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Nigel J. Mason

Publications and source records attributed to Nigel J. Mason.

At least 19 recordsLinked to original sources

An interstellar energetic and non-aqueous pathway to peptide formation

The origin of the molecular building blocks of life is a central question in science. A few $\alpha$-amino acids such as glycine, the simplest proteinogenic amino acid, have been detected in meteorites and comets, indicating an extraterrestrial origin for some prebiotic molecules. However, the formation of peptides, short chains of $\alpha$-amino acids linked by peptide bonds, under astrophysical conditions has remained unresolved. Here we show that the building blocks of proteins can form in interstellar ice analogues exposed to ionising radiation, without the presence of liquid water. Using isotopically labelled glycine irradiated with protons at cryogenic temperatures, we detect the formation of glycylglycine, the simplest dipeptide, along with deuterated and non-deuterated water as by-products. Peptide bond formation is confirmed by infrared spectroscopy and high-resolution mass spectrometry, which also reveal the production of other complex organic species. These findings demonstrate a non-aqueous route to peptide formation under space-like conditions and suggest that such molecules could form in the cold interstellar medium and be incorporated into forming planetary systems. Our results challenge aqueous-centric models of early biochemical evolution and broaden potential settings for the origins of life.

astro-ph.SR

Influence of DFT Functionals on Low-Energy Electron Scattering Cross Sections of Nitric Oxide

Nitric oxide (NO) is important in biological, atmospheric, plasma, industrial, and astrophysical environments, where reliable electron-collision data support modelling charged-particle interactions with matter. Its well-known experimental properties make it suitable for assessing how the target electronic-structure description affects low-energy electron scattering calculations. In this work, NO properties were evaluated using B3LYP, M06-2X, PBE0, and $\omega$B97X-D3, with basis sets ranging from minimal to quadruple-zeta quality. Bond length, dipole moment, ionisation potential, and polarisability were compared with experiment to assess the sensitivity of the target description to the functional and basis set. The aug-cc-pVQZ basis set was then used to generate target models for ab initio R-matrix calculations over 0.1--20 eV. The total cross sections show low-energy resonance features, with the strongest functional dependence around the broad peak near 0.8--1.0 eV. A sharper, higher-energy structure is also observed below 2 eV, shifting from 1.74 to 1.82 eV depending on the functional. Differential cross sections show modest functional sensitivity, with more noticeable angular differences at 7.5 and 10 eV. These results show that the DFT functional and basis set affect the target properties, with the resulting target description influencing low-energy electron-scattering observables of NO. The comparison supports $\omega$B97X-D3/aug-cc-pVTZ geometry optimisation followed by aug-cc-pVQZ target-property calculations as a practical protocol for R-matrix modelling of NO.

physics.atm-clus

Prospects for Astrobiology and Technosignature Searches with the Vera C. Rubin Observatory Legacy Survey of Space and Time

The Vera C. Rubin Observatory Legacy Survey of Space and Time (LSST) will map sources in multiband colour--variability space. We present a prototype coherence-based framework for astrobiology and technosignature searches, in which candidates are treated as structured departures from natural astrophysical manifolds rather than isolated photometric outliers. We illustrate the framework with three simulated cases: five Kuiper Belt Object (KBO) surface/activity states, a grid of 649 synthetic exoplanet spectra with vegetation-red-edge-like (VRE) perturbations, and 500 synthetic multiband light curves, each projected into LSST-like observable space and analysed through colour geometry, chromatic variability, and cross-band coherence. Key results include a full-colour Mahalanobis distance $D\approx5.1$ for the weak-coma KBO state (${\sim}5\sigma$ in the five-dimensional colour vector), an indicative VRE coherence threshold at $f_{\rm crit}\approx0.13$, and an idealised stacking forecast reaching $5\sigma$ under optimistic assumptions. We show, using a small Gaia~DR3 stellar sample, that stellar colour and photometric stability may inform the prioritisation of Galactic regions for applying such coherence diagnostics.

astro-ph.IM

Structural effects of boron doping in diamond crystals for gamma-ray light-source applications: Insights from molecular dynamics simulations

