Interstellar H2CO. II - 2-centimeter emission from the Orion molecular cloud
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Evans, N. J., II↗
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Cooling of the 6-centimeter and 2-centimeter doublets of interstellar H2CO by collision - An accurate quantum-mechanical calculation
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Garrison, B. J.↗
Ab initio Quantum Chemical Studies of Reactions in Astrophysical Ices. Reactions Involving CH3OH, CO2, CO, HNCO in H2CO/NH3/H2O Ices
While reactions between closed shell molecules generally involve prohibitive barriers in the gas phase, prior experimental and theoretical studies have demonstrated that some of these reactions are significantly enhanced when confined within an icy grain mantle and can occur efficiently at temperatures below 100 K with no additional energy processing. The archetypal case is the reaction of formaldehyde (H2CO) and ammonia (NH3) to yield hydroxymethylamine (NH2CH2OH). In the present work we have characterized reactions involving methanol (CH3OH), carbon dioxide (CO2), carbon monoxide (CO), and isocyanic acid (HNCO) in search of other favorable cases. Most of the emphasis is on CH3OH, which was investigated in the two-body reaction with one H2CO and the three-body reaction with two H2CO molecules. The addition of a second H2CO to the product of the reaction between CH3OH and H2CO was also considered as an alternative route to longer polyoxymethylene polymers of the -CH2O- form. The reaction between HNCO and NH3 was studied to determine if it can compete against the barrierless charge transfer process that yields OCN(-) and NH4(+). Finally, the H2CO + NH3 reaction was revisited with additional benchmark calculations that confirm that little or no barrier is present when it occurs in ice.
Woon, David E.↗
Development of a Photoacoustic Formaldehyde Monitor
Key indoor air quality pollutant formaldehyde (H2CO) is tracked on International Space Station (ISS) using passive badges returned to the ground periodically for analysis. The process is time-consuming both in preparation and for analysis upon return 6-12 months later. Badges also require precious crew time for deploy, retrieval and stow. As NASA’s focus in space exploration shifts to the Moon and Mars, archival sample return becomes increasingly impractical, so the aim of this project is to develop a highly reliable real-time analyzer for H2CO at low concentrations with data downlinked. Potential sources of H2CO include materials off gassing, use of formalin as a tissue fixative in biological payloads and overheating of acetal polymers. The Spacecraft Maximum Allowable Concentration (SMAC) for H2CO is 100 ppb for exposures of 7 days or longer. ISS concentrations recently run only 10 - 30 ppb but have spiked as high as 60 ppb in the past. Gateway real time monitoring requirements call for a range of 8 - 140 ppb. For this project, a concentration range of 5 - 500 ppb H2CO is targeted. The core tunable diode laser spectroscopy (TDLS) technology was developed by Vista Photonics through the NASA and US Navy Small Business Innovation Research (SBIR) programs. Monitors based on this technology have been demonstrated on ISS, trialed on a nuclear submarine and are in production as Anomaly Gas Analyzers for both ISS and Orion. Initially, direct absorption TDLS was used exclusively in these monitors, however, the H2CO target concentration is much lower, and a longer wavelength required, so a photoacoustic spectroscopy (PAS) technique was adapted, where the laser excitation is detected by a sensitive microphone vs. a conventional photodetector. This paper will discuss the results of NASA-JSC laboratory testing of a prototype PAS based formaldehyde monitor and explore potential adaptations for Gateway missions and beyond.
Paul D Mudgett↗
Formaldehyde and organic molecule production in astrophysical ices at cryogenic temperatures
Thermally promoted formaldehyde (H2CO) reactions in cryogenic ices have been studied to test their importance as a source of organic molecules in comets and interstellar ices. Ices containing H2CO, H2O, CH3OH, CO, and NH3 were investigated by using infrared spectroscopy. Small traces of NH3 (NH3/H2CO equal to or greater than 0.005) are sufficient to convert significant fractions (40 percent or greater) of the H2CO into more complex organics. However, H2CO reactions do not proceed without NH3. Spectral evidence for reaction onset appeared between 40 and 80 K, depending on the ice. Five distinct products were formed. These principally consist of polyoxymethylene and related derivatives. Polyoxymethylene itself was not made in significant amounts in cometary analogs. These products differ from those produced by ultraviolet and particle irradiation. The nature and relative amounts of the products depend on the initial composition, making these materials excellent tracers of a comet's history. About 3 percent of the organics in p-Halley's coma could have been produced by thermal H2CO reactions.
