arXiv subjects

H. Linnartz

Publications and source records attributed to H. Linnartz.

At least 19 recordsLinked to original sources

arXiv2024

Ice inventory towards the protostar Ced 110 IRS4 observed with the James Webb Space Telescope. Results from the ERS Ice Age program

This work focuses on the ice features toward the binary protostellar system Ced 110 IRS 4A and 4B, and observed with JWST as part of the Early Release Science Ice Age collaboration. We aim to explore the JWST observations of the binary protostellar system Ced~110~IRS4A and IRS4B to unveil and quantify the ice inventories toward these sources. We compare the ice abundances with those found for the same molecular cloud. The analysis is performed by fitting or comparing laboratory infrared spectra of ices to the observations. Spectral fits are carried out with the ENIIGMA fitting tool that searches for the best fit. For Ced~110~IRS4B, we detected the major ice species H$_2$O, CO, CO$_2$ and NH$_3$. All species are found in a mixture except for CO and CO$_2$, which have both mixed and pure ice components. In the case of Ced~110~IRS4A, we detected the same major species as in Ced~110~IRS4B, as well as the following minor species CH$_4$, SO$_2$, CH$_3$OH, OCN$^-$, NH$_4^+$ and HCOOH. Tentative detection of N$_2$O ice (7.75~$\mu$m), forsterite dust (11.2~$\mu$m) and CH$_3^+$ gas emission (7.18~$\mu$m) in the primary source are also presented. Compared with the two lines of sight toward background stars in the Chameleon I molecular cloud, the protostar has similar ice abundances, except in the case of the ions that are higher in IRS4A. The clearest differences are the absence of the 7.2 and 7.4~$\mu$m absorption features due to HCOO$^-$ and icy complex organic molecules in IRS4A and evidence of thermal processing in both IRS4A and IRS4B as probed by the CO$_2$ ice features. We conclude that the binary protostellar system Ced~110~IRS4A and IRS4B has a large inventory of icy species. The similar ice abundances in comparison to the starless regions in the same molecular cloud suggest that the chemical conditions of the protostar were set at earlier stages in the molecular cloud.

astro-ph.SR↗

arXiv2024

Photofragmentation of Corannulene (C20H10) and Sumanene (C21H12) cations in gas phase and its Astrophysical implications

The aromatic infrared Bands (AIBs) dominate the mid-infrared spectra of many galactic and extragalactic sources. These AIBs are generally attributed to fluorescent emission from aromatic molecules. Unified efforts from experimentalists and theoreticians to assign these AIB features have recently gotten additional impetus with the launch of the James Webb Space Telescope (JWST) as the Mid-InfraRed Instrument (MIRI) delivers mid-IR spectrum with greatly increased sensitivity and spectral resolution. PAHs in space can exist in either neutral or ionic forms, absorb UV photons and undergo fragmentation, becoming a rich source of small hydrocarbons. This top-down mechanism of larger PAHs fragmenting into smaller species is of utmost importance in photo-dissociation regions (PDR) in space. In this work, we experimentally and theoretically investigate the photo-fragmentation pathways of two astronomically significant PAH cations - corannulene (C20H10) and sumanene (C21H12) that are structural motifs of fullerene C60, to understand their sequential fragmentation pathways. The photo-fragmentation experiments exhibit channels that are much different from planar PAHs. The breakdown of carbon skeleton is found to have different pathways for C20H10 and C21H12 because of the number and positioning of pentagon rings; yet the most abundant low mass cations produced by these two species are found to be similar. The low mass cations showcased in this work could be of interest for their astronomical detections. For completeness, the qualitative photo fragmentation behaviour of the dicationic corannulene and sumanene have also been experimented, but the potential energy surface of these dications are beyond the scope of this paper.

