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All sourcesNASA NTRSDOE OSTI
DOE OSTI2024

Capturing the generation and structural transformations of molecular ions

Molecular ions are ubiquitous and play pivotal roles in many reactions, particularly in the context of atmospheric and interstellar chemistry. However, their structures and conformational transitions, particularly in the gas phase, are less explored than those of neutral molecules owing to experimental difficulties. A case in point is the halonium ions, whose highly reactive nature and ring strain make them short-lived intermediates that are readily attacked even by weak nucleophiles and thus challenging to isolate or capture before they undergo further reaction. Here we show that mega-electronvolt ultrafast electron diffraction (MeV-UED), used in conjunction with resonance-enhanced multiphoton ionization, can monitor the formation of 1,3-dibromopropane (DBP) cations and their subsequent structural dynamics forming a halonium ion. We find that the DBP + cation remains for a substantial duration of 3.6 ps in aptly named ‘dark states’ that are structurally indistinguishable from the DBP electronic ground state. The structural data, supported by surface-hopping simulations and ab initio calculations, reveal that the cation subsequently decays to iso-DBP + , an unusual intermediate with a four-membered ring containing a loosely bound bromine atom, and eventually loses the bromine atom and forms a bromonium ion with a three-membered-ring structure. We anticipate that the approach used here can also be applied to examine the structural dynamics of other molecular ions and thereby deepen our understanding of ion chemistry.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
NASA NTRS1989

Angular motion of a PAH molecule in interstellar environment

Polycyclic aromatic hydrocarbon (PAH) molecules have recently been proposed as an important and hitherto undetected component of the Interstellar Medium (ISM). The theory was based on an explanation of the Unidentified IR Emission Bands by Leger et al. It has already led to a verified prediction on extended galactic and extragalactic emissions measured by IRAS, or by a recent balloon borne experiment. The physics that rules the motion of such molecules in the ISM was studied, taking into account their coupling with the ambient gas, the radiation field (absorption and emission) and the static magnetic field. This is important for many implications of the PAH theory such as the radio emission by these molecules or the expected polarization of their IR emission. A reflection nebulae is considered where the situation is rather well known. Every day life of a mean PAH molecule in such a region is as follows: every 3 hrs a UV photon is absorbed heating the molecule to a thousand degs; the temperature decay due to cooling by IR emission follows then within a few seconds. A collision with a molecule of gas occurs typically once a week, while an H atom is ejected or captured at the same rate. A typical cooling cycle after a heat impulse is given. The PAH molecules studied as representative of the family has typically 50 atoms, a radius of 4.5 A, is circular and has a molecular mass of M = 300; its permanent dipole moment is 3 Debye.

Rouan, D.↗
NASA NTRS2012

An In-Depth Study of the Abundance Pattern in the Hot Interstellar Medium in NGC 4649

We present our X-ray imaging spectroscopic analysis of data from deep Suzuku and XMM-Newton Observatory exposures of the Virgo Cluster elliptical galaxy NGC 4649 (M60), focusing on the abundance pattern in the hot interstellar medium (ISM). All measured elements show a radial decline in abundance, with the possible exception of O. We construct steady state solutions to the chemical evolution equations that include infall in addition to stellar mass return and SNIa enrichment, and consider recently published SNIa yields. By adjusting a single model parameter to obtain a match to the global abundance pattern in NGC 4649 we infer that accretion of subsolar metallicity external gas has reduced the overall ISM metallicity and diluted the effectiveness of SNIa to skew the pattern towards low alpha/Fe ratios, and estimate the combination of SNIa rate and level of dilution. Evidently, newly-introduced gas is heated as it is integrated into. and interacts with, the hot gas that is already present. These results indicate a complex flow and enrichment history for NGC 4649, reflecting the continual evolution of elliptical galaxies beyond the formation epoch. The heating and circulation of accreted gas may help reconcile this dynamic history with the mostly passive evolution of elliptical stellar populations. In an appendix we examine the effects of the recent updated atomic database AtomDB in spectral fitting of thermal plasmas with hot ISM temperatures in the elliptical galaxy range.

