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N. F. W. Ligterink

Publications and source records attributed to N. F. W. Ligterink.

27 records · Page 2Linked to original sources

The formation of peptide-like molecules on interstellar dust grains

Molecules with an amide functional group resemble peptide bonds, the molecular bridges that connect amino acids, and may thus be relevant in processes that lead to the formation of life. In this study, the solid state formation of some of the smallest amides is investigated in the laboratory. To this end, CH$_{4}$:HNCO ice mixtures at 20 K are irradiated with far-UV photons, where the radiation is used as a tool to produce the radicals required for the formation of the amides. Products are identified and investigated with infrared spectroscopy and temperature programmed desorption mass spectrometry. The laboratory data show that NH$_{2}$CHO, CH$_{3}$NCO, NH$_{2}$C(O)NH$_{2}$, CH$_{3}$C(O)NH$_{2}$ and CH$_{3}$NH$_{2}$ can simultaneously be formed. The NH$_{2}$CO radical is found to be key in the formation of larger amides. In parallel, ALMA observations towards the low-mass protostar IRAS 16293-2422B are analysed in search of CH$_{3}$NHCHO (N-methylformamide) and CH$_{3}$C(O)NH$_{2}$ (acetamide). CH$_{3}$C(O)NH$_{2}$ is tentatively detected towards IRAS 16293-2422B at an abundance comparable with those found towards high-mass sources. The combined laboratory and observational data indicates that NH$_{2}$CHO and CH$_{3}$C(O)NH$_{2}$ are chemically linked and form in the ice mantles of interstellar dust grains. A solid-state reaction network for the formation of these amides is proposed.

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The ALMA-PILS survey: Stringent limits on small amines and nitrogen-oxides towards IRAS 16293-2422B

Hydroxylamine (NH$_{2}$OH) and methylamine (CH$_{3}$NH$_{2}$) have both been suggested as precursors to the formation of amino acids and are therefore of interest to prebiotic chemistry. Their presence in interstellar space and formation mechanisms, however, are not well established. We aim to detect both amines and their potential precursor molecules NO, N$_{2}$O and CH$_{2}$NH towards the low-mass protostellar binary IRAS 16293--2422, in order to investigate their presence and constrain their interstellar formation mechanisms around a young Sun-like protostar. ALMA observations from the unbiased, high angular resolution and sensitivity Protostellar Interferometric Line Survey (PILS) are used. Spectral transitions of the molecules under investigation are searched for with the CASSIS line analysis software. CH$_2$NH and N$_{2}$O are detected for the first time towards a low-mass source, the latter molecule through confirmation with the single-dish TIMASSS survey. NO is also detected. CH$_{3}$NH$_{2}$ and NH$_{2}$OH are not detected and stringent upper limit column densities are determined. The non-detection of CH$_{3}$NH$_{2}$ and NH$_{2}$OH limits the importance of formation routes to amino acids involving these species. The detection of CH$_{2}$NH makes amino acid formation routes starting from this molecule plausible. The low abundances of CH$_2$NH and CH$_{3}$NH$_{2}$ compared to Sgr B2 indicate that different physical conditions influence their formation in low- and high-mass sources.

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The ALMA-PILS survey: first detection of methyl isocyanide (CH$_3$NC) in a solar-type protostar

Methyl isocyanide (CH$_3$NC) is the isocyanide with the largest number of atoms confirmed in the interstellar medium (ISM), but it is not an abundant molecule, having only been detected towards a handful of objects. Conversely, its isomer, methyl cyanide (CH$_3$CN), is one of the most abundant complex organic molecules detected in the ISM, with detections in a variety of low- and high-mass sources. We use ALMA observations from the Protostellar Interferometric Line Survey (PILS) to search for methyl isocyanide and compare its abundance with that of its isomer methyl cyanide. We use a new line catalogue from the Cologne Database for Molecular Spectroscopy (CDMS) to identify methyl isocyanide lines. We also model the chemistry with an updated version of the three-phase chemical kinetics model {\em MAGICKAL}, presenting the first chemical modelling of methyl isocyanide to date. We detect methyl isocyanide for the first time in a solar-type protostar, IRAS 16293$-$2422 B, and present upper limits for its companion protostar, IRAS 16293$-$2422 A. Methyl isocyanide is found to be at least 20 times more abundant in source B compared to source A, with a CH$_3$CN/CH$_3$NC abundance ratio of 200 in IRAS 16293--2422 B and >5517 in IRAS 16293$-$2422 A. We also present the results of a chemical model of methyl isocyanide chemistry in both sources, and discuss the implications on methyl isocyanide formation mechanisms and the relative evolutionary stages of both sources.