astro-ph.GA↗

arXiv2024

Laser-induced fragmentation of coronene cations

Polycyclic aromatic hydrocarbons are an important component of the interstellar medium of galaxies and photochemistry plays a key role in the evolution of these species in space. Here, we explore the photofragmentation behaviour of the coronene cation (C24H12+) using time of flight mass spectrometry. The experiments show photodissociation fragmentation channels including the formation of bare carbon clusters (Cn+) and hydrocarbon chains (CnHx+). The mass spectrum of coronene is dominated by peaks from C11+ and C7H+. Density functional theory was used to calculate relative energies, potential dissociation pathways, and possible structures for relevant species. We identify 6-6 to 5-7 ring isomerisation as a key step in the formation of both the bare carbon clusters and the hydrocarbon chains observed in this study. We present the dissociation mechanism outlined here as a potential formation route for C60 and other astrochemically relevant species.

astro-ph.GA↗

arXiv2024

The EDIBLES Survey. VIII. Band profile alignment of diffuse interstellar bands

Context: There have been many attempts to identify families of diffuse interstellar bands (DIBs) with perfectly correlating band strengths. Although major efforts have been made to classify broadly based DIB families and important insights have been gained, no family has been identified with sufficient accuracy or statistical significance to prove that a series of selected DIBs originates from the same carrier. This can be attributed in part to the exclusive use of equivalent widths to establish DIB families. Aims: In a change of strategy, we search for DIBs that are highly correlated in both band strength and profile shape. This approach increases the chance of correlating DIBs being members of one family and originating from the same carrier molecule. We also search for correlations between DIB profile families and atomic interstellar lines, with the goal of further chemically constraining possible DIB carriers. Methods: We adapted the well-known method of time-series alignment to perform a spectral alignment; that is, DIB alignment. In a second step, we analysed the alignment results using a clustering analysis. This method required a statistically significant data set of DIB sight lines. The ESO Diffuse Interstellar Bands Large Exploration Survey (EDIBLES) data were perfectly suited for this application. Results: We report eight DIB families with correlating strengths and profiles, as well as four previously unreported DIBs in the visual range, found using DIB alignment. All profile family members show Pearson correlation coefficients in band strength higher than 0.9. In particular, we report the 6614 - 6521 AA DIB pair, in which both DIBs show the same triple-peak substructure and an unprecedented band strength Pearson correlation coefficient of 0.9935. The presented approach opens up new perspectives that can guide the laboratory search for DIB carriers.

astro-ph.GA↗

arXiv2024

JOYS: MIRI/MRS spectroscopy of gas-phase molecules from the high-mass star-forming region IRAS 23385+6053

Space-based mid-IR spectroscopy provides tracers of warm gas in star-forming regions that are inaccessible from the ground. Past mid-IR spectra of bright high-mass protostars in the hot-core phase typically showed strong absorption features from molecules such as CO$_2$, C$_2$H$_2$, and HCN. However, little is known about their fainter counterparts at earlier stages. We thus aim to characterize the gas-phase molecular features in JWST MIRI/MRS observations of the young high-mass star-forming region IRAS 23385+6053. Spectra were extracted from two mid-IR sources and three H$_2$ bright outflow knots in the MIRI/MRS field of view. Rich molecular spectra with emission from CO, H$_2$, HD, H$_2$O, C$_2$H$_2$, HCN, CO$_2$, and OH are detected towards the two mid-IR sources. However, only CO and OH are seen towards the brightest H$_2$ knots, suggesting that the majority of the observed species are associated with disks or hot core regions rather than outflows. Simple Local thermodynamic equilibrium (LTE) slab models were used to fit the observed molecular features. The LTE model fits to $^{12}$CO$_{2}$, C$_{2}$H$_{2}$, and HCN emission suggest warm $120-200$ K emission arising from a disk surface around one or both protostars. Weak $\sim500$ K H$_2$O emission at $\sim$ 6-7 $\mu$m is detected towards one mid-IR source, whereas $250-1050$ K H$_2$O absorption is found in the other. The H$_2$O absorption may occur in the disk atmosphere due to strong accretion-heating of the midplane, or in a disk wind viewed at an ideal angle for absorption. CO emission may originate in the hot inner disk or outflow shocks. OH emission is likely excited in a non-LTE manner through water photodissociation or chemical formation. The observations are consistent with disks having already formed in the young IRAS 23385+6053 system, but further observations are needed to disentangle the effects of geometry and evolution.