Lowenstein, Michael↗
NASA NTRS2012

An In-Depth Study of the Abundance Pattern in the Hot Interstellar Medium in NGC 4649

We present our X-ray imaging spectroscopic analysis of data from deep Suzaku and XMM-Newton Observatory exposures of the Virgo Cluster elliptical galaxy NGC 4649 (M60), focusing on the abundance pattern in the hot interstellar medium (ISM). All measured elements show a radial decline in abundance, with the possible exception of Oxygen. We construct steady state solutions to the chemical evolution equations that include infall in addition to stellar mass return and Type Ia supernovae (SNIa) enrichment, and consider recently published SNIa yields. By adjusting a single model parameter to obtain a match to the global abundance pattern in NGC 4649 we infer that introduction of subsolar metallicity external gas has reduced the overall ISM metallicity and diluted the effectiveness of SNIa to skew the pattern towards low alpha/Fe ratios, and estimate the combination of SNIa rate and level of dilution. Evidently, newly-introduced gas is heated as it is integrated into, and interacts with, the hot gas that is already present. These results indicate a complex flow and enrichment history for NGC 4649, reflecting the continual evolution of elliptical galaxies beyond the formation epoch. The heating and circulation of accreted gas may help reconcile this dynamic history with the mostly passive evolution of elliptical stellar populations. In an appendix we examine the effects of the recent updated atomic database AtomDB in spectral fitting of thermal plasmas with hot ISM temperatures in the elliptical galaxy range.

Loewenstein, Michael↗
NASA NTRS2013

Photo-Induced Deuterium Enrichment in Residues Produced from the UV Irradiation of Pyrimidine in H2O and H2O+NH3 Ices

Organic compounds found in meteorites often show isotopic signatures of their interstellar/protosolar heritage as enrichments in D and 15N. Meteoritic organics found to be enriched in D include amino acids, hydroxy and dicarboxylic acids, as well as polycyclic aromatic hydrocarbons (PAHs). Processes that can produce isotopic enrichments in presolar/protosolar materials include gas-phase ion-molecule reactions, gas-grain surface reactions, and unimolecular photo-dissociation reactions involving PAHs. Because many molecules in interstellar clouds are enriched in D, the presence of D anomalies in meteorites is thought to originate from preserved or slightly altered interstellar/protostellar materials. However, the link between isotopic enrichments seen in space and those in meteoritic compounds and their relationship remain unclear. In this work, we present results of hydrogen isotopic fractionation for compounds in organic residues produced from the UV irradiation using an H2- discharge UV lamp of H2O:pyrimidine = 20:1 and H2O:NH3:pyrimidine = 20:2:1 ice mixtures at low temperature (is less than 20 K). After irradiation, the resulting residues are dissolved in H2O and analyzed with gas chromatography-mass spectrometry coupled with isotope ratio mass spectrometry (GC-MS/IRMS) [1], following a protocol similar to that used for previous analyses of comparable samples [2,3]. We used this technique to measure compound-specific D/H isotopic ratios for the initial pyrimidine and for two photo-products present in the residues, namely, 2,2'-bipyrimidine and an unidentified bipyrimidine isomer [2-4]. Measuring D enrichments in bipyrimidines has the advantage that the H atoms on these molecules are not easily exchangeable with other compounds, in particular the H2O and NH3 present in the ices or the solvents used to extract the samples for GC-MS/IRMS measurements. The δD value for the initial pyrimidine, measured with a high-temperature conversion elemental analyzer connected to the IRMS, was found to be -30% per mille. Preliminary measurements made on a residue produced from the UV irradiation of an H2O:NH3:pyrimidine = 20:2:1 ice mixture indicate δD values of +118% per mille for 2,2'- bipyrimidine and +92% per mille for the other bipyrimidine isomer, and therefore show a significant D enrichment during the photo-processing and warm-up that lead to their formation [5]. New measurements are currently being performed on a number of residues produced from simpler H2O:pyrimidine = 20:1 ice mixtures under different experimental conditions and will be presented here.

