From underwear to non-equilibrium thermodynamics: physical chemistry informs the origin of life
Editorial for the themed issue on ‘Prebiotic Chemistry and the Molecular Origins of Life’. The dictum Omne vivum ex vivo is misleading: life must have arisen from non-living matter.
Is formamide a geochemically plausible prebiotic solvent?
From a geochemical perspective, significant amounts of pure formamide (HCONH2) would have likely been rare on the early Earth.
Sunlight as an energetic driver in the synthesis of molecules necessary for life
This review considers how photochemistry and sunlight-driven reactions can abiotically generate prebiotic molecules necessary for the evolution of life.
On the lack of evolutionary continuity between prebiotic peptides and extant enzymes
The significance of experiments that claim to simulate the properties of prebiotic small peptides and polypeptides as models of the polymers that may have preceded proteins is critically addressed.
A symbiotic view of the origin of life at hydrothermal impact crater-lakes
Submarine hydrothermal vents are generally considered as the likely habitats for the origin and evolution of early life on Earth.
Prebiotic synthesis of nucleic acids and their building blocks at the atomic level – merging models and mechanisms from advanced computations and experiments
Main directions for future computational studies on the origin of the first nucleic acids is outlined.
A ‘bottom up’, ab initio computational approach to understanding fundamental photophysical processes in nitrogen containing heterocycles, DNA bases and base pairs
A systematic computational study of non-radiative decay pathways following UV excitation of selected heterocycles, DNA bases, nucleosides and base-pairs in the gas phase.
Formation of supramolecular assemblies and liquid crystals by purine nucleobases and cyanuric acid in water: implications for the possible origins of RNA
The free nucleobases and mononucleotides of RNA do not form Watson–Crick base pairs in water, a fact that presents several challenges for the prebiotic synthesis of RNA.
Cysteine containing dipeptides show a metal specificity that matches the composition of seawater
Cysteine containing dipeptide metal affinities do not follow the Irving–Williams series but rather follow the concentration trends found in seawater.
Photochemical etiology of promising ancestors of the RNA nucleobases
Barbituric acid and 2,4,6-triaminopyrimidine dissipate ultraviolet radiation efficiently as heat to the environment, thus supporting their feasibility as prebiotic ancestors to the RNA nucleobases.
Pyrite surface environment drives molecular adsorption: cystine on pyrite(100) investigated by X-ray photoemission spectroscopy and low energy electron diffraction
The annealing process for pre-treatment of pyrite surfaces is a critical parameter in promoting ordering on the surface and it has chemical implications on the cystine adsorbed molecules.
Life in the light: nucleic acid photoproperties as a legacy of chemical evolution
Nucleobases exhibit protection against UV photodamage by rapid internal conversion to the ground state. This property may have led to prebiotic photochemical selection.
Ultrafast excited-state dynamics of isocytosine
Nonadiabatic molecular dynamics simulations elucidate the ultrafast photodeactivation mechanisms of alternative nucleobase isocytosine.
THz time-domain spectroscopy of mixed CO2–CH3OH interstellar ice analogs
THz spectroscopy provides an exquisitely sensitive probe into the long-range structure and segregation of mixtures of two primary interstellar ice constituents: carbon dioxide and methanol.
Photophysical properties of pyrrolocytosine, a cytosine fluorescent base analogue
The fluorescence properties of pyrrolocytosine, a cytosine analogue, are investigated using high level ab initio methods, and they are found to be affected by hydrogen bonding to water molecules, as well as by pi-stacking with guanine.
Unified reaction pathways for the prebiotic formation of RNA and DNA nucleobases
The reaction pathways for the prebiotic formation of nucleobases are complex and lead to the formation of a mixture of products.
Internal conversion and intersystem crossing pathways in UV excited, isolated uracils and their implications in prebiotic chemistry
The photodynamic properties of molecules determine their ability to survive in harsh radiation environments.
Probing of molecular replication and accumulation in shallow heat gradients through numerical simulations
Shallow temperature gradients across porous rocks drive highly efficient molecular accumulation processes while simultaneously subjecting them to frequent temperature oscillations.
The evolution of the surface of the mineral schreibersite in prebiotic chemistry
We demonstrate a synthesis of the meteoritic mineral schreibersite (Fe,Ni)3P, study its surface chemistry, and show prebiotic phosphorylation.
The efficiency of driving chemical reactions by a physical non-equilibrium is kinetically controlled
A model system illustrates how the coupling efficiency of a physical non-equilibrium to a chemical reaction is affected by the relative timescales of the respective kinetics.
Non-radiative processes in protonated diazines, pyrimidine bases and an aromatic azine
Protonated diazines have very short excited state lifetimes.
Synthesis of barbituric acid containing nucleotides and their implications for the origin of primitive informational polymers
Nucleotides containing barbituric acid were synthesized and polymerized under prebiotically relevant conditions. This study demonstrates the plausibility of the emergence of primitive informational polymers from ribonucleotides with alternate heterocycles.
Lower temperature optimum of a smaller, fragmented triphosphorylation ribozyme
The temperature optimum of a triphosphorylation ribozyme shifted to lower temperature, after size reduction and fragmentation.
Possible interstellar formation of glycine through a concerted mechanism: a computational study on the reaction of CH2NH, CO2 and H2
Computational studies on the reaction of CH2NH, CO2 and H2 show the possible interstellar formation of glycine in both hot-cores and cold interstellar clouds.
About this collection
This themed collection showcases the growing importance of physical chemistry in understanding the processes involved in the origins of life. The collection was Guest Edited by Professor Irene A. Chen and Professor Mattanjah S. de Vries and is free to access for a limited time.