astro-ph.GA↗

arXiv2024

A deep search for large complex organic species toward IRAS16293-2422 B at 3 mm with ALMA

Complex organic molecules (COMs) have been detected ubiquitously in protostellar systems. However, at shorter wavelengths (~0.8mm) it is more difficult to detect larger molecules than at longer wavelengths (~3mm) because of the increase of millimeter dust opacity, line confusion, and unfavorable partition function. We aim to search for large molecules (>8 atoms) in the ALMA Band 3 spectrum of IRAS 16293-2422 B. We search for more than 70 molecules and identify as many lines as possible in the spectrum. The spectral settings were set to specifically target three-carbon species such as propanol and glycerol. We identify lines of 31 molecules including many oxygen-bearing COMs such as CH3OH and c-C2H4O and a few nitrogen- and sulfur-bearing ones such as HOCH2CN and CH3SH. The largest detected molecules are gGg-(CH2OH)2 and CH3COCH3. We do not detect glycerol or propanol but provide upper limits for them which are in line with previous laboratory and observational studies. The line density in Band 3 is only ~2.5 times lower in frequency space than in Band 7. From the detected lines in Band 3 at a $\gtrsim 6\sigma$ level, ~25-30% of them could not be identified indicating the need for more laboratory data of rotational spectra. We find similar column densities and column density ratios of COMs (within a factor ~2) between Band 3 and Band 7. The effect of dust optical depth for IRAS 16293-2422 B at an off-source location on column densities and column density ratios is minimal. Moreover, for warm protostars, long wavelength spectra are not only crowded, but also take longer integration times to reach the same sensitivity limit. The 3mm search has not yet resulted in detection of larger and more complex molecules in warm sources. A full deep ALMA Band 2-3 (i.e., 3-4 mm) survey is needed to assess whether low frequency data have the potential to reveal more complex molecules in warm sources.

astro-ph.GA↗

arXiv2023

JWST Observations of Young protoStars (JOYS+): Detection of icy complex organic molecules and ions. I. CH$_4$, SO$_2$, HCOO$^-$, OCN$^-$, H$_2$CO, HCOOH, CH$_3$CH$_2$OH, CH$_3$CHO, CH$_3$OCHO, CH$_3$COOH

Complex organic molecules (COMs) detected in the gas phase are thought to be mostly formed on icy grains, but no unambiguous detection of icy COMs larger than CH3OH has been reported so far. Exploring this matter in more detail has become possible with the JWST the critical 5-10 $\mu$m range. In the JOYS+ program, more than 30 protostars are being observed with the MIRI/MRS. This study explores the COMs ice signatures in the low and high-mass protostar, IRAS 2A and IRAS 23385, respectively. We fit continuum and silicate subtracted observational data with IR laboratory ice spectra. We use the ENIIGMA fitting tool to find the best fit between the lab data and the observations and to performs statistical analysis of the solutions. We report the best fits for the spectral ranges between 6.8 and 8.6 $\mu$m in IRAS 2A and IRAS 23385, originating from simple molecules, COMs, and negative ions. The strongest feature in this range (7.7 $\mu$m) is dominated by CH4 and has contributions of SO2 and OCN-. Our results indicate that the 7.2 and 7.4 $\mu$m bands are mostly dominated by HCOO-. We find statistically robust detections of COMs based on multiple bands, most notably CH3CHO, CH3CH2OH, and CH3OCHO. The likely detection of CH3COOH is also reported. The ice column density ratios between CH3CH2OH and CH3CHO of IRAS 2A and IRAS 23385, suggests that these COMs are formed on icy grains. Finally, the derived ice abundances for IRAS 2A correlate well with those in comet 67P/GC within a factor of 5. Based on the MIRI/MRS data, we conclude that COMs are present in interstellar ices, thus providing additional proof for a solid-state origin of these species in star-forming regions. The good correlation between the ice abundances in comet 67P and IRAS 2A is in line with the idea that cometary COMs can be inherited from the early protostellar phases.