Boron-doped diamond crystals (BDD, C$_{1-x}$B$_{x}$) exhibit exceptional mechanical strength, electronic tunability, and resistance to radiation damage. This makes them promising materials for use in gamma-ray crystal-based light sources. To better understand and quantify the structural distortions introduced by doping, which are critical for maintaining channelling efficiency, we perform atomistic-level molecular dynamics simulations on periodic C$_{1-x}$B$_{x}$ systems of various sizes. These simulations allow the influence of boron concentration on the lattice constant and the (110) and (100) inter-planar distances to be evaluated over the concentration range from pure diamond (0%) to 5% boron at room temperature (300 K). Linear relationships between both lattice constant and inter-planar distance with increasing dopant concentration are observed, with a deviation from Vegard's Law. This deviation is larger than that reported by other theoretical and computational studies; however, this may be attributed to an enhanced crystal quality over these studies, a vital aspect when considering gamma-ray crystal light source design. The methodology presented here incorporates several refinements to closely reflect the conditions of microwave plasma chemical vapour deposition (MPCVD) crystal growth. Validation of the methodology is provided through a comprehensive statistical analysis of the structure of our generated crystals. These results enable reliable atomistic modelling of doped diamond crystals and support their use in the design and fabrication of periodically bent structures for next-generation gamma-ray light source technologies.

cond-mat.mtrl-sci

Influence of bending parameters on crystalline undulator radiation peak stability for 530 MeV positron channelling

We investigate the stability of crystalline undulator radiation (CUR) peaks emitted by 530 MeV positron channelling in periodically bent C(110) crystals with varying bending amplitudes and bending periods. Relativistic molecular dynamics simulations were performed to quantify how these parameters affect the intensity and position of the CUR peak. The continuous potential approximation was used to identify isolines of constant peak energy, providing a reference for regions of spectral stability. MD results show that increasing the bending amplitude shifts the CUR peak to lower photon energies, while decreasing the period shifts it to higher energies, with both trends accompanied by enhanced dechannelling. For crystal parameters similar to recent experiments conducted at the MAinz MIkrotron (MAMI), the simulated CUR peak appears near 0.515 MeV. These results demonstrate that the CUR peak remains stable across a broad range of bending amplitudes and periods, providing quantitative estimates of the sensitivity of the emitted radiation to variations in the crystal bending parameters.

physics.acc-ph

Electron Irradiation of Crystalline Nitrous Oxide Ice at Low Temperatures: Applications to Outer Solar System Planetary Science

The radiation chemistry and physics of solid N2O have been increasingly studied due to its potential presence on the surfaces of cold, outer Solar System bodies. However, to date, no study has investigated systematically the influence of temperature on this chemistry and physics. In this present study, crystalline N2O ices were irradiated using 2 keV electrons at five different temperatures in the 20-60 K range and the radiolytic dissociation of the molecular solid (as well as the radiolytic formation of seven product molecules) was quantified through the G-value. Our results indicate that temperature does indeed play a role in the radiolytic destruction of crystalline N2O, with higher temperatures being associated with higher destruction G-values. The formation G-values of NO, NO2, N2O2, N2O3, N2O4, N2O5, and O3 were also noted to vary with temperature, with each product molecule exhibiting a distinct trend. The applications of our experimental results to further understanding solid-phase radiation chemistry in the outer Solar System are discussed.

cond-mat.mtrl-sci

Dopant concentration effects on Si$_{1-x}$Ge$_{x}$ crystals for emerging light-source technologies: A molecular dynamics study

In this study, we conduct atomistic-level molecular dynamics simulations on fixed-sized silicon-germanium (Si$_{1-x}$Ge$_{x}$) crystals to elucidate the effects of dopant concentration and temperature on the crystalline inter-planar distances. Our calculations consider a range of Ge dopant concentrations between pure Si (0%) and 15%, and for both the optimised system state and a temperature of 300 K. We observe a linear relationship between Ge concentration and inter-planar distance and lattice constant, in line with the approximation of Vegard's Law, and other experimental and computational results. These findings will be employed in conjunction with future studies to establish precise tolerances for use in crystal growth, crucial for the manufacture of crystals intended for emerging gamma-ray crystal-based light source technologies.

physics.atom-ph

Condensed Matter Systems Exposed to Radiation: Multiscale Theory, Simulations, and Experiment

