Deuterium enrichment of ammonia produced by surface N+H/D addition reactions at low temperature

The surface formation of NH3 and its deuterated isotopologues – NH_2D, NHD_2, and ND_3 – is investigated at low temperatures through the simultaneous addition of hydrogen and deuterium atoms to nitrogen atoms in CO-rich interstellar ice analogues. The formation of all four ammonia isotopologues is only observed up to 15 K, and drops below the detection limit for higher temperatures. Differences between hydrogenation and deuteration yields result in a clear deviation from a statistical distribution in favour of deuterium enriched species. The data analysis suggests that this is due to a higher sticking probability of D atoms to the cold surface, a property that may generally apply to molecules that are formed in low temperature surface reactions. The results found here are used to interpret ammonia–deuterium fractionation as observed in pre-protostellar cores

Calculation of The Lifetimes of Thin Stripper Targets Under Bombardment of Intense Pulsed Ions

The problems of stripper target behavior in the nonstationary intense particle beams are considered. The historical sketch of studying of radiation damage failure of carbon targets under ion bombardment is presented. The simple model of evaporation of a target by an intensive pulsing beam is supposed. Stripper foils lifetimes in the nonstationary intense particle can be described by two failure mechanisms: radiation damage accumulation and evaporation of target. At the maximal temperatures less than 2500K the radiation damage are dominated; at temperatures above 2500K the mechanism of evaporation of a foil prevails. The proposed approach has been applied to the discription of behaviour of stripper foils in the BNL linac and SNS conditions.Comment: 12 pages, 5 figure

SURFRESIDE2: An ultrahigh vacuum system for the investigation of surface reaction routes of interstellar interest

Article / Letter to editorSterrewach

H-atom addition and abstraction reactions in mixed CO, H2CO and CH3OH ices: an extended view on complex organic molecule formation

Complex organic molecules (COMs) have been observed not only in the hot cores surrounding low- and high- mass protostars, but also in cold dark clouds. Therefore, it is interesting to understand how such species can be formed without the presence of embedded energy sources. We present new laboratory experiments on the low-temperature solid state formation of three complex molecules: methyl formate (HC(O)OCH3), glycolaldehyde (HC(O)CH2OH) and ethylene glycol (H2C(OH)CH2OH), through recombination of free radicals formed via H-atom addition and abstraction reactions at different stages in the CO-H2CO-CH3OH hydrogenation network at 15 K. The experiments extend previous CO hydrogenation studies and aim at resembling the physical&chemical conditions typical of the CO freeze-out stage in dark molecular clouds, when H2CO and CH3OH form by recombination of accreting CO molecules and H-atoms on ice grains. We confirm that H2CO, once formed through CO hydrogenation, not only yields CH3OH through ongoing H-atom addition reactions, but is also subject to H-atom-induced abstraction reactions, yielding CO again. In a similar way, H2CO is also formed in abstraction reactions involving CH3OH. The dominant methanol H-atom abstraction product is expected to be CH2OH, while H-atom additions to H2CO should at least partially proceed through CH3O intermediate radicals. The occurrence of H-atom abstraction reactions in ice mantles leads to more reactive intermediates (HCO, CH3O and CH2OH) than previously thought, when assuming sequential H-atom addition reactions only. This enhances the probability to form COMs through radical-radical recombination without the need of UV photolysis or cosmic rays as external triggers.Comment: 20 pages, 8 figure

Relevance of the H_2 + O reaction pathway for the surface formation of interstellar water. Combined experimental and modeling study