astro-ph.SR↗

arXiv2023

JOYS+: mid-infrared detection of gas-phase SO$_2$ emission in a low-mass protostar. The case of NGC 1333 IRAS2A: hot core or accretion shock?

JWST/MIRI has sharpened our infrared eyes toward the star formation process. This paper presents the first mid-infrared detection of gaseous SO$_2$ emission in an embedded low-mass protostellar system. MIRI-MRS observations of the low-mass protostellar binary NGC 1333 IRAS2A are presented from the JWST Observations of Young protoStars (JOYS+) program, revealing emission from the SO$_2~ν_3$ asymmetric stretching mode at 7.35 micron. The results are compared to those derived from high-angular resolution SO$_2$ data obtained with ALMA. The SO$_2$ emission from the $ν_3$ band is predominantly located on $\sim50-100$ au scales around the main component of the binary, IRAS2A1. A rotational temperature of $92\pm8$ K is derived from the $ν_3$ lines. This is in good agreement with the rotational temperature derived from pure rotational lines in the vibrational ground state (i.e., $ν=0$) with ALMA ($104\pm5$ K). However, the emission of the $ν_3$ lines is not in LTE given that the total number of molecules predicted by a LTE model is found to be a factor $2\times10^4$ higher than what is derived for the $ν=0$ state. This difference can be explained by a vibrational temperature that is $\sim100$ K higher than the derived rotational temperature of the $ν=0$ state. The brightness temperature derived from the continuum around the $ν_3$ band of SO$_2$ is $\sim180$ K, which confirms that the $ν_3=1$ level is not collisionally populated but rather infrared pumped by scattered radiation. This is also consistent with the non-detection of the $ν_2$ bending mode at 18-20 micron. Given the rotational temperature, the extent of the emission ($\sim100$ au in radius), and the narrow line widths in the ALMA data (3.5 km/s), the SO$_2$ in IRAS2A likely originates from ice sublimation in the central hot core around the protostar rather than from an accretion shock at the disk-envelope boundary.

astro-ph.SR↗

arXiv2023

JOYS: Disentangling the warm and cold material in the high-mass IRAS 23385+6053 cluster

(abridged) We study and compare the warm (>100 K) and cold (<100 K) material toward the high-mass star-forming region IRAS 23385+6053 (IRAS 23385 hereafter) combining high angular resolution observations in the mid-infrared (MIR) with the JWST Observations of Young protoStars (JOYS) project and with the NOEMA at mm wavelengths at angular resolutions of 0.2"-1". The spatial morphology of atomic and molecular species is investigated by line integrated intensity maps. The temperature and column density of different gas components is estimated using H2 transitions (warm and hot component) and a series of CH3CN transitions as well as 3 mm continuum emission (cold component). Toward the central dense core in IRAS 23385 the material consists of relatively cold gas and dust (~50 K), while multiple outflows create heated and/or shocked H2 and show enhanced temperatures (~400 K) along the outflow structures. An energetic outflow with enhanced emission knots of [Fe II] and [Ni II] hints at J-type shocks, while two other outflows have enhanced emission of only H2 and [S I] caused by C-type shocks. The latter two outflows are also more prominent in molecular line emission at mm wavelengths (e.g., SiO, SO, H2CO, and CH3OH). Even higher angular resolution data are needed to unambiguously identify the outflow driving sources given the clustered nature of IRAS 23385. While most of the forbidden fine structure transitions are blueshifted, [Ne II] and [Ne III] peak at the source velocity toward the MIR source A/mmA2 suggesting that the emission is originating from closer to the protostar.