Schutte, W. A.↗
Theoretical Studies of the Extra-terrestrial Chemistry of Biogenic Elements and Compounds
Results are presented on the following:(A) Ab initio quantum chemical studies of reactions in astrophysical ices.Theoretical electronic structure calculations were used to investigate reactions between formaldehyde (H2CO) and both hydrogen cyanide (HCN) and isocyanide (HNC) in search of other favorable reactions such as ammonia-formaldehyde addition, which was found in a recent theoretical study to be strongly enhanced when it occurs within cold ices.The present study examines further reactions between this product and H2CO in ices.(B) Heterogeneous hydrogenation of CO and H2CO on icy grain mantles.Formaldehyde (H2CO) and methanol (CH30H) are thought to be produced in the interstellar medium by the successive hydrogenation of carbon monoxide (CO) on grain surfaces. In the gas phase, the steps in which H adds to CO and H2CO possess modest barriers and are too inefficient to account for the observed abundances. Recent laboratory work has confirmed that formaldehyde and methanol are formed when H atoms are deposited on CO ice at 12 K. The present study employed ab initio quantum chemical calculations to investigate the impact of water ice on the sequential hydrogenation of CO.(C) Ice-bound condensed-phase reactions involving formic acid (HCOOH), methylenimine (CH2NH), hydrogen cyanide (HCN), hydrogen isocyanide (HNC), and ammonia ( 3) were investigated in order to characterize possible pathways to larger organic species that are efficient at the cold temperatures prevalent in cometary nuclei and the interstellar medium. (D) Pathways to glycine and other amino acids in ultraviolet-irradiated ices determined via quantum chemical modeling.(E) Photoionization in ultraviolet processing of astrophysical ice analogs at cryogenic temperatures.
Woon, David E.↗
Radio detection of formaldehyde emission from Comet Halley
The J(K-1 K1) = -1(11) -10(10) transition of H2CO was detected in emission at 4829.659 MHz from Comet Halley. The H2CO emission line had a peak intensity of 2.66 + or - 0.78 mJy/beam with a small blueshift of -0.76 + or - 0.40 km/s, which is consistent with the anisotropic outgassing of the nucleus in the solar direction found for other cometary species. Data analysis suggests that cometary H2CO was produced from an extended source in the coma as well as directly from the nucleus and that it was not refrigerated as in interstellar dark nebulae. The derived H2CO production rate of 1.5 x 10 to the 28th molecules/s is obtained which is consistent with observational and theoretical findings.
Snyder, Lewis E.↗
Submillimeter molecular line observations of cometary Levy (1990c)
Observations of HCN and H2CO in Comet Levy (1990c) obtained at the Caltech Submillimeter Observatory during August 1990 are presented. The HCN J=3-2 rotational line was measured at high spectral resolution (0.1 km/s) and mapped at 13 points over a region of approximately 1.5 arcmin. Analysis of the line profile and the map suggest only slight deviations from the distribution expected for isotropic outgassing of HCN from the nucleus at a velocity of 0.7 plus or minus 0.1 km/s. Observations of the HCN J=4-3 and H2CO5(sub 15)4(sub 14) transitions were obtained simultaneously on two days following the HCN J=3-2 measurements. These transitions are the first submillimeter spectral lines to be detected in a comet. Five point maps of the emission show good consistency between the J=3-2 and J=4-3 HCN observations for an HCN production rate of 2 x 10(exp 26) and a rotational temperature of approximately 30 K. The map of H2CO emission indicates that it is more extended than the prediction of models in which H2CO originates entirely from the nucleus. H2CO may also originate from an extended source in the coma.
Schloerb, F. Peter↗
An experimental study of the organic molecules produced in cometary and interstellar ice analogs by thermal formaldehyde reactions
Results of an experimental study tracing thermal formaldehyde reactions in astrophysically relevant ices in dense molecular clouds are reported. The formaldehyde chemistry during warm-up of ices containing H2CO and one or more of the molecules H2O, CH3OH, CO, O2, and NH3 were monitored using IR spectroscopy. Conversion of H2CO into residues was observed to start at about 40 K for NH3:H2CO ices and at about 80 K in H2O-rich ices. A total of five different organic products of these reactions were distinguished: POM and reaction products of H2CO and H2O, CH3OH, and NH3. Given the measured reaction paths and efficiencies, it is estimated that on the order of 1 percent of the organics found in the coma of Comet P/Halley could have been produced by thermal formaldehyde reactions taking place in the nucleus.