The formation of interstellar water is commonly accepted to occur on the surfaces of icy dust grains in dark molecular clouds at low temperatures (10–20 K), involving hydrogenation reactions of oxygen allotropes. As a result of the large abundances of molecular hydrogen and atomic oxygen in these regions, the reaction H_2 + O has been proposed to contribute significantly to the formation of water as well. However, gas-phase experiments and calculations, as well as solid-phase experimental work contradict this hypothesis. Here, we use precisely executed temperature-programmed desorption (TPD) experiments in an ultra-high vacuum setup combined with kinetic Monte Carlo simulations to establish an upper limit of the water production starting from H_2 and O. These reactants were brought together in a matrix of CO_2 in a series of (control) experiments at different temperatures and with different isotopological compositions. The water detected with the quadrupole mass spectrometer upon TPD was found to originate mainly from contamination in the chamber itself. However, if water is produced in small quantities on the surface through H_2 + O, this can only be explained by a combined classical and tunneled reaction mechanism. An absolutely conservative upper limit for the reaction rate was derived with a microscopic kinetic Monte Carlo model that converts the upper limit into the highest possible reaction rate. Incorporating this rate into simulation runs for astrochemically relevant parameters shows that the upper limit to the contribution of the reaction H_2 + O in OH, and hence water formation, is 11% in dense interstellar clouds. Our combined experimental and theoretical results indicate, however, that this contribution is most likely much lower

Novel approach to distinguish between vacuum UV-induced ice photodesorption and photoconversion. Investigation of CH_4, CH_3OH, and CH_3CN

Laboratory astrophysics and astrochemistr

Anomalous behavior of the acoustic phonon velocity and elastic constants of relaxor ferroelectric PbMg1/3Ta2/3O3

The behavior of longitudinal acoustic (LA) and transverse acoustic (TA) phonons in a cubic relaxor PbMg1/3Ta2/3O3 (PMT) ferroelectric has been investigated by Brillouin light scattering. Analysis of the temperature dependences of phonon velocity in the temperature range from 50 to 870 K has revealed anomalies in the vicinity of the Burns temperature (TB≈570 K) for LA phonons and a wide frequency-dependent minimum of the velocities of LA and TA phonons in the same temperature region as the dielectric response anomaly. Using experimental data, temperature dependences of the C11 and C44 elastic constants have been calculated. The elastic constants have been found to be frequency-independent in the gigahertz range. The results obtained are discussed in the framework of modern ideas on the crystalline lattice dynamics of relaxor ferroelectrics

Photolysis of Acetonitrile in a Water-rich Ice as a Source of Complex Organic Molecules: CH3CN and H2O:CH3CN Ices

Context. Many C-, O-, and H-containing complex organic molecules (COMs) have been observed in the interstellar medium (ISM) and their formation has been investigated in laboratory experiments. An increasing number of recent detections of large N-bearing COMs motivates our experimental investigation of their chemical origin. Aims. We investigate the potential role of acetonitrile (CH3CN) as a parent molecule to N-bearing COMs, motivated by its omnipresence in the ISM and structural similarity to another well-known precursor species, CH3OH. The aim of the present work is to characterize the chemical complexity that can result from vacuum UV photolysis of a pure CH3CN ice and a more realistic mixture of H2O:CH3CN. Methods. The CH3CN ice and H2O:CH3CN ice mixtures were UV irradiated at 20 K. Laser desorption post ionization time-of-flight mass spectrometry was used to detect the newly formed COMs in situ. We examined the role of water in the chemistry of interstellar ices through an analysis of two different ratios of H2O:CH3CN (1:1 and 20:1). Results. We find that CH3CN is an excellent precursor to the formation of larger nitrogen-containing COMs, including CH3CH2CN, NCCN/CNCN, and NCCH2CH2CN. During the UV photolysis of H2O:CH3CN ice, the water derivatives play a key role in the formation of molecules with functional groups of: imines, amines, amides, large nitriles, carboxylic acids, and alcohols. We discuss possible formation pathways for molecules recently detected in the ISM. © ESO 2021.Acknowledgements. M.B. and H.L. acknowledge the European Union (EU) and Horizon 2020 funding awarded under the Marie Skłodowska-Curie action to the EUROPAH consortium (grant number 722346) as well as NOVA 5 funding. Additional funding has been realized through a NWO-VICI grant. This work has been supported by the Danish National Research Foundation through the Center of Excellence “InterCat” (Grant agreement no.: DNRF150). We thank N. F. W. Ligterink, A. G. G. M. Tielens, J. Terwischa van Scheltinga, J. Bouwman and T. Lamberts for helpful discussions