astro-ph.SR↗

arXiv2023

A JWST inventory of protoplanetary disk ices: The edge-on protoplanetary disk HH 48 NE, seen with the Ice Age ERS program

Ices are the main carriers of volatiles in protoplanetary disks and are crucial to our understanding of the chemistry that ultimately sets the organic composition of planets. The ERS program Ice Age on the JWST follows the ice evolution through all stages of star and planet formation. JWST/NIRSpec observations of the edge-on Class II protoplanetary disk HH~48~NE reveal spatially resolved absorption features of the major ice components H$_2$O, CO$_2$, CO, and multiple weaker signatures from less abundant ices NH$_3$, OCN$^-$, and OCS. Isotopologue $^{13}$CO$_2$ ice has been detected for the first time in a protoplanetary disk. Since multiple complex light paths contribute to the observed flux, the ice absorption features are filled in by ice-free scattered light. The $^{12}$CO$_2$/$^{13}$CO$_2$ ratio of 14 implies that the $^{12}$CO$_2$ feature is saturated, without the flux approaching 0, indicative of a very high CO$_2$ column density on the line of sight, and a corresponding abundance with respect to hydrogen that is higher than ISM values by a factor of at least a few. Observations of rare isotopologues are crucial, as we show that the $^{13}$CO$_2$ observation allows us to determine the column density of CO$_2$ to be at an order of magnitude higher than the lower limit directly inferred from the observed optical depth. Radial variations in ice abundance, e.g., snowlines, are significantly modified since all observed photons have passed through the full radial extent of the disk. CO ice is observed at perplexing heights in the disk, extending to the top of the CO-emitting gas layer. We argue that the most likely interpretation is that we observe some CO ice at high temperatures, trapped in less volatile ices like H$_2$O and CO$_2$. Future radiative transfer models will be required to constrain the implications on our current understanding of disk physics and chemistry.

astro-ph.EP↗

arXiv2023

Water ice: temperature-dependent refractive indexes and their astrophysical implications

Interstellar ices are largely composed of frozen water. It is important to derive fundamental parameters for H$_2$O ice such as absorption and scattering opacities for which accurate complex refractive indexes are needed. The primary goal of this work is to derive ice-grain opacities based on accurate H$_2$O ice complex refractive indexes and to assess their impact on the derivation of ice column densities and porosity in space. We use the \texttt{optool} code to derive ice-grain opacities values based on new mid-IR complex refractive index measurements of H$_2$O ice. Next, we use those opacities in the \texttt{RADMC-3D} code to run a radiative transfer simulation of a protostellar envelope containing H$_2$O ice. This is used to calculate water ice column densities. We find that the real refractive index in the mid-IR of H$_2$O ice at 30~K is $\sim$14\% lower than previously reported in the literature. This has a direct impact on the ice column densities derived from the simulations of embedded protostars. We find that ice porosity plays a significant role in the opacity of icy grains and that the H$_2$O libration mode can be used as a diagnostic tool to constrain the porosity level. Finally, the refractive indexes presented here allow us to estimate a grain size detection limit of 18~$\mu$m based on the 3~$\mu$m band whereas the 6~$\mu$m band allows tracing grain sizes larger than 20~$\mu$m. Based on radiative transfer simulations using new mid-IR refractive indexes, we conclude that H$_2$O ice leads to more absorption of infrared light than previously estimated. This implies that the 3 and 6~$\mu$m bands remain detectable in icy grains with sizes larger than 10~$\mu$m. Finally, we propose that also the H$_2$O ice libration band can be a diagnostic tool to constrain the porosity level of the interstellar ice, in addition to the OH dangling bond, which is routinely used for this purpose.