Laboratory Astrochemistry↗
NASA NTRS1990

Lyman alpha radiation in external galaxies

The Ly alpha line of atomic hydrogen is often a luminous component of the radiation emitted by distant galaxies. Except for those galaxies which have a substantial central source of non-stellar ionizing radiation, most of the Ly alpha radiation emitted by galaxies is generated within regions of the interstellar medium which are photoionized by starlight. Conversely, much of the energy radiated by photoionized regions is carried by the Ly alpha line. Only hot, massive stars are capable of ionizing hydrogen in the interstellar medium which surrounds them, and because such stars are necessarily short-lived, Ly alpha emission traces regions of active star formation. Researchers argue that the strength of the Ly alpha emission observed from external galaxies may be used to estimate quantitatively the dust content of the emitting region, while the Ly alpha line profile is sensitive to the presence of shock waves. Interstellar dust particles and shock waves are intimately associated with the process of star formation in two senses. First, both dust particles and shock waves owe their existence to stellar activity; second, they may both serve as agents which facilitate the formation of stars, shocks by triggering gravitational instabilities in the interstellar gas that they compress, and dust by shielding star-forming molecular clouds from the ionizing and dissociative effects of external UV radiation. By using Ly alpha observations as a probe of the dust content in diffuse gas at high redshift, we might hope to learn about the earliest epochs of star formation.

Neufeld, David A.↗
NASA NTRS2001

Organic Signature of Dust from the Interstellar Medium (ISM)

Dust in the ISM carries an "organic" signature in form of a distinct group of C-H stretching bands, both in emission and absorption, around 3.4 micrometers. These bands agree with the symmetrical and asymmetrical C-H stretching vibrations of aliphatic -CH2- entities and are thought to be associated with organic molecules on the surface of dust grains. We show that this interpretation is inconsistent with laboratory experiments. Synthetic MgO and natural olivine single crystals, grown from a CO/CO2/H2O-saturated melt, exhibit the same C-H stretching bands but those bands are clearly associated with C-H entities inside the dense mineral matrix. The multitude of C-H stretching bands suggests that the C-H bonds arise from polyatomic C(sub n) entities. We heated the MgO and olivine crystals to temperatures between 550-1000 K to pyrolyze the C-H bonds and to cause the C-H stretching bands to disappear. Upon annealing at moderate temperatures between 300-390 K the C-H stretching bands reappear within a few days to weeks. The C-H stretching band intensity increases linearly with the square root of time. Thus, while the pyrolysis broke the C-H bonds and caused the H to disperse in the mineral matrix, the H atoms (or H2 molecules) are sufficiently mobile to return during annealing and reestablish the C-H bonds. Dust grains that condense in a gas-laden environment (outflow of late-stage stars or in dense molecular clouds) probably incorporate the same type of Cn-H entities. Imbedded in and in part bonded to the surrounding mineral matrix, the Cn-H entities display C-H stretching bands in the 3.4 micrometer region, but their lower frequency librational modes are so strongly coupled to the lattice modes that they broaden excessively and thus become unobservable.

Freund, Friedemann↗
DOE OSTI2024

The atomic gas sequence and mass–metallicity relation from dwarfs to massive galaxies

Galaxy scaling relations provide insights into the processes that drive galaxy evolution. The extension of these scaling relations into the dwarf galaxy regime is of particular interest. This is because dwarf galaxies represent a crucial stage in galaxy evolution, and understanding them could also shed light on their role in reionizing the early Universe. There is currently no consensus on the processes that dominate the evolution of dwarfs. In this work, we constrain the atomic gas sequence (stellar mass versus atomic gas fraction) and mass–metallicity relation (stellar mass versus gas-phase metallicity) from dwarf (⁠10 6.5 M ⊙ ⁠) to massive (⁠10 11.5 M ⊙ ) galaxies in the local Universe. The combined optical and 21-cm spectroscopic observations of the Dark Energy Spectroscopic Instrument and Arecibo Legacy Fast ALFA surveys allow us to constrain both scaling relations simultaneously. We find a slope change of the atomic gas sequence at a stellar mass of ~10 9 M ⊙ ⁠. We also find that the shape and scatter of the atomic gas sequence and mass–metallicity relation are strongly linked for both dwarfs and more massive galaxies. Consequently, the low-mass slope change of the atomic gas sequence is imprinted onto the mass–metallicity relation of dwarf galaxies. The mass scale of the measured slope change is consistent with a predicted escape velocity threshold below which low-mass galaxies experience significant supernova-driven gas loss, as well as with a reduction in cold gas accretion onto more massive galaxies.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2022

Gas-Phase Study of the Elementary Reaction of the D1-Ethynyl Radical (C 2 D; X 2 Σ + ) with Propylene (C 3 H 6 ; X 1 A') under Single-Collision Conditions

