Hydrogen cyanide (HCN), a key molecule of significant importance in contemporary perspectives on prebiotic chemistry, originates in planetary atmospheres from various processes, such as photochemistry, thermochemistry, and impact chemistry, as well as from delivery by impacts. The resilience of HCN during periods of heavy bombardment, a phenomenon caused by an influx of material on unstable trajectories after accretion, remains relatively understudied. This study extensively investigates the stability of HCN under impact conditions simulated using a laboratory Nd:YAG laser in the ELISE experimental setup. High-resolution infrared spectroscopy was employed to monitor the gas phase composition during these simulations. Impact chemistry was simulated in bulk nitrogen atmospheres with varying mixing ratios of HCN and water vapor. The probed range of compositions spans from ∼0 to 1.8% of HCN and 0 to 2.7% of H2O in a ∼1 bar nitrogen atmosphere. The primary decomposition products of HCN are CO and CO2 in the presence of water and unidentified solid phase products in dry conditions. Our experiments revealed a range of initial HCN decomposition rates between 2.43 × 1015 and 5.17 × 1017 molec J-1 of input energy depending on the initial composition. Notably, it is shown that the decomposition process induced by the laser spark simulating the impact plasma is nonlinear, with the duration of the irradiation markedly affecting the decomposition rate. These findings underscore the necessity for careful consideration and allowance for margins when applying these rates to chemical models of molecular synthesis and decomposition in planetary atmospheres.

• Publication type
• Journal Article MeSH

Recent results in prebiotic chemistry implicate hydrogen cyanide (HCN) as the source of carbon and nitrogen for the synthesis of nucleotide, amino acid and lipid building blocks. HCN can be produced during impact events by reprocessing of carbonaceous and nitrogenous materials from both the impactor and the atmosphere; it can also be produced from these materials by electrical discharge. Here we investigate the effect of high energy events on a range of starting mixtures representative of various atmosphere-impactor volatile combinations. Using continuously scanning time-resolved spectrometry, we have detected ·CN radical and excited CO as the initially most abundant products. Cyano radicals and excited carbon monoxide molecules in particular are reactive, energy-rich species, but are resilient owing to favourable Franck-Condon factors. The subsequent reactions of these first formed excited species lead to the production of ground-state prebiotic building blocks, principally HCN.

• MeSH
• Atmosphere * MeSH
• Nitrogen chemistry   MeSH
• Hydrogen Cyanide chemistry   MeSH
• Carbon Monoxide chemistry   MeSH
• Prebiotics * MeSH
• Carbon chemistry   MeSH
• Earth, Planet * MeSH
• Publication type
• Journal Article MeSH
• Research Support, Non-U.S. Gov't MeSH
• Names of Substances
• Nitrogen MeSH
• Hydrogen Cyanide MeSH
• Carbon Monoxide MeSH
• Prebiotics * MeSH
• Carbon MeSH

The Miller-Urey experiments pioneered modern research on the molecular origins of life, but their actual relevance in this field was later questioned because the gas mixture used in their research is considered too reducing with respect to the most accepted hypotheses for the conditions on primordial Earth. In particular, the production of only amino acids has been taken as evidence of the limited relevance of the results. Here, we report an experimental work, combined with state-of-the-art computational methods, in which both electric discharge and laser-driven plasma impact simulations were carried out in a reducing atmosphere containing NH3 + CO. We show that RNA nucleobases are synthesized in these experiments, strongly supporting the possibility of the emergence of biologically relevant molecules in a reducing atmosphere. The reconstructed synthetic pathways indicate that small radicals and formamide play a crucial role, in agreement with a number of recent experimental and theoretical results.

• Keywords
• asteroid impact, life origins, reducing atmosphere,
• MeSH
• Ammonia chemistry   MeSH
• Atmosphere MeSH
• Models, Chemical MeSH
• Evolution, Chemical MeSH
• Formamides chemistry   MeSH
• Carbon Monoxide chemistry   MeSH
• Oxidation-Reduction MeSH
• Origin of Life MeSH
• RNA chemistry   MeSH
• Publication type
• Journal Article MeSH
• Research Support, Non-U.S. Gov't MeSH
• Names of Substances
• Ammonia MeSH
• formamide MeSH Browser
• Formamides MeSH
• Carbon Monoxide MeSH
• RNA MeSH

The coincidence of the Late Heavy Bombardment (LHB) period and the emergence of terrestrial life about 4 billion years ago suggest that extraterrestrial impacts could contribute to the synthesis of the building blocks of the first life-giving molecules. We simulated the high-energy synthesis of nucleobases from formamide during the impact of an extraterrestrial body. A high-power laser has been used to induce the dielectric breakdown of the plasma produced by the impact. The results demonstrate that the initial dissociation of the formamide molecule could produce a large amount of highly reactive CN and NH radicals, which could further react with formamide to produce adenine, guanine, cytosine, and uracil. Based on GC-MS, high-resolution FTIR spectroscopic results, as well as theoretical calculations, we present a comprehensive mechanistic model, which accounts for all steps taking place in the studied impact chemistry. Our findings thus demonstrate that extraterrestrial impacts, which were one order of magnitude more abundant during the LHB period than before and after, could not only destroy the existing ancient life forms, but could also contribute to the creation of biogenic molecules.

• Keywords
• LIDB, asteroid impact, biomolecules, origin of life,
• Publication type
• Journal Article MeSH
• Research Support, Non-U.S. Gov't MeSH