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Themed collection Prebiotic chemistry and the molecular origins of life

24 articles
Editorial

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.

Graphical abstract: From underwear to non-equilibrium thermodynamics: physical chemistry informs the origin of life
Perspective

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.

Graphical abstract: Is formamide a geochemically plausible prebiotic solvent?
Perspective

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.

Graphical abstract: Sunlight as an energetic driver in the synthesis of molecules necessary for life
Perspective

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.

Graphical abstract: On the lack of evolutionary continuity between prebiotic peptides and extant enzymes
Perspective

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.

Graphical abstract: A symbiotic view of the origin of life at hydrothermal impact crater-lakes
Perspective

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.

Graphical abstract: Prebiotic synthesis of nucleic acids and their building blocks at the atomic level – merging models and mechanisms from advanced computations and experiments
Open Access Perspective

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.

Graphical abstract: A ‘bottom up’, ab initio computational approach to understanding fundamental photophysical processes in nitrogen containing heterocycles, DNA bases and base pairs
Communication

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.

Graphical abstract: Formation of supramolecular assemblies and liquid crystals by purine nucleobases and cyanuric acid in water: implications for the possible origins of RNA
Open Access Communication

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.

Graphical abstract: Cysteine containing dipeptides show a metal specificity that matches the composition of seawater
Communication

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.

Graphical abstract: Photochemical etiology of promising ancestors of the RNA nucleobases
Paper

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.

Graphical abstract: Pyrite surface environment drives molecular adsorption: cystine on pyrite(100) investigated by X-ray photoemission spectroscopy and low energy electron diffraction
Paper

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.

Graphical abstract: Life in the light: nucleic acid photoproperties as a legacy of chemical evolution
Paper

Ultrafast excited-state dynamics of isocytosine

Nonadiabatic molecular dynamics simulations elucidate the ultrafast photodeactivation mechanisms of alternative nucleobase isocytosine.

Graphical abstract: Ultrafast excited-state dynamics of isocytosine
Paper

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.

Graphical abstract: THz time-domain spectroscopy of mixed CO2–CH3OH interstellar ice analogs
Paper

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.

Graphical abstract: Photophysical properties of pyrrolocytosine, a cytosine fluorescent base analogue
Paper

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.

Graphical abstract: Unified reaction pathways for the prebiotic formation of RNA and DNA nucleobases
Paper

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.

Graphical abstract: Internal conversion and intersystem crossing pathways in UV excited, isolated uracils and their implications in prebiotic chemistry
Open Access Paper

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.

Graphical abstract: Probing of molecular replication and accumulation in shallow heat gradients through numerical simulations
Paper

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.

Graphical abstract: The evolution of the surface of the mineral schreibersite in prebiotic chemistry
Open Access Paper

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.

Graphical abstract: The efficiency of driving chemical reactions by a physical non-equilibrium is kinetically controlled
Paper

Non-radiative processes in protonated diazines, pyrimidine bases and an aromatic azine

Protonated diazines have very short excited state lifetimes.

Graphical abstract: Non-radiative processes in protonated diazines, pyrimidine bases and an aromatic azine
Paper

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.

Graphical abstract: Synthesis of barbituric acid containing nucleotides and their implications for the origin of primitive informational polymers
Open Access Paper

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.

Graphical abstract: Lower temperature optimum of a smaller, fragmented triphosphorylation ribozyme
Paper

Possible interstellar formation of glycine through a concerted mechanism: a computational study on the reaction of CH2[double bond, length as m-dash]NH, CO2 and H2

Computational studies on the reaction of CH2[double bond, length as m-dash]NH, CO2 and H2 show the possible interstellar formation of glycine in both hot-cores and cold interstellar clouds.

Graphical abstract: Possible interstellar formation of glycine through a concerted mechanism: a computational study on the reaction of CH2 [[double bond, length as m-dash]] NH, CO2 and H2
24 articles

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.

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