Ambient-light-induced intermolecular Coulombic decay in unbound pyridine monomers

Barik, Saroj; Dutta, Saurav; Behera, Nihar Ranjan; Kushawaha, Rajesh K.; Sajeev, Y.; Aravind, G.

doi:10.1038/s41557-022-01002-2

Cited by 10 publications

(12 citation statements)

References 32 publications

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“…However, since these high-energy radiation tracks do not provide a favorable environment for the proliferation of enough prebiotic molecules, the direct role of secondary electrons in the chemical evolution of prebiotic molecules has remained largely unexplored. The role of vLEEs in prebiotic chemical evolution has become relevant following a recent report that large numbers of vLEEs are efficiently produced even upon the absorption of ambient-intensity UV photons in a system abundant with π -molecules 10 .…”

Section: Mainmentioning

confidence: 99%

“…However, the role of multifaceted indirect effects of UV radiation on prebiotic chemical evolution has not been sufficiently discussed. 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 .…”

Section: Mainmentioning

confidence: 99%

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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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Section: Mainmentioning

confidence: 99%

Section: Mainmentioning

confidence: 99%

Prebiotic chemical origin of biomolecular complementarity

Sajeev

2023

Commun Chem

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“…Cluster formation in supersonic free expansion is important in generating isolated molecules for laser plasma experiments 1 , generation of fast electrons and ions 2 , conversion of high-energy charge particles into neutral atoms 3 and generating superhot microplasma for laser fusion experiments 4 . Furthermore, the information regarding cluster formation is an important aspect in the study of photo induced chemical reactions 5 . Clusters are formed when free expanding jet undergoes isentropic cooling along the flow and the temperature of the gas reaches below the condensation point.…”

Section: Introductionmentioning

confidence: 99%

Spatial mapping of low pressure cluster jets using Rayleigh scattering

Patel

Geethika

Thomas

et al. 2023

Sci Rep

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In this work, we report evolution of atomic clusters in a highly under-expanded supersonic jet of Argon. A high resolution and sensitive Rayleigh scattering based experimental set-up is designed to overcome the limitations encountered in conventional set-ups. Further, the measurement range could be extended from a few nozzle diameters to 50 nozzle diameters. Simultaneously, we had been able to generate 2D profiles of the distribution of clusters inside the jet. This paves the way to track the growth of clusters along the flow direction experimentally, which until now was limited to few nozzle diameters. The results show that spatial distribution of clusters inside the supersonic core deviates considerably from the prediction of the free expansion model. We exploit this to estimate cluster growth along the expansion direction. Further, it is observed that the growth of the clusters gets saturated after a certain distance from the nozzle. At the jet boundary, we see substantial cluster strengthening immediately upstream of barrel shock while the normal shock exhibits disintegration of clusters. These observations are noticed for the first time, which, we believe will further the understanding of cluster dynamics in a supersonic jet.

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“…In the T-shape structure, a CH group is interacting through the H atom with the other ring to form a CH−π interaction. Compared to the numerous existing studies of the benzene dimer, there is a scarcity of investigations of N-containing heteroaromatic dimers especially by experiment, in spite of their clear biochemical importance. − For example, N heteroatoms are prevalent in nucleic acid bases that influence the molecular interaction energies and hence the structures and dynamics of DNA and RNA. − …”

mentioning

confidence: 99%

Revealing the Role of N Heteroatoms in Noncovalent Aromatic Interactions by Ultrafast Intermolecular Coulombic Decay

Zhou,

Jia,

Xue

et al. 2024

J. Phys. Chem. Lett.

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Despite the widely recognized importance of noncovalent interactions involving aromatic rings in many fields, our understanding of the underlying forces and structural patterns, especially the impact of heteroaromaticity, is still incomplete. Here, we investigate the relaxation processes that follow inner-valence ionization in a range of molecular dimers involving various combinations of benzene, pyridine, and pyrimidine, which initiate an ultrafast intermolecular Coulombic decay process. Multiparticle coincidence momentum spectroscopy, combined with ab initio calculations, enables us to explore the principal orientations of these fundamental dimers and, thus, to elucidate the influence of N heteroatoms on the relative preference of the aromatic π-stacking, H-bonding, and CH−π interactions and their dependence on the number of nitrogen atoms in the rings. Our studies reveal a sensitive tool for the structural imaging of molecular complexes and provide a more complete understanding of the effects of N heteroatoms on the noncovalent aromatic interactions at the molecular level.

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Ambient-light-induced intermolecular Coulombic decay in unbound pyridine monomers

Cited by 10 publications

References 32 publications

Prebiotic chemical origin of biomolecular complementarity

Prebiotic chemical origin of biomolecular complementarity

Spatial mapping of low pressure cluster jets using Rayleigh scattering

Revealing the Role of N Heteroatoms in Noncovalent Aromatic Interactions by Ultrafast Intermolecular Coulombic Decay

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