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Methanol ice co-desorption as a mechanism to explain cold methanol in the gas-phase

Methanol is formed via surface reactions on icy dust grains. Methanol is also detected in the gas-phase at temperatures below its thermal desorption temperature and at levels higher than can be explained by pure gas-phase chemistry. The process that controls the transition from solid state to gas-phase methanol in cold environments is not understood. The goal of this work is to investigate whether thermal CO desorption provides an indirect pathway for methanol to co-desorb at low temperatures. Mixed CH$_{3}$OH:CO/CH$_{4}$ ices were heated under UHV (ultra-high vacuum) conditions and ice contents are traced using RAIRS (reflection absorption IR spectroscopy), while desorbing species were detected mass spectrometrically. An updated gas-grain chemical network was used to test the impact of the results of these experiments. The physical model used is applicable for TW Hya, a protoplanetary disk in which cold gas-phase methanol has recently been detected. Methanol release together with thermal CO desorption is found to be an ineffective process in the experiments, resulting in an upper limit of $\leq$ 7.3 $\times$ 10$^{-7}$ CH3OH molecules per CO molecule over all ice mixtures considered. Chemical modelling based on the upper limits shows that co-desorption rates as low as 10$^{-6}$ CH$_{3}$OH molecules per CO molecule are high enough to release substantial amounts of methanol to the gas-phase at and around the location of the CO thermal desorption front in a protoplanetary disk. The impact of thermal co-desorption of CH3OH with CO as a grain-gas bridge mechanism is compared with that of UV induced photodesorption and chemisorption.

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First detection of cyanamide (NH$_2$CN) towards solar-type protostars

Searches for the prebiotically-relevant cyanamide (NH$_2$CN) towards solar-type protostars have not been reported in the literature. We here present the first detection of this species in the warm gas surrounding two solar-type protostars, using data from the Atacama Large Millimeter/Submillimeter Array Protostellar Interferometric Line Survey (PILS) of IRAS 16293-2422 B and observations from the IRAM Plateau de Bure Interferometer of NGC1333 IRAS2A. We furthermore detect the deuterated and $^{13}$C isotopologues of NH$_2$CN towards IRAS 16293-2422 B. This is the first detection of NHDCN in the interstellar medium. Based on a local thermodynamic equilibrium analysis, we find that the deuteration of cyanamide ($\sim$ 1.7%) is similar to that of formamide (NH$_2$CHO), which may suggest that these two molecules share NH$_2$ as a common precursor. The NH$_2$CN/NH$_2$CHO abundance ratio is about 0.2 for IRAS 16293-2422 B and 0.02 for IRAS2A, which is comparable to the range of values found for Sgr B2. We explored the possible formation of NH$_2$CN on grains through the NH$_2$ + CN reaction using the chemical model MAGICKAL. Grain-surface chemistry appears capable of reproducing the gas-phase abundance of NH$_2$CN with the correct choice of physical parameters.

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Infrared spectra of complex organic molecules in astronomically relevant ice matrices. I. Acetaldehyde, ethanol, and dimethyl ether

Context. The number of identified complex organic molecules (COMs) in inter- and circumstellar gas-phase environments is steadily increasing. Recent laboratory studies show that many such species form on icy dust grains. At present only smaller molecular species have been directly identified in space in the solid state. Accurate spectroscopic laboratory data of frozen COMs, embedded in ice matrices containing ingredients related to their formation scheme, are still largely lacking. Aims. This work provides infrared reference spectra of acetaldehyde (CH$_3$CHO), ethanol (CH$_3$CH$_2$OH), and dimethyl ether (CH$_3$OCH$_3$) recorded in a variety of ice environments and for astronomically relevant temperatures, as needed to guide or interpret astronomical observations, specifically for upcoming James Webb Space Telescope observations. Methods. Fourier transform transmission spectroscopy (500-4000 cm$^{-1}$ / 20-2.5 $μ$m, 1.0 cm$^{-1}$ resolution) was used to investigate solid acetaldehyde, ethanol and dimethyl ether, pure or mixed with water, CO, methanol, or CO:methanol. These species were deposited on a cryogenically cooled infrared transmissive window at 15~K. A heating ramp was applied, during which IR spectra were recorded until all ice constituents were thermally desorbed. Results. We present a large number of reference spectra that can be compared with astronomical data. Accurate band positions and band widths are provided for the studied ice mixtures and temperatures. Special efforts have been put into those bands of each molecule that are best suited for identification. For acetaldehyde the 7.427 and 5.803 $μ$m bands are recommended, for ethanol the 11.36 and 7.240 $μ$m bands are good candidates, and for dimethyl ether bands at 9.141 and 8.011 $μ$m can be used. All spectra are publicly available in the Leiden Database for Ice.

