larger organic molecules than previously expected.
Neutrons produced by the carbon fusion reaction 12C(12C,n)23Mg play an important role in stellar nucleosynthesis. However, past studies have shown large discrepancies between experimental data and theory, leading to an uncertain cross section extrapolation at astrophysical energies. We present the first direct measurement that extends deep into the astrophysical energy range along with a new and improved extrapolation technique based on experimental data from the mirror reaction 12C(12C,p)23Na. The new reaction rate has been determined with a well-defined uncertainty that exceeds the precision required by astrophysics models. Using our constrained rate, we find that 12C(12C,n)23Mg is crucial to the production of Na and Al in Pop-III Pair Instability Supernovae. It also plays a non-negligible role in the production of weak s-process elements as well as in the production of the important galactic gamma-ray emitter 60Fe.
The thermal desorption of ammonia (NH$_3$) from single crystal forsterite (010) has been investigated using temperature-programmed desorption. The effect of defects on the desorption process has been probed by the use of a rough cut forsterite surface prepared from the cleaved forsterite sample. Several approaches have been used to extract the desorption energy and pre-exponential factor describing the desorption kinetics. In the sub-monolayer coverage regime, the NH$_3$ desorption shows a broad distribution of desorption energies, indicating the presence of different adsorption sites, which results in an apparent coverage-dependent desorption energy. This distribution is sensitive to the surface roughness with the cut forsterite surface displaying a significantly broader distribution of desorption energies compared to the cleaved forsterite surface. The cut forsterite surface exhibits sites with desorption energies up to 62.5 kJ mol$^{-1} $ in comparison to a desorption energy of up to 58.0 kJ mol$^{-1} $ for the cleaved surface. Multilayer desorption is independent of the nature of the forsterite surface used, with a desorption energy of ($25.8pm0.9$) kJ mol$^{-1} $. On astrophysically relevant heating time-scales, the presence of a coverage dependent desorption energy distribution results in a lengthening of the NH$_3$ desorption time-scale by $5.9times 10^4$ yr compared to that expected for a single desorption energy. In addition, the presence of a larger number of high-energy adsorption sites on the rougher cut forsterite surface leads to a further lengthening of ca. 7000 yr.
The Hipparcos orbiting observatory has revealed a large number of helium-core-burning clump stars in the Galactic field. These low-mass stars exhibit signatures of extra-mixing processes that require modeling beyond the first dredge-up of standard models. The 12C/13C ratio is the most robust diagnostic of deep mixing, because it is insensitive to the adopted stellar parameters. In this work we present 12C/13C determinations in a sample of 34 Galactic clump stars as well as abundances of nitrogen, carbon and oxygen. Abundances of carbon were studied using the C2 Swan (0,1) band head at 5635.5 A. The wavelength interval 7980-8130 A with strong CN features was analysed in order to determine nitrogen abundances and 12C/13C isotope ratios. The oxygen abundances were determined from the [O I] line at 6300 A. Compared with the Sun and dwarf stars of the Galactic disk, mean abundances in the investigated clump stars suggest that carbon is depleted by about 0.2 dex, nitrogen is enhanced by 0.2 dex and oxygen is close to abundances in dwarfs. Comparisons to evolutionary models show that the stars fall into two groups: the one is of first ascent giants with carbon isotope ratios altered according to the first dredge-up prediction, and the other one is of helium-core-burning stars with carbon isotope ratios altered by extra mixing. The stars investigated fall to these groups in approximately equal numbers.
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