This paper reviews the new highly interdisciplinary research field studying the behavior of condensed matter systems exposed to radiation. The paper highlights several relevant examples of recent advances in the field and provides a roadmap for the development of the field in the next decade. Condensed matter systems exposed to radiation may have very different natures, being inorganic, organic or biological, finite or infinite, be composed of many different molecular species or materials, existing in different phases (solid, liquid, gaseous or plasma) and operating under different thermodynamic conditions. The essential and novel element of this research is that, despite the vast diversity of such systems, many of the key phenomena related to the behavior of irradiated systems (such as radiation-induced damage, mechanisms of damage repair and control, radiation protection, etc.) are very similar and can be understood based on the same fundamental theoretical principles and computational approaches. One of the essential features of the aforementioned phenomena concerns their multiscale nature as the manifestation of the radiation-induced effects occurring at different spatial and temporal scales ranging from the atomic to the macroscopic. The multiscale nature of the effects and similarity of their manifestation in systems of different origins necessarily brings together different disciplines, such as physics, chemistry, biology, materials and nano-science, and biomedical research, demonstrating numerous interlinks and commonalities between them. This research field is highly relevant to many novel and emerging technologies and medical applications.

physics.chem-ph

Topical Issue "Dynamics of Systems on the Nanoscale (2021)". Editorial

Exploration of the structure formation and dynamics of animate and inanimate matter on the nanometer scale is a highly interdisciplinary field of rapidly emerging research. It is relevant for various molecular and nanoscale systems of different origins and compositions and concerns numerous phenomena originating from physics, chemistry, biology, and materials science. This topical issue presents a collection of research papers devoted to different aspects of the Dynamics of Systems on the Nanoscale. Some of the contributions discuss specific applications of the research results in several modern and emerging technologies, such as controlled nanofabrication with charged particle beams or the design and practical realization of novel gamma-ray crystal-based light sources. Most works presented in this topical issue were reported at the joint Sixth International Conference "Dynamics of Systems on the Nanoscale" and the tenth International Symposium "Atomic Cluster Collisions" (DySoN-ISACC 2021), which were held in Santa Margherita Ligure, Italy, in October 2021.

physics.chem-ph

Atomistic modelling and structural characterisation of coated gold nanoparticles for biomedical applications

This study presents the results of atomistic structural characterisation of 3.7 nm diameter gold nanoparticles (NP) coated with polymer polyethylene glycol (PEG)-based ligands of different lengths (containing $2-14$ monomers) and solvated in water. The system size and composition are selected in connection to several experimental studies of radiosensitisation mechanisms of gold NPs. The coating structure and water distribution near the NP surface are characterised on the atomistic level by means of molecular dynamics simulations. The results of simulations carried out in this study, combined with the results of our recent study [J. Phys. Chem. A 126 (2022) 2170] and those from the field of polymer physics, are used to calculate key structural parameters of the coatings of radiosensitising gold NPs. On this basis, connections between the coating structure and distribution of water are established for different NP sizes as well as lengths and surface densities of coating molecules. The quantitative analysis of water distribution in the vicinity of coated metal NPs can be used to evaluate the radiosensitising effectiveness of a particular NP system based on the proximity of water to the NP metal core, which should impact the production of hydroxyl radicals and reactive oxygen species in the vicinity of metal NPs exposed to ionising radiation.

physics.atm-clus

Bombardment of CO ice by cosmic rays: I. Experimental insights into the microphysics of molecule destruction and sputtering

We present a dedicated experimental study of microscopic mechanisms controlling radiolysis and sputtering of astrophysical ices due to their bombardment by cosmic ray ions. Such ions are slowed down due to inelastic collisions with bound electrons, resulting in ionization and excitation of ice molecules. In experiments on CO ice irradiation, we show that the relative contribution of these two mechanisms of energy loss to molecule destruction and sputtering can be probed by selecting ion energies near the peak of the electronic stopping power. We have observed a significant asymmetry, both in the destruction cross section and the sputtering yield, for pairs of ion energies corresponding to same values of the stopping power on either side of the peak. This implies that the stopping power does not solely control these processes, as usually assumed in the literature. Our results suggest that electronic excitations represent a significantly more efficient channel for radiolysis and, possibly, also for sputtering of CO ice. We also show that the charge state of incident ions as well as the rate for CO$^+$ production in the ice have negligible effect on these processes.

astro-ph.IM

Proton and electron irradiations of CH4:H2O mixed ices

The organic chemistry occurring in interstellar environments may lead to the production of complex molecules that are relevant to the emergence of life. Therefore, in order to understand the origins of life itself, it is necessary to probe the chemistry of carbon-bearing molecules under conditions that simulate interstellar space. Several of these regions, such as dense molecular cores, are exposed to ionizing