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The ALMA-PILS survey: Detection of CH$_{3}$NCO toward the low-mass protostar IRAS 16293-2422 and laboratory constraints on its formation

Methyl isocyanate (CH$_{3}$NCO) belongs to a select group of interstellar molecules considered to be relevant precursors in the formation of larger organic compounds, including those with peptide bonds. The molecule has only been detected in a couple of high-mass protostars and potentially on comets. A formation route on icy grains has been postulated for this molecule but experimental evidence is lacking. Here we extend the range of environments where methyl isocyanate is found, and unambiguously identify CH$_{3}$NCO through the detection of 43 unblended transitions in the ALMA Protostellar Interferometric Line Survey (PILS) of the low mass solar-type protostellar binary IRAS 16293-2422. The molecule is detected toward both components of the binary with a ratio HNCO/CH$_3$NCO $\sim$4--12. The isomers CH$_{3}$CNO and CH$_3$OCN are not identified, resulting in upper abundance ratios of CH$_{3}$NCO/CH$_{3}$CNO > 100 and CH$_{3}$NCO/CH$_3$OCN > 10. The resulting abundance ratios compare well with those found for related N-containing species toward high-mass protostars. To constrain its formation, a set of cryogenic UHV experiments is performed. VUV irradiation of CH$_{4}$:HNCO mixtures at 20 K strongly indicate that methyl isocyanate can be formed in the solid-state through CH$_{3}$ and (H)NCO recombinations. Combined with gas-grain models that include this reaction, the solid-state route is found to be a plausible scenario to explain the methyl isocyanate abundances found in IRAS 16293-2422.

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The ALMA-PILS survey: First detections of deuterated formamide and deuterated isocyanic acid in the interstellar medium

Formamide (NH$_2$CHO) has previously been detected in several star-forming regions and is thought to be a precursor for different prebiotic molecules. Its formation mechanism is still debated, however. Observations of formamide, related species and their isopotologues may provide useful clues to the chemical pathways leading to their formation. The Protostellar Interferometric Line Survey (PILS) represents an unbiased high angular resolution and sensitivity spectral survey of the low-mass protostellar binary IRAS 16293-2422 with the Atacama Large Millimeter/submillimeter Array (ALMA). We detect for the first time the three singly deuterated forms of NH$_2$CHO (NH$_2$CDO, cis- and trans-NHDCHO) as well as DNCO towards the component B of this binary source. The images reveal that the different isotopologues are all present in the same region. Based on observations of the $^{13}$C isotopologues of formamide and a standard $^{12}$C/$^{13}$C ratio, the deuterium fractionation is found to be similar for the three different forms with a value of about 2%. The DNCO/HNCO ratio is also comparable to the D/H ratio of formamide ($\sim$1%). These results are in agreement with the hypothesis that NH$_2$CHO and HNCO are chemically related through grain surface formation.

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Search for methylamine in high mass hot cores

We aim to detect methylamine, CH$_{3}$NH$_{2}$, in a variety of hot cores and use it as a test for the importance of photon-induced chemistry in ice mantles and mobility of radicals. Specifically, CH$_3$NH$_2$ cannot be formed from atom addition to CO whereas other NH$_2$-containing molecules such as formamide, NH$_2$CHO, can. Submillimeter spectra of several massive hot core regions were taken with the James Clerk Maxwell Telescope. Abundances are determined with the rotational diagram method where possible. Methylamine is not detected, giving upper limit column densities between 1.9 $-$ 6.4 $\times$ 10$^{16}$ cm$^{-2}$ for source sizes corresponding to the 100 K envelope radius. Combined with previously obtained JCMT data analyzed in the same way, abundance ratios of CH$_{3}$NH$_{2}$, NH$_{2}$CHO and CH$_{3}$CN with respect to each other and to CH$_{3}$OH are determined. These ratios are compared with Sagittarius B2 observations, where all species are detected, and to hot core models. The observed ratios suggest that both methylamine and formamide are overproduced by up to an order of magnitude in hot core models. Acetonitrile is however underproduced. The proposed chemical schemes leading to these molecules are discussed and reactions that need further laboratory studies are identified. The upper limits obtained in this paper can be used to guide future observations, especially with ALMA.

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