astro-ph.IM↗

arXiv2023

CoCCoA: Complex Chemistry in hot Cores with ALMA. Selected oxygen-bearing species

Complex organic molecules (COMs) have been observed to be abundant in the gas phase toward protostars. Deep line surveys have been carried out only for a limited number of well-known high-mass star forming regions using the Atacama Large Millimeter/submillimeter Array (ALMA), which has unprecedented resolution and sensitivity. Statistical studies on oxygen-bearing COMs (O-COMs) in high-mass protostars using ALMA are still lacking. With the recent CoCCoA survey, we are able to determine the column density ratios of six O-COMs with respect to methanol (CH$_3$OH) in a sample of 14 high-mass protostellar sources to investigate their origin through ice and/or gas-phase chemistry. The selected species are: acetaldehyde (CH$_3$CHO), ethanol (C$_2$H$_5$OH), dimethyl ether (DME, CH$_3$OCH$_3$), methyl formate (MF, CH$_3$OCHO), glycolaldehyde (GA, CH$_2$OHCHO), and ethylene glycol (EG, (CH$_2$OH)$_2$). DME and MF have the highest and most constant ratios within one order of magnitude, while the other four species have lower ratios and exhibit larger scatter by 1-2 orders of magnitude. We compare the O-COM ratios of high-mass CoCCoA sources with those of 5 low-mass protostars available from the literature, along with the results from experiments and simulations. We find that the O-COM ratios with respect to methanol are on the same level in both the high- and low-mass samples, which suggests that these species are mainly formed in similar environments during star formation, probably in ice mantles on dust grains during early pre-stellar stages. Current simulations and experiments can reproduce most observational trends with a few exceptions, and hypotheses exist to explain the differences between observations and simulations/experiments, such as the involvement of gas-phase chemistry and different emitting areas of molecules.

astro-ph.GA↗

arXiv2023

JOYS: JWST Observations of Young protoStars: Outflows and accretion in the high-mass star-forming region IRAS23385+605

Aims: The JWST program JOYS (JWST Observations of Young protoStars) aims at characterizing the physical and chemical properties of young high- and low-mass star-forming regions, in particular the unique mid-infrared diagnostics of the warmer gas and solid-state components. We present early results from the high-mass star formation region IRAS23385+6053. Methods: The JOYS program uses the MIRI MRS with its IFU to investigate a sample of high- and low-mass star-forming protostellar systems. Results: The 5 to 28mum MIRI spectrum of IRAS23385+6053 shows a plethora of features. While the general spectrum is typical for an embedded protostar, we see many atomic and molecular gas lines boosted by the higher spectral resolution and sensitivity compared to previous space missions. Furthermore, ice and dust absorption features are also present. Here, we focus on the continuum emission, outflow tracers like the H2, [FeII] and [NeII] lines as well as the potential accretion tracer Humphreys alpha HI(7--6). The short-wavelength MIRI data resolve two continuum sources A and B, where mid-infrared source A is associated with the main mm continuum peak. The combination of mid-infrared and mm data reveals a young cluster in its making. Combining the mid-infrared outflow tracer H2, [FeII] and [NeII] with mm SiO data shows a complex interplay of at least three molecular outflows driven by protostars in the forming cluster. Furthermore, the Humphreys alpha line is detected at a 3-4sigma level towards the mid-infrared sources A and B. Following Rigliaco et al. (2015), one can roughly estimate accretion luminosities and corresponding accretion rates between ~2.6x10^-6 and ~0.9x10^-4 M_sun/yr. This is discussed in the context of the observed outflow rates. Conclusions: The analysis of the MIRI MRS observations for this young high-mass star-forming region reveals connected outflow and accretion signatures.