The bimolecular gas-phase reactions of the D1-ethynyl radical (C 2 D; X 2 Σ + ) with propylene (C 3 H 6 ; X 1 A’) and partially substituted D3-3,3,3-propylene (C 2 H 3 CD 3 ; X 1 A’) were studied under single collision conditions utilizing the crossed molecular beams technique. Combining our laboratory data with electronic structure and statistical calculations, the D1-ethynyl radical is found to add without barrier to the C1 and C2 carbons of the propylene reactant, resulting in doublet C 5 H 6 D intermediate(s) with lifetime(s) longer than their rotational period(s). These intermediates undergo isomerization and unimolecular decomposition via atomic hydrogen loss through tight exit transition states forming predominantly cis/trans-3-penten-1-yne ((HCC)CH=CH(CH 3 )) and to a minor amount 3-methyl-3-buten-1-yne ((HCC)C(CH 3 )=CH 2 ) via overall exoergic reactions. Although the title reaction does not lead to the cyclopentadiene molecule (c-C 5 H 6 , X 1 A 1 ), high temperature environments can convert the identified acyclic C 5 H 6 isomers through hydrogen atom assisted isomerization to cyclopentadiene (c-C 5 H 6 , X 1 A 1 ). Since both the ethynyl radical and propylene reactants have been observed in cold interstellar environments such as TMC-1 and the reaction is exoergic and all barriers lie below the energy of the separated reactants, the these C 5 H 6 product isomers are predicted to form in those low temperature regions.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
NASA NTRS1992

Laboratory astrophysics under the ultraviolet, visible, and gravitational astrophysics research program: Oscillator strengths for ultraviolet atomic transitions

The conditions within astrophysical environments can be derived from observational data on atomic and molecular lines. For instance, the density and temperature of the gas are obtained from relative populations among energy levels. Information on populations comes about only when the correspondence between line strength and abundance is well determined. The conversion from line strength to abundance involves knowledge of meanlives and oscillator strengths. For many ultraviolet atomic transitions, unfortunately, the necessary data are either relatively imprecise or not available. Because of the need for more and better atomic oscillator strengths, our program was initiated. Through beam-foil spectroscopy, meanlives of ultraviolet atomic transitions are studied. In this technique, a nearly isotopically pure ion beam of the desired element is accelerated. The beam passes through a thin carbon foil (2 mg/cu cm), where neutralization, ionization, and excitation take place. The dominant process depends on the energy of the beam. Upon exiting the foil, the decay of excited states is monitored via single-photon-counting techniques. The resulting decay curve yields a meanlife. The oscillator strength is easily obtained from the meanlife when no other decay channels are presented. When other channels are present, additional measurements or theoretical calculations are performed in order to extract an oscillator strength. During the past year, three atomic systems have been studied experimentally and/or theoretically; they are Ar, I, Cl I, and N II. The results for the first two are important for studies of interstellar space, while the work on N II bears on processes occurring in planetary atmospheres.

Federman, Steven R.↗
NASA NTRS2007

Determination of the Far-Infrared Cosmic Background Using COBE/DIRBE and WHAM Data

Determination of the cosmic infrared background (CIB) at far infrared wavelengths using COBE/DIRBE data is limited by the accuracy to which foreground interplanetary and Galactic dust emission can be modeled and subtracted. Previous determinations of the far infrared CIB (e.g., Hauser et al. 1998) were based on the detection of residual isotropic emission in skymaps from which the emission from interplanetary dust and the neutral interstellar medium were removed. In this paper we use the Wisconsin H(alpha) Mapper (WHAM) Northern Sky Survey as a tracer of the ionized medium to examine the effect of this foreground component on determination of the CIB. We decompose the DIRBE far infrared data for five high Galactic latitude regions into HI- and H(alpha)- correlated components and a residual component. Eased on FUSE H2 absorption line observations, the contribution of a11 H2-correlated component is expected to he negligible. We find the H(alpha)-correlated component to be consistent with zero for each region, and we find that addition of an H(alpha)-correlated component in modeling the foreground emission has negligible effect on derived CIB results. Our CIB detections and 2(sigma) upper limits are essentially the same as those derived by Hauser et al. and are given by (nu)I(sub nu)(nW/sq m/sr) < 75, < 32, 25+/-8, and 13+/-3 at gamma = 60, 100, 140, and 240 microns, respectively. Our residuals have not been subjected to a detailed anisotropy test, so our CIB results do not supersede those of Hauser et al. Mie derive upper limits on the 100 micron emissivity of the ionized medium that are typically about 40% of the 100 micron emissivity of the neutral atomic medium. This low value may be caused in part by a lower dust-to-gas mass ratio in the ionized medium than in the neutral medium, and in part by a shortcoming of using H(alpha) intensity as a tracer of far infrared emission. If H(alpha) is not a reliable tracer, our analysis would underestimate the emissivity of the ionized medium, and both our analysis and the Hauser et al. analysis may slightly overestimate the CIB. We estimate the possible effect for the CIB to be only about 5%, which is much smaller than the quoted uncertainties. From a comparison of the Hauser et al. CIB results with the integrated galaxy brightness from Spitzer source counts, we obtain 2(sigma) upper limits on a possible diffuse CIB component that are 26 nW/sq m/sr at 140 microns and 8.5 nW/sq m/sr at 240 microns.

Odegard, N.↗
NASA NTRS1995

Time-Dependent Photodissociation Regions

We present theoretical models of the time-dependent thermal and chemical structure of molecular gas suddenly exposed to far-ultraviolet (FUV) (6 eV less than hv less than 13.6 eV) radiation fields and the consequent time- dependent infrared emission of the gas. We focus on the response of molecular hydrogen for cloud densities ranging from n = 10(exp 3) to 10(exp 6)/cu cm and FUV fluxes G(sub 0) = 10(exp 3)-10(exp 6) times the local FUV interstellar flux. For G(sub 0)/n greater than 10(exp -2) cu cm, the emergent H(sub 2) vibrational line intensities are initially larger than the final equilibrium values. The H(sub 2) lines are excited by FUV fluorescence and by collisional excitation in warm gas. Most of the H(sub 2) intensity is generated at a characteristic hydrogen column density of N approximately 10(exp 21)/sq cm, which corresponds to an FUV optical depth of unity caused by dust opacity. The time dependence of the H(sub 2) intensities arises because the initial abundances of H(sub 2) at these depths is much higher than the equilibrium values, so that H(sub 2) initially competes more effectively with dust in absorbing FUV photons. Considerable column densities of warm (T approximately 1000) K H(sub 2) gas can be produced by the FUV pumping of H(sub 2) vibrational levels followed by collisional de-excitation, which transfers the energy to heat. In dense (n greater than or approximately 10(exp 5)/cu cm) gas exposed to high (G(sub 0) greater than or approximately 10(exp 4)) fluxes, this warm gas produces a 2-1 S(1)/1-0 S(l) H(sub 2) line ratio of approximately 0.1, which mimics the ratio found in shocked gas. In lower density regions, the FUV pumping produces a pure-fluorescent ratio of approximately 0.5. We also present calculations of the time dependence of the atomic hydrogen column densities and of the intensities of 0 I 6300 A, S II 6730 A, Fe II 1.64 microns, and rotational OH and H20 emission. Potential applications include star-forming regions, clouds near active galactic nuclei, and planetary nebulae. We apply our models to five planetary nebulae and conclude that only BD +30deg3639 shows evidence of enhanced H(sub 2) emission due to (high) nonequilibrium H(sub 2) abundances.

Hollenbach, David↗
DOE OSTI2023

Crystal chemistry at high pressure

The chemistry we are taught in school, and we experience in our daily existence occurs at 1 atm. However, pressure spans an astounding 62 orders of magnitude in the Universe in going from the void of interstellar space to the crushing conditions at the center of a neutron star. The way in which pressure affects chemistry is important for Earth and planetary sciences, materials science, in understanding the extreme conditions experienced in nuclear explosions, and it may be key in addressing the future energy needs of our society. In this article we outline how the often neglected pressure variable affects chemistry, beginning from the way in which atomic energy levels are altered. This lays the foundation for understanding the unique crystal and electronic structures that emerge when matter is squeezed, as well as pressure’s effect on chemical reactivity. Finally, we give an overview of the main concepts behind conventional, or phonon-mediated, superconductivity, and describe how the pressure variable may be key in discovering and designing light-element based materials whose superconducting critical temperatures approach room temperature. Here, we discuss some of the main families of superconducting hydrides that have been predicted computationally, and the experimental successes in this exciting and rapidly developing field.

Chemical bonding↗
DOE OSTI2021

Applying the Tremaine–Weinberg Method to Nearby Galaxies: Stellar-mass-based Pattern Speeds and Comparisons with ISM Kinematics

We apply the Tremaine–Weinberg method to 19 nearby galaxies using stellar mass surface densities and velocities derived from the PHANGS-MUSE survey, to calculate (primarily bar) pattern speeds (Ω{sub P}). After quality checks, we find that around half (10) of these stellar-mass-based measurements are reliable. For those galaxies, we find good agreement between our results and previously published pattern speeds, and we use rotation curves to calculate major resonance locations (corotation radii and Lindblad resonances). We also compare these stellar-mass-derived pattern speeds with Hα (from MUSE) and CO(J = 2 − 1) emission from the PHANGS-ALMA survey. We find that in the case of these clumpy interstellar medium (ISM) tracers, this method erroneously gives a signal that is simply the angular frequency at a representative radius set by the distribution of these clumps (Ω{sub clump}), and that this Ω{sub clump} is significantly different from Ω{sub P} (∼20% in the case of Hα, and ∼50% in the case of CO). Thus, we conclude that it is inadvisable to use “pattern speeds” derived from ISM kinematics. Finally, we compare our derived pattern speeds and corotation radii, along with bar properties, to the global parameters of these galaxies. Consistent with previous studies, we find that galaxies with a later Hubble type have a larger ratio of corotation radius to bar length, more molecular-gas-rich galaxies have higher Ω{sub P}, and more bulge-dominated galaxies have lower Ω{sub P}. Unlike earlier works, however, there are no clear trends between the bar strength and Ω{sub P}, nor between the total stellar mass surface density and the pattern speed.

74 ATOMIC AND MOLECULAR PHYSICS↗
NASA NTRS1990

Empirical relationships between gas abundances and UV selective extinction

Several studies of gas-phase abundances in lines of sight through the outer edges of dense clouds are summarized. These lines of sight have 0.4 less than E(B-V) less than 1.1 and have inferred spatial densities of a few hundred cm(-3). The primary thrust of these studies has been to compare gaseous abundances in interstellar clouds that have various types of peculiar selective extinction. To date, the most notable result has been an empirical relationship between the CN/Fe I abundance ratio and the depth of the 2200 A extinction bump. It is not clear at the present time, however, whether these two parameters are linearly correlated or the data are organized into two discrete ensembles. Based on 19 samples and assuming the clouds form discrete ensembles, lines of sight that have a CN/Fe I abundance ratio greater than 0.3 (dex) appear to have a shallow 2.57 plus or minus 0.55 bump compared to 3.60 plus or minus 0.36 for other dense clouds and compared to the 3.6 Seaton (1979) average. The difference in the strength of the extinction bump between these two ensembles is 1.03 plus or minus 0.23. Although a high-resolution IUE survey of dense clouds is far from complete, the few lines of sight with shallow extinction bumps all show preferential depletion of certain elements, while those lines of sight with normal 2200 A bumps do not. Ca II, Cr II, and Mn II appear to exhibit the strongest preferential depletion compared to S II, P II, and Mg II. Fe II and Si II depletions also appear to be enhanced somewhat in the shallow-bump lines of sight. It should be noted that Copernicus data suggest all elements, including the so-called nondepletors, deplete in diffuse clouds (Snow and Jenkins 1980, Joseph 1988). Those lines of sight through dense clouds that have normal 2200 A extinction bumps appear to be extensions of the depletions found in the diffuse interstellar medium. That is, the overall level of depletion is enhanced, but the element-to-element abundances are similar to those in diffuse clouds. In a separate study, the abundances of neutral atoms were studied in a dense cloud having a shallow 2200 A bump and in one with a normal strength bump.

Joseph, Charles L.↗
NASA NTRS2013

Chemical Enrichment and Physical Conditions in IZw18*

Low-metallicity star-forming dwarf galaxies are prime targets to understand the chemical enrichment of the interstellar medium. The H I region contains the bulk of the mass in blue compact dwarfs, and it provides important constraints on the dispersal and mixing of heavy elements released by successive star-formation episodes. The metallicity of the H I region is also a critical parameter to investigate the future star-formation history, as metals provide most of the gas cooling that will facilitate and sustain star formation. Aims. Our primary objective is to study the enrichment of the H I region and the interplay between star-formation history and metallicity evolution. Our secondary obje ctive is to constrain the spatial- and time-scales over which the HI and H II regions are enriched, and the mass range of stars responsible for the heavy element production. Finally, we aim to examine the gas heating and cooling mechanisms in the H I region. Methods. We observed the most metal-poor star-forming galaxy in the Local Universe, I Zw 18, with the Cosmic Origin Spectrograph onboard Hubble. The abundances in the neutral gas are derived from far-ultraviolet absorption-lines (H I, CIII, CIIi*, N I, OI,...) and are compared to the abundances in the H II region. Models are constructed to calculate the ionization structure and the thermal processes. We investigate the gas cooling in the HIi region through physical diagnostics drawn from the fine-structure level of C+. Results. We find that H I region abundances are lower by a factor of approx 2 as compared to the H II region. There is no differential depletion on dust between the H I and H II region. Using sulfur as a metallicity tracer, we calculate a metallicity of 1/46 Z(solar) (vs. 1/31 Z(solar) in the H II region). From the study of the C/O, [O/Fe], and N/O abundance ratios, we propose that C, N, O, and Fe are mainly produced in massive stars. We argue that the H I envelope may contain pockets of pristine gas with a metallicity essentially null. Finally, we derive the physical conditions in the H I region by investigating the C II* absorption line. The cooling rate derived from C II* is consistent with collisions with H(sup 0) atoms in the diffuse neutral gas. We calculate the star-formation rate from the CII* cooling rate assuming that photoelectric effect on dust is the dominant gas heating mechanism. Our determination is in good agreement with the values in the literature if we assume a low dust-to-gas ratio (approx 2000 times lower than the Milky Way value).

far-ultraviolet absorption-lines↗
DOE OSTI2025

Molecular Mass Growth Processes to Polycyclic Aromatic Hydrocarbons through Radical–Radical Reactions Exploiting Photoionization Reflectron Time-of-Flight Mass Spectrometry

Polycyclic aromatic hydrocarbons (PAHs) represent critical building blocks in molecular mass growth processes to carbonaceous nanoparticles, referred to as interstellar and circumstellar grains along with soot particles in astrophysical environments and combustion systems, respectively. Recent advancements on elucidating elementary steps to PAHs have utilized reactions of aromatic radicals, resonantly stabilized free radicals, and aliphatic radicals with closed shell hydrocarbons. However, the role of radical–radical reactions (RRRs) leading to PAHs has remained largely unexplored on the molecular level due to preceding experimental challenges in producing sufficiently high number densities of radical reactants for isomer-selective detection of products from bimolecular and termolecular reactions. This Account offers the latest developments in our knowledge on the mechanisms and pathways to PAHs via RRRs probed in a chemical microreactor at temperatures as high as 1600 K. Product preservation in a molecular beam coupled with synchrotron vacuum ultraviolet photoionization reflectron time-of-flight mass spectrometry and photoelectron photoion coincidence spectroscopy enabled isomer-selective detection of PAHs of up to three rings by their photoionization efficiency curves, which were fit with a linear combination of reference curves for identification. Experiments were combined with computational fluid dynamics modeling of the physicochemical processes in the microreactor, as well as high-level electronic structure calculations to reveal the reaction pathways of each system. Six distinct reaction mechanisms were discovered in this work: propargyl addition─benzannulation (PABA), methyl addition─ring expansion (MARE), cyclopentadienyl addition─naphthylization (CPAN), fulvenallenyl addition─cyclization─aromatization (FACA), benzyl addition─aromatization (BAA), and phenyl addition─pentacyclization (PAP). By systematically varying the number of carbon atoms in the radical reactants, molecular mass growth processes involving reactions between radicals with odd numbers of carbon atoms access aromatics carrying one, two, or three six-membered rings, whereas reactions between even- and odd-carbon-numbered radicals produce aromatics combining five- and six-membered rings. Our investigations reveal unconventional cycloadditions on excited state triplet surfaces, additions of radicals to low spin density carbon-centered radicals, spiroaromatic and fulvene-type intermediates, and highly strained bicyclic reaction intermediates, challenging current perceptions of PAH molecular mass growth processes. All of the listed mechanisms, except for FACA, feature endoergic reactions or barriers which lie above the separated reactants and therefore might be central to circumstellar environments of carbon-rich stars and planetary nebulae as their descendants, but they play no role in the gas phase of cold molecular clouds where temperatures as low as 10 K dominate. Altogether, this work provides detailed reaction mechanisms of PAH growth processes, advancing our knowledge of the chemistry of carbonaceous matter in the universe.

Addition reactions↗
NASA NTRS1994

Composition of interstellar clouds in the disk and halo. 2: Gamma(sup 2) Velorum

High-resolution observations of gamma(sup 2) Vel with the Goddard High-Resolution Spectrograph (GHRS) echelle on the Hubble Space Telescope reveal the presence of seven narrow absorption components, with LSR velocities between -23 and +9 km s(exp -1). Three of these show column density ratios N(S(++))/N(S(+)) and N(P(++))/N(P+)) of about 1 or more, and can be identified as H II regions, while the other four are H I regions, consistent with the O I profile and with the overall H(sup 0) column density of 5.9 x 10(exp 19) cm(exp -2), given the usual assumptions that S is undepleted while O has a depletion D(O) = -0.3 dex. The depletions of Fe, Si, and Mn, which could be measure accurately for two of the four H I regions (components 6 and 7), differ somewhat from the values of D(sub ws) found for slowly moving warm clouds in HD 93521; in particular, for the component at 4.0 km s(exp -1) (No. 6), abosolute of D exceeds absolute of D(sub ws) by 0.1-0.4 dex, while for that at 9.3 km s(exp -1) (No. 7), absolute of D equals absolute of D(sub ws) on the average. The observed ratio of Fe + Mg atoms to Si atoms in the grains of component 6 is 2.04 +/-0.10, consistent with an olivine grain composition; the Fe/Mg ratio is 1.5 +/- 0.2. The electron density in component 6, determined from the C II(sup *) feature, is 0.075 +/- 0.013 cm (exp -3), about two-thirds of that found for clouds of this velocity in HD 93521. In the two conspicuous H II regions, components 3 and 4, n(sub e), determined from the Si II(sup *) feature, is about 1 cm(exp -3). From the column density of S(+) + S(++) in these two components, the total H II path length is about 40 pc. With the radius of a wind-blown bubble around gamma(sup 2) Vel set equal to 60 pc, the effective Stromgren radius is about 100 pc, requiring that T approx. equal to 50,000 K for the Wolf-Rayet component of the gamma(sup 2) Vel binary. Since zeta Pup is a comparable source of ionizing radiation, this temperature is an upper limit. The profiles of the strongest H2 absorption features, from Copernicus archives, indicate that the absorbing molecules have a mean velocity identical with that of the strongest H II component (No. 4). We have no explanation for the possible presence of these H2 molecules in a region of ionized H. Alternatively, the H2 profiles can be explained by molecules in the two adjacent (in velocity) H I regions, components 2 and 5, provided their H I gas has densities and temperatures typical of normal cold clouds. The GHRS data show absorption by highly ionized atoms Si(3+) and C(3+), N(4+) in broad features, in addition to the narrow-line absorption by Si(3+) and C(3+) observed in the dominant H II components, Nos. 3 and 4. The broad C(3+) and N(4+) features have widths corresponding to T in the range (4-8) x 10(exp 5) K, consistent with the broad O(5+) line shown in Copernicus data. Despite some observational uncertainties, the ratios of column densities in the broad C(3+), N(4+), and O(5+) features agree to +/- 0.1 dex with theoretical values for warm gas, heating and evaporating by thermal conduction from an adjacent hot region. Outward evaporation from an isolated cloud in a hot ambient gas cannot be distinguished, on the basis of these data, from inward evaporation of a warm shell, compressed by an expanding, hot stellar-wind bubble. For several halo stars, the C IV/O VI ratio has a quite different average value, perhaps consistent with cooling of infalling hot gas instead of conductive heating and evaporation.

Fitzpatrick, Edward L.↗