Schutte, W. A.↗
Externally Heated Protostellar Cores in the Ophiuchus Star-Forming Region
We present APEX 218 GHz observations of molecular emission in a complete sample of embedded protostars in the Ophiuchus star-forming region. To study the physical properties of the cores, we calculate H2CO and c-C3H2 rotational temperatures, both of which are good tracers of the kinetic temperature of the molecular gas. We find that the H2CO temperatures range between 16K and 124K, with the highest H2CO temperatures toward the hot corino source IRAS 16293-2422 (69-124 K) and the sources in the rho Oph A cloud (23-49 K) located close to the luminous Herbig Be star S1, which externally irradiates the rho Oph A cores. On the other hand, the c-C3H2 rotational temperature is consistently low (7-17 K) in all sources. Our results indicate that the c-C3H2 emission is primarily tracing more shielded parts of the envelope whereas the H2CO emission (at the angular scale of the APEX beam; 3600 au in Ophiuchus) mainly traces the outer irradiated envelopes, apart from in IRAS16293-2422, where the hot corino emission dominates. In some sources, a secondary velocity component is also seen, possibly tracing the molecular outflow.
CH3OH↗
Chemical effects of large impacts on the earth's primitive atmosphere
The production of HCN and H2CO by large impacts on the earth's primitive atmosphere is modelled using thermochemical equilibrium and chemical kinetic calculations of the composition of shocked air parcels for a wide range of temperatures, pressures, and initial compositions. For atmospheres with C/O of one or more, the results suggest that bolide impacts cause HCN volume mixing ratios of approximately 10 to the -3rd to -5th in the impact region and global average ratios of 10 to the -5th to the -12th. The corresponding H2CO mixing ratios in the impact region are 10 to the -7th to -9th; nonglobal mixing can occur, however, as H2CO is rapidly destroyed or rained out of the atmosphere within days to hours. Rainout to the oceans of 3-15 percent of the HCN produced can provide 3-14 x 10 to the 11th mol HCN per year.
Fegley, B., Jr.↗
A survey of formaldehyde in high Galactic latitudes
The discovery of formaldehyde (H2CO) in four out of 15 CO-clouds observed in high Galactic latitudes is reported. For one of these a velocity-integrated formaldehyde map is presented. The clouds are clearly connected to CO clouds described by de Vries et al. (1986), to Lynds bright and dark nebulae (Lynds, 1963), and to the Galactic infrared cirrus (Low et al., 1984). The distribution of CO and H2CO clouds is compared. The depths of the l(10-11)H2CO lines show no correlation to the integrated J = l-0(C-12)O line intensities.
Heithausen, A.↗
On the identification of formaldehyde in Halley's comet
The v1 and v5 infrared bands of formaldehyde in Halley's comet have been synthesized, using a line-by-line model for solar infrared fluorescence from low-temperature H2CO. Fully resolved spectra were convolved to spectral resolutions comparable with those used on the IKS spectrometer on the Vega 1 spacecraft. Excellent agreement is obtained between the observed and modeled spectra, permitting a definite identification of H2CO in Halley's comet. The retrieved production rate is 4.5 + or - 0.5 x 10 to the 28th molecules/s, and the rotational temperature is probably less than 150 K, with a best-fit value of about 50 K. Production rates (or upper limits) are also retrieved from ground-based spectra of Comets Halley and Wilson (1986), and it is shown that the production rate of H2CO exhibits significant temporal variability, relative to H2O, in Comet Halley.
Mumma, Michael J.↗
Millimetre observations of comets P/Brorsen-Metcalf (1989o) and Austin (1989c1) with the IRAM 30-m radio telescope
Millimeter observations with the IRAM 30 m telescope were conducted in comet P/Brorsen-Metcalf (1989o) on September 1989 and Austin (1989c1) on April and May 1990. The HCN J(1-0) and J(3-2) lines were detected in both comets. The HCN production rate relative to water in P/Brorsen-Metcalf is comparable to that previously measured in comet P/Halley, while that inferred in comet Austin might be smaller by a factor of two. The H2CO(3 sub 12 - 2 sub 11) transition, marginally observed in comet P/Brorsen-Metcalf, was firmly detected in May 1990 in comet Austin. Observations performed at offset positions suggest that the source of H2CO might be distributed. The H2CO abundance is on the order of 0.5 percent that of water for both comets, assuming a scalelength of 10(exp 4) km at 1 AU from the Sun for the distributed source. During the May observing period of comet Austin, two new species were detected for the first time in a comet: hydrogen sulfide (H2S) through its 1(sub 10) - 1(sub 01) ortho line at 169 GHz, and methanol (CH3OH) through J(3-2) delta K = 0 transitions at 145 GHz. Preliminary estimates of their abundances are 1.5 x 10(exp -3) for H2S and 8 x 10(exp -3) for CH3OH.