astro-ph.SR↗

arXiv2023

Resonant infrared irradiation of CO and CH3OH interstellar ices

Solid-phase photo-processes involving icy dust grains greatly affect the chemical evolution of the interstellar medium by leading to the formation of complex organic molecules and by inducing photodesorption. So far, the focus of laboratory studies has been mainly on the impact of energetic ultraviolet (UV) photons on ices, but direct vibrational excitation by infrared (IR) photons is expected to influence the morphology and content of interstellar ices as well. However, little is still known about the mechanisms through which this excess vibrational energy is dissipated, and its implications on the structure and ice photochemistry. In this work, we present a systematic investigation of the behavior of interstellar relevant CO and CH3OH ice analogues upon resonant excitation of vibrational modes using tunable infrared radiation, leading to both the quantification of infrared-induced photodesorption and insights in the impact of vibrational energy dissipation on ice morphology. We utilize an ultrahigh vacuum setup at cryogenic temperatures to grow pure CO and CH3OH ices, as well as mixtures of the two. We expose the ices to intense, near-monochromatic mid-infrared free-electron-laser radiation to selectively excite the species. The dissipation of vibrational energy is observed to be highly dependent on the excited mode and the chemical environment of the ice. All amorphous ices undergo some degree of restructuring towards a more organized configuration upon on-resonance irradiation. Moreover, IR-induced photodesorption is observed to occur for both pure CO and CH3OH ices, with interstellar photodesorption efficiencies of the order of 10 molecules cm-2 s-1 (i.e., comparable to or higher than UV-induced counterparts). Indirect photodesorption of CO upon vibrational excitation of CH3OH in ice mixtures is also observed to occur, particularly in environments rich in methanol.

astro-ph.GA↗

arXiv2023

An Ice Age JWST inventory of dense molecular cloud ices

Icy grain mantles are the main reservoir of the volatile elements that link chemical processes in dark, interstellar clouds with the formation of planets and composition of their atmospheres. The initial ice composition is set in the cold, dense parts of molecular clouds, prior to the onset of star formation. With the exquisite sensitivity of JWST, this critical stage of ice evolution is now accessible for detailed study. Here we show the first results of the Early Release Science program "Ice Age" that reveal the rich composition of these dense cloud ices. Weak ices, including, $^{13}$CO$_2$, OCN$^-$, $^{13}$CO, OCS, and COMs functional groups are now detected along two pre-stellar lines of sight. The $^{12}$CO$_2$ ice profile indicates modest growth of the icy grains. Column densities of the major and minor ice species indicate that ices contribute between 2 and 19% of the bulk budgets of the key C, O, N, and S elements. Our results suggest that the formation of simple and complex molecules could begin early in a water-ice rich environment.

astro-ph.GA↗

arXiv2022

The formation of CO$_2$ through consumption of gas-phase CO on vacuum-UV irradiated water ice

[Abridged] Observations of protoplanetary disks suggest that they are depleted in gas-phase CO. It has been posed that gas-phase CO is chemically consumed and converted into less volatile species through gas-grain processes. Observations of interstellar ices reveal a CO$_2$ component within H$_2$O ice suggesting co-formation. The aim of this work is to experimentally verify the interaction of gas-phase CO with solid-state OH radicals above the sublimation temperature of CO. Amorphous solid water (ASW) is deposited at 15 K and followed by vacuum-UV (VUV) irradiation to dissociate H$_2$O and create OH radicals. Gas-phase CO is simultaneously admitted and only adsorbs with a short residence time on the ASW. Products in the solid state are studied with infrared spectroscopy and once released into the gas phase with mass spectrometry. Results show that gas-phase CO is converted into CO$_2$, with an efficiency of 7-27%, when interacting with VUV irradiated ASW. Between 40 and 90 K, CO$_2$ production is constant, above 90 K, O$_2$ production takes over. In the temperature range of 40-60 K, the CO$_2$ remains in the solid state, while at temperatures $\geq$ 70 K the formed CO$_2$ is released into the gas phase. We conclude that gas-phase CO reacts with solid-state OH radicals above its sublimation temperature. This gas-phase CO and solid-state OH radical interaction could explain the observed CO$_2$ embedded in water-rich ices. It may also contribute to the observed lack of gas-phase CO in planet-forming disks, as previously suggested. Our experiments indicate a lower water ice dissociation efficiency than originally adopted in model descriptions of planet-forming disks and molecular clouds. Incorporation of the reduced water ice dissociation and increased binding energy of CO on a water ice surfaces in these models would allow investigation of this gas-grain interaction to its full extend.

