Visible-light photoionization of aromatic molecules in water-ice: Organic chemistry across the universe with less energy

Lignell, Antti; Tenelanda-Osorio, Laura Isabel; Gudipati, Murthy S.

doi:10.1016/j.cplett.2021.138814

Cited by 7 publications

(3 citation statements)

References 48 publications

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“…It has been shown that PAHs embedded in ASW, when irradiated by VUV light, undergo erosion processes and lead to oxidation products such as alcohols and ketones [12] via the formation of cationic intermediates. Interestingly, the formation of oxygenated PAHs is also observed in ASW when using low energy UV-visible irradiation [13][14][15][16]. It has also been shown that small complexes of coronene and water isolated in cryogenic argon matrices exhibit photochemical reactions similar to those observed in ASW [17].…”

Section: Introductionmentioning

confidence: 83%

Water Clusters in Interaction with Corannulene in a Rare Gas Matrix: Structures, Stability and IR Spectra

et al. 2022

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The interaction of polycyclic aromatic hydrocarbons (PAHs) with water is of paramount importance in atmospheric and astrophysical contexts. We report here a combined theoretical and experimental study of corannulene-water interactions in low temperature matrices and of the matrix’s influence on the photoreactivity of corannulene with water. The theoretical study was performed using a mixed density functional based tight binding/force field approach to describe the corannulene-water clusters trapped in an argon matrix, together with Born-Oppenheimer molecular dynamics to determine finite-temperature IR spectra. The results are discussed in the light of experimental matrix isolation FTIR spectroscopic data. We show that in the solid phase, π isomers of (C20H10)(H2O)n, with n = 2 or 3, are energetically favored. These π complexes are characterized by small shifts in corannulene vibrational modes and large shifts in water bands. These π structures, particularly stable in the case of the water trimer where the water cluster is trapped “inside” the corannulene bowl, may account for the difference in photoreactivity of non-planar–compared to planar–PAHs with water. Indeed, planar PAHs such as pyrene and coronene embedded in H2O:Ar matrices form σ isomers and react with water to form alcohols and quinones under low energy UV irradiation, whereas no photoreactivity was observed for corannulene under the same experimental conditions.

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Section: Introductionmentioning

confidence: 83%

Water Clusters in Interaction with Corannulene in a Rare Gas Matrix: Structures, Stability and IR Spectra

et al. 2022

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“…The most important indirect effects of shortwave UV radiation in a chemical medium is the production of vLEEs 10 , 32 – 34 . Many photochemical channels have been recently reported that enable the efficient production of vLEEs as a result of shortwave UV irradiation in medium containing π molecules 10 , 32 , 33 . In the reported ICD experiments of refs.…”

Section: Mainmentioning

confidence: 99%

Prebiotic chemical origin of biomolecular complementarity

Sajeev

2023

Commun Chem

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The early Earth, devoid of the protective stratospheric ozone layer, must have sustained an ambient prebiotic physicochemical medium intensified by the co-existence of shortwave UV photons and very low energy electrons (vLEEs). Consequently, only intrinsically stable molecules against these two co-existing molecular destructors must have proliferated and thereby chemically evolved into the advanced molecules of life. Based on this view, we examined the stability inherent in nucleobases and their complementary pairs as resistance to the molecular damaging effects of shortwave UV photons and vLEEs. This leads to the conclusion that nucleobases could only proliferated as their complementary pairs under the unfavorable prebiotic conditions on early Earth. The complementary base pairing not only enhances but consolidates the intrinsic stability of nucleobases against short-range UV photons, vLEEs, and possibly many as-yet-unknown deleterious agents co-existed in the prebiotic conditions of the early Earth. In short, complementary base pairing is a manifestation of chemical evolution in the unfavorable prebiotic medium created by the absence of the stratospheric ozone layer.

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“…35,53,54 The photochemistry of pyrene in water ice has also been studied. 55,56 Pyrene and other PAHs have been the subject of many theoretical studies. Singh et al 57 have performed R-matrix calculations to obtain electron scattering cross sections for anthracene and pyrene in the range 0.1-15 eV.…”

Section: Introductionmentioning

confidence: 99%

Coincidence mass spectrometry study of double ionization of pyrene by 70 eV electron impact

van der Burgt,

Gradziel

2024

Phys. Chem. Chem. Phys.

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Visible-light photoionization of aromatic molecules in water-ice: Organic chemistry across the universe with less energy

Cited by 7 publications

References 48 publications

Water Clusters in Interaction with Corannulene in a Rare Gas Matrix: Structures, Stability and IR Spectra

Water Clusters in Interaction with Corannulene in a Rare Gas Matrix: Structures, Stability and IR Spectra

Prebiotic chemical origin of biomolecular complementarity

Coincidence mass spectrometry study of double ionization of pyrene by 70 eV electron impact

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