Photochemical reaction processes during vacuum-ultraviolet irradiation of water ice

Yabushita, Akihiro; Hama, Tetsuya; Kawasaki, Masahiro

doi:10.1016/j.jphotochemrev.2013.01.001

Cited by 34 publications

(41 citation statements)

References 179 publications

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“…The present experimental study suggests that formation of nitrile functional groups through gas-phase reactions following N 2 photodissociation is plausible (38). Once formed, these functional groups may freeze-out in the ice and possibly synthesize PANHs with high 15 N enrichment under UV exposure within the ice (37,(39)(40)(41) (Fig. 4).…”

Section: Discussionmentioning

confidence: 67%

Massive isotopic effect in vacuum UV photodissociation of N ₂ and implications for meteorite data

Chakraborty

Muskatel

Jackson

et al. 2014

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

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Nitrogen isotopic distributions in the solar system extend across an enormous range, from −400‰, in the solar wind and Jovian atmosphere, to about 5,000‰ in organic matter in carbonaceous chondrites. Distributions such as these require complex processing of nitrogen reservoirs and extraordinary isotope effects. While theoretical models invoke ion-neutral exchange reactions outside the protoplanetary disk and photochemical self-shielding on the disk surface to explain the variations, there are no experiments to substantiate these models. Experimental results of N 2 photolysis at vacuum UV wavelengths in the presence of hydrogen are presented here, which show a wide range of enriched δ 15 N values from 648‰ to 13,412‰ in product NH 3 , depending upon photodissociation wavelength. The measured enrichment range in photodissociation of N 2 , plausibly explains the range of δ 15 N in extraterrestrial materials. This study suggests the importance of photochemical processing of the nitrogen reservoirs within the solar nebula.nitrogen isotopes | organic molecules | perturbation

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Section: Discussionmentioning

confidence: 67%

Massive isotopic effect in vacuum UV photodissociation of N ₂ and implications for meteorite data

Chakraborty

Muskatel

Jackson

et al. 2014

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

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“…[38] Another possible route is the uptake of acetylene into the water/ice phase, in which the generation of reactive-oxygen species under UV radiation could be favored at lower energies. The atmospheric processing of acetylene in the presence of water in gas phase leads to the formation of reactive intermediates as glyoxal, which can enter the liquid/solid water pool readily due to its high Henrys law constant.…”

Section: Productmentioning

confidence: 99%

A New Route for the Prebiotic Synthesis of Nucleobases and Hydantoins in Water/Ice Solutions Involving the Photochemistry of Acetylene

Menor‐Salván

Marín-Yaseli

2013

Chemistry A European J

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The origin of nucleobases and other heterocycles is a classic question in the chemistry of the origins of life. The construction of laboratory models for the abiotic synthesis of nitrogen heterocycles in plausible natural conditions also aids the understanding and prediction of chemical species in the Solar System. Here, we report a new explanation for the origin of hydantoins, purines, and pyrimidines in eutectic water/ice/urea solutions driven by ultraviolet irradiation (in the 185-254 nm range, UVC) of acetylene under anoxic conditions. An analysis of the products indicates the synthesis of hydantoin and 5-hydroxyhydantoin, the purines uric acid, xanthine, and guanine, and the pyrimidines uracil and cytosine. The synthesis occurred together with the photo-oxidation of bases in a complex process for which possible pathways are proposed. In conclusion, an acetylene-containing atmosphere could contribute to the origin of nucleobases in the presence of a urea/water system by an HCN-independent mechanism. The presence of ice has a dual role as a favorable medium for the synthesis of nucleobases and protection against degradation and as a source of free radicals for the synthesis of highly oxidized heterocycles. A mechanism for the origin of hydantoins and uracil from urea in plausible conditions for prebiotic chemistry is also proposed.

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“…Characterisation of amorphous solid water (ASW) is of general interest in surface chemistry [1][2][3][4][5] , but especially relevant to astrophysics and planetary science where solid water is an important component of comets 6 , planetary satellites 7,8 , and the icy mantles that coat interstellar dust grains [9][10][11] . The surface chemistry of nano-to micrometre-sized particles plays an important role in molecular synthesis in interstellar space 12 .…”

Section: Introductionmentioning

confidence: 99%

“…The surface chemistry of nano-to micrometre-sized particles plays an important role in molecular synthesis in interstellar space 12 . In cold, dense molecular clouds, dust grain particles are covered by icy mantles that contain mainly H 2 O in combination with minor quantities of other molecules such as CO, CO 2 , NH 3 , and CH 4 [13][14][15][16][17][18][19][20][21] .…”

Section: Introductionmentioning

confidence: 99%

“…Fontani et al 42 show that surface chemistry has an important role in determining the fractional deuteration of some molecules (e.g. NH 3 and CH 3 OH) formed on the interstellar grain mantles. This study confirmed that the deuterated fractions of N 2 H + and CH 3 OH, respectively, are good tracers of massive starless cores and early proto-stellar phases, where the evaporation or sputtering of the grain mantles occurs most efficiently 42 .…”

Section: Introductionmentioning

confidence: 99%

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Molecular hydrogen production from amorphous solid water during low energy electron irradiation

Gadallah

Marchione

Koehler

et al. 2017

Phys. Chem. Chem. Phys.

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This work investigates the production of molecular hydrogen isotopologues (H 2 , HD, and D 2 ) during low energy electron irradiation of layered and isotopically labelled thin films of amorphous solid water (ASW) in ultrahigh vacuum. Experimentally, the production of these molecules with both irradiation time and incident electron energy in the range 400 to 500 eV is reported as a function of the depth of a buried D 2 O layer in an H 2 O film. H 2 is produced consistently in all measurements, reflecting the H 2 O component of the film, though it does exhibit a modest reduction in intensity at the time corresponding to product escape from the buried D 2 O layer. In contrast, HD and D 2 production exhibit peaks at times corresponding to product escape from the buried D 2 O layer in the composite film. These features broaden the deeper the HD or D 2 is formed due to diffusion. A simple random-walk model is presented that can qualitatively explain the appearance profile of these peaks as a function of the incident electron penetration.

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Photochemical reaction processes during vacuum-ultraviolet irradiation of water ice

Cited by 34 publications

References 179 publications

Massive isotopic effect in vacuum UV photodissociation of N ₂ and implications for meteorite data

Massive isotopic effect in vacuum UV photodissociation of N ₂ and implications for meteorite data

A New Route for the Prebiotic Synthesis of Nucleobases and Hydantoins in Water/Ice Solutions Involving the Photochemistry of Acetylene

Molecular hydrogen production from amorphous solid water during low energy electron irradiation

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Photochemical reaction processes during vacuum-ultraviolet irradiation of water ice

Cited by 34 publications

References 179 publications

Massive isotopic effect in vacuum UV photodissociation of N 2 and implications for meteorite data

Massive isotopic effect in vacuum UV photodissociation of N 2 and implications for meteorite data

A New Route for the Prebiotic Synthesis of Nucleobases and Hydantoins in Water/Ice Solutions Involving the Photochemistry of Acetylene

Molecular hydrogen production from amorphous solid water during low energy electron irradiation

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Massive isotopic effect in vacuum UV photodissociation of N ₂ and implications for meteorite data

Massive isotopic effect in vacuum UV photodissociation of N ₂ and implications for meteorite data