astro-ph.IM↗

arXiv2022

LIDA - The Leiden Ice Database for Astrochemistry

High quality vibrational spectra of solid-phase molecules in ice mixtures and for temperatures of astrophysical relevance are needed to interpret infrared observations toward protostars and background stars. Over the last 25 years, the Laboratory for Astrophysics at Leiden Observatory has provided more than 1100 spectra of diverse ice samples. Timely with the recent launch of the James Webb Space Telescope, we have fully upgraded the Leiden Ice Database for Astrochemistry (LIDA) adding recently measured spectra. The goal of this manuscript is to describe what options exist to get access to and work with a large collection of IR spectra, and the UV/vis to mid-infrared refractive index of H2O ice and astronomy-oriented online tools to support the interpretation of IR ice observations. LIDA uses Flask and Bokeh for generating the web pages and graph visualization, respectively, SQL for searching ice analogues within the database and Jmol for 3D molecule visualization. The infrared data in the database are recorded via transmission spectroscopy of ice films condensed on cryogenic substrates. The real UV/vis refractive indices of H2O ice are derived from interference fringes created from the simultaneous use of a monochromatic HeNe laser beam and a broadband Xe-arc lamp, whereas the real and imaginary mid-IR values are theoretically calculated. LIDA also offers online tools. The first tool, SPECFY, used to create a synthetic spectrum of ices towards protostars. The second tool aims at the calculation of mid-infrared refractive index values. LIDA allows to search, download and visualize experimental data of astrophysically relevant molecules in the solid phase, as well as to provide the means to support astronomical observations. As an example, we analyse the spectrum of the protostar AFGL 989 using the resources available in LIDA and derive the column densities of H2O, CO and CO2 ices.

astro-ph.IM↗

arXiv2022

Reconciling spectroscopy with dynamics in global potential energy surfaces: the case of the astrophysically relevant SiC$_{2}$

SiC$_2$ is a fascinating molecule due to its unusual bonding and astrophysical importance. In this work, we report the first global potential energy surface (PES) for ground-state SiC$_2$ using the combined-hyperbolic-inverse-power-representation (CHIPR) method and accurate ab initio energies. The calibration grid data is obtained via a general dual-level protocol developed afresh herein that entails both coupled-cluster and multireference configuration interaction energies jointly extrapolated to the complete basis set limit. Such an approach is specially devised to recover much of the spectroscopy from the PES, while still permitting a proper fragmentation of the system to allow for reaction dynamics studies. Besides describing accurately the valence strongly-bound region that includes both the cyclic global minimum and isomerization barriers, the final analytic PES form is shown to properly reproduce dissociation energies, diatomic potentials, and long-range interactions at all asymptotic channels, in addition to naturally reflect the correct permutational symmetry of the potential. Bound vibrational state calculations have been carried out, unveiling an excellent match of the available experimental data on $c$-$\mathrm{SiC}_{2}(^{1}A_1)$. To further exploit the global nature of the PES, exploratory quasi-classical trajectory calculations for the endothermic $\mathrm{C_{2}\!+\!Si}\rightarrow\mathrm{SiC\!+\!C}$ reaction are also performed, yielding thermalized rate coefficients for temperatures up to $5000$ K. The results hint for the prominence of this reaction in the innermost layers of the circumstellar envelopes around carbon-rich stars, thence conceivably playing therein a key contribution to the gas-phase formation of SiC, and eventually, solid SiC dust.

physics.chem-ph↗