Colom, P.↗
Identification and yield of carbonic acid and formaldehyde in irradiated ices
Carbonic acid, (OH)2CO, was tentatively identified in the IR spectrum of a proton irradiated CO2 + H2O ice mixture. In this report, we present additional evidence for a more definitive identification of (OH)2CO with (1) the infrared spectrum of a residue obtained by proton irradiation of CO2 + D2O ice mixture, and (2) the IR spectra of solid phases of formaldehyde (H2CO), acetone (CH3)2CO, and dimethyl carbonate (OCH3)2CO, which are structurally similar to (OH)2CO. IR characteristics (peak frequencies and complex refractive indices of the compounds in point 2) are also reported. In particular, the integrated absorption coefficients for the C-O band for the compounds in point 2 do not vary by more than 20 percent. Based on these values, we estimate the yields of H2CO and (OH)2CO by proton irradiation or ice mixtures. Both H2CO and (OH)2CO are possible irradiation products of cometary and planetary ices.
Dellorusso, Neil↗
The formaldehyde ortho/para ratio as a probe of dark cloud chemistry and evolution
We present measurements of the H2CO ortho/para ratio toward four star-forming cores, L723, L1228, L1527, and L43, and one quiescent core, L1498. Combining these data with earlier results by Minh et al., three quiescent cores are found to have ortho/para ratios near 3, the ratio of statistical weights expected for gas-phase formation processes. In contrast, ortho/para ratios are 1.5-2.1 in five star-forming cores, suggesting thermalization at a kinetic temperature of 10 K. We attribute modification of the ortho/para ratio in the latter cores to formation and/or equilibration of H2CO on grains with sub-sequent release back into the gas phase due to the increased energy inputs from the forming star and outflow. We see accompanying enhancements in the H2CO abundance relative to H, to support this idea. The results suggest that the formaldehyde ortho/para ratio can differentiate between quiescent cores and those in which low-mass star formation has occurred.
Non-NASA Center↗
Envelope structure of deeply embedded young stellar objects in the Serpens Molecular Cloud
Aperture-synthesis and single-dish (sub-) millimeter molecular-line and continuum observations reveal in great detail the envelope structure of deeply embedded young stellar objects (SMM 1 = FIRS 1, SMM 2, SMM 3, SMM 4) in the densely star-forming Serpens Molecular Cloud. SMM 1, 3, and 4 show partially resolved (>2" = 800 AU) continuum emission in the beam of the Owens Valley Millimeter Array at lambda = 3.4-1.4 mm. The continuum visibilities accurately constrain the density structure in the envelopes, which can be described by a radial power law with slope -2.0 +/- 0.5 on scales of 300 to 8000 AU. Inferred envelope masses within a radius of 8000 AU are 8.7, 3.0, and 5.3 Msolar for SMM 1, 3, and 4, respectively. A point source with 20%-30% of the total flux at 1.1 mm is required to fit the observations on long baselines, corresponding to warm envelope material within approximately 100 AU or a circumstellar disk. No continuum emission is detected interferometrically toward SMM 2, corresponding to an upper limit of 0.2 Msolar assuming Td = 24 K. The lack of any compact dust emission suggests that the SMM 2 core does not contain a central protostar. Aperture-synthesis observations of the 13CO, C18O, HCO+, H13CO+, HCN, H13CN, N2H+ 1-0, SiO 2-1, and SO 2(2)-1(1) transitions reveal compact emission toward SMM 1, 3, and 4. SMM 2 shows only a number of clumps scattered throughout the primary field of view, supporting the conclusion that this core does not contain a central star. The compact molecular emission around SMM 1, 3, and 4 traces 5"-10" (2000-4000 AU) diameter cores that correspond to the densest regions of the envelopes, as well as material directly associated with the molecular outflow. Especially prominent are the optically thick HCN and HCO+ lines that show up brightly along the walls of the outflow cavities. SO and SiO trace shocked material, where their abundances may be enhanced by 1-2 orders of magnitude over dark-cloud values. A total of 31 molecular transitions have been observed with the James Clerk Maxwell and Caltech Submillimeter telescopes in the 230, 345, 490, and 690 GHz atmospheric windows toward all four sources, containing, among others, lines of CO, HCO+, HCN, H2CO, SiO, SO, and their isotopomers. These lines show 20-30 km s-1 wide line wings, deep and narrow (1-2 km s-1) self-absorption, and 2-3 km s-1 FWHM line cores. The presence of highly excited lines like 12CO 4-3 and 6-5, 13CO 6-5, and several H2CO transitions indicates the presence of material with temperatures > or approximately 100 K. Monte Carlo calculations of the molecular excitation and line transfer show that the envelope model derived from the dust emission can successfully reproduce the observed line intensities. The depletion of CO in the cold gas is modest compared to values inferred in objects like NGC 1333 IRAS 4, suggesting that the phase of large depletions through the entire envelope is short lived and may be influenced by the local star formation density. Emission in high-excitation lines of CO and H2CO requires the presence of a small amount of approximately 100 K material, comprising less than 1% of the total envelope mass and probably associated with the outflow or the innermost region of the envelope. The derived molecular abundances in the warm (Tkin > 20 K) envelope are similar to those found toward other class 0 YSOs like IRAS 16293-2422, though some species appear enhanced toward SMM 1. Taken together, the presented observations and analysis provide the first comprehensive view of the physical and chemical structure of the envelopes of deeply embedded young stellar objects in a clustered environment on scales between 1000 and 10,000 AU.
NASA Discipline Exobiology↗
The 2.5-12 micrometers spectrum of comet Halley from the IKS-VEGA experiment
The infrared instrument IKS flown on board the VEGA space probes was designed for the detection of emission bands of parent molecules, and for a measurement of the size and temperature of the thermal emitting nuclear region. The instrument had three channels with cooled detectors: an "imaging channel" designed to modulate the signal of the nucleus and two spectroscopic channels operating at 2.5-5 and 6-12 micrometers, respectively, equipped with circular variable filters of resolving power approximately 50. This paper presents and discusses the results from the spectral channels. On VEGA 1, usable spectra were obtained at distances D from the comet nucleus ranging from 250,000 to 40,000 km corresponding to fields of view 4000 and 700 km in diameter, respectively. The important internal background signal caused by the instrument itself, which could not be cooled, had to be eliminated. Since no sky chopping was performed, we obtain difference spectra between the current spectrum and a reference spectrum with little or no cometary signal taken at the beginning of the observing sequence (D approximately 200,000 km). Final discrimination between cometary signal and instrumental background is achieved using their different time evolution, since the instrumental background is proportional to the slow temperature drift of the instrument, and the cometary signal due to parent molecules or dust grains is expected to vary in first order as D-1. The 2.5-5 micrometers IKS spectra definitely show strong narrow signals at 2.7 and 4.25 micrometers, attributed to the nu 3 vibrational bands of H2O and CO2, respectively, and a broader signal in the region 3.2-3.5 micrometers, which may be attributed to CH-bearing molecules. All these signals present the expected D-1 intensity variation. Weaker emission features at 3.6 and 4.7 micrometers could correspond to the nu 1 and nu 5 bands of H2CO and the (1 - 0) band of CO, respectively. Molecular production rates are derived from the observed emissions, assuming that they are due to resonance fluorescence excited by the Sun's infrared radiation. For the strong bands of H2O and CO2, the rovibrational lines are optically thick, and radiative transfer is taken into account. We derive production rates, at the moment of the VEGA 1 flyby, of approximately 10(30) sec-1 for H2O, approximately 2.7 x 10(28) sec-1 for CO2, approximately 5 x 10(28) sec-1 for CO, and 4 x 10(28) sec-1 for H2CO, if attributions to CO and H2CO are correct. The production rate of carbon atoms in CH-bearing molecules is approximately 9 x 10(29) sec-1 assuming fluorescence of molecules in the gas phase, but could be much less if the 3.2-3.5 micrometers emission is attributed to C-H stretch in polycyclic aromatic hydrocarbons or small organic grains. In addition, marginal features are present at 4.85 and 4.45 micrometers, tentatively attributed to OCS and molecules with the CN group, respectively. Broad absorption at 2.8-3.0 micrometers, as well as a narrow emission at 3.15 micrometers, which follow well the D-1 intensity variation, might be due to water ice. Emission at 2.8 micrometers is also possibly present, and might be due to OH created in vibrationally excited states after water photodissociation. The 6-12 micrometers spectrum does not show any molecular emission, nor emission in the 7.5-micrometers region. The spectrum is dominated by silicate emission showing a double structure with maxima at 9.0 and 11.2 micrometers, which suggests the presence of olivine.
NASA Discipline Number 52-10↗