In-Situ Probing of Radiation-Induced Processing of Organics in Astrophysical Ice Analogs—novel Laser Desorption Laser Ionization Time-of-Flight Mass Spectroscopic Studies

Gudipati, Murthy S.; Yang, Rui Q.

doi:10.1088/2041-8205/756/1/l24

Cited by 66 publications

(54 citation statements)

References 50 publications

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“…Understanding how soot forms and interacts with OC can lead to more efficient combustion technologies that reduce soot emissions, which would have many benefits (e.g., reduced global warming and anthropogenic hydrological impact and reduced concentrations of toxic and carcinogenic environmental pollutants). Flame studies of soot and related OC are, however, also important because they can provide benchmarks for hydrocarbon growth and oxidation models important in other research fields, such as astrophysics (43) and fuel cells (44).…”

Section: Discussionmentioning

confidence: 99%

Formation and emission of large furans and oxygenated hydrocarbons from flames

Johansson

Dillstrom

Monti

et al. 2016

Proc. Natl. Acad. Sci. U.S.A.

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Many oxygenated hydrocarbon species formed during combustion, such as furans, are highly toxic and detrimental to human health and the environment. These species may also increase the hygroscopicity of soot and strongly influence the effects of soot on regional and global climate. However, large furans and associated oxygenated species have not previously been observed in flames, and their formation mechanism and interplay with polycyclic aromatic hydrocarbons (PAHs) are poorly understood. We report on a synergistic computational and experimental effort that elucidates the formation of oxygen-embedded compounds, such as furans and other oxygenated hydrocarbons, during the combustion of hydrocarbon fuels. We used ab initio and probabilistic computational techniques to identify low-barrier reaction mechanisms for the formation of large furans and other oxygenated hydrocarbons. We used vacuum-UV photoionization aerosol mass spectrometry and X-ray photoelectron spectroscopy to confirm these predictions. We show that furans are produced in the high-temperature regions of hydrocarbon flames, where they remarkably survive and become the main functional group of oxygenates that incorporate into incipient soot. In controlled flame studies, we discovered ∼100 oxygenated species previously unaccounted for. We found that large alcohols and enols act as precursors to furans, leading to incorporation of oxygen into the carbon skeletons of PAHs. Our results depart dramatically from the crude chemistry of carbonand oxygen-containing molecules previously considered in hydrocarbon formation and oxidation models and spearhead the emerging understanding of the oxidation chemistry that is critical, for example, to control emissions of toxic and carcinogenic combustion by-products, which also greatly affect global warming.furans | oxygenated hydrocarbons | soot | organic carbon | black carbon

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Section: Discussionmentioning

confidence: 99%

Formation and emission of large furans and oxygenated hydrocarbons from flames

Johansson

Dillstrom

Monti

et al. 2016

Proc. Natl. Acad. Sci. U.S.A.

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“…Indeed, recently a number of new developments have been reported. [22][23][24][25][26][27][28][29][30][31][32] Successful experiments have been reported in which TPD has been combined with vacuum UV (VUV) single photo-ionisation time-of-flight mass spectrometry (TOF-MS), measuring the mass from desorbing species from the ice. 22,23 Diagnostic techniques such as Substrate/Matrix Assisted Laser Desorption Ionisation Time-ofFlight Mass Spectrometry ((S/M)ALDI-TOF-MS) have been introduced.…”

Section: Introductionmentioning

confidence: 99%

“…A similar approach was recently applied, to investigate radiation-induced processes of Polycyclic Aromatic Hydrocarbons (PAHs), embedded in interstellar ice analogous, using Resonant Enhanced Multi Photon Ionisation (REMPI) as ionisation source. 24,25 Alternatively, the laser energy can be coupled into the substrate to induce the thermal desorption of ice constituents. 28,29,[33][34][35][36] The desorbed ice constituents are subsequently ionised, for example, using electron impact ionisation, and analysed with a TOF-MS.…”

Section: Introductionmentioning

confidence: 99%

Laser desorption time-of-flight mass spectrometry of ultraviolet photo-processed ices

Paardekooper

Bossa

Isokoski

et al. 2014

Review of Scientific Instruments

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A new ultra-high vacuum experiment is described that allows studying photo-induced chemical processes in interstellar ice analogues. MATRI(2)CES - a Mass Analytical Tool to study Reactions in Interstellar ICES applies a new concept by combining laser desorption and time-of-flight mass spectrometry with the ultimate goal to characterize in situ and in real time the solid state evolution of organic compounds upon UV photolysis for astronomically relevant ice mixtures and temperatures. The performance of the experimental setup is demonstrated by the kinetic analysis of the different photoproducts of pure methane (CH4) ice at 20 K. A quantitative approach provides formation yields of several new species with up to four carbon atoms. Convincing evidence is found for the formation of even larger species. Typical mass resolutions obtained range from M/ΔM ∼320 to ∼400 for CH4 and argon, respectively. Additional tests show that the typical detection limit (in monolayers) is ⩽0.02 ML, substantially more sensitive than the regular techniques used to investigate chemical processes in interstellar ices.

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“…Other studies [45,46] have revealed that under conditions similar to those in the interstellar medium, polynuclear aromatic hydrocarbons (PAH) change to amino acids and nucleotides through hydrogenation, hydroxylation or partial oxidation. The database for tracking PAH in the universe has been updated and enriched.…”

Section: Cosmic Dustmentioning

confidence: 99%

Natural Sources of Nanoparticles

Strambeanu¹,

Demetrovici²,

Dragoş

2014

Nanoparticles' Promises and Risks

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This chapter deals with the major natural sources of nanoparticles in the atmosphere: volcanic eruptions, desert surfaces, dust from cosmic sources located in the solar system or outside it. Details are given about the composition of very fine particles according to their type, the successive or parallel chemical transformations that can occur among them or when they meet the major components of the atmosphere (nitrogen, oxygen, carbon dioxide). The authors specify possible ways of evolution from the mineral kingdom to organic substances through nanoparticles originating from cosmic dust, based on suppositions that are provided in the literature of the field and accepted based on physical and chemical computational models.

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In-Situ Probing of Radiation-Induced Processing of Organics in Astrophysical Ice Analogs—novel Laser Desorption Laser Ionization Time-of-Flight Mass Spectroscopic Studies

Cited by 66 publications

References 50 publications

Formation and emission of large furans and oxygenated hydrocarbons from flames

Formation and emission of large furans and oxygenated hydrocarbons from flames

Laser desorption time-of-flight mass spectrometry of ultraviolet photo-processed ices

Natural Sources of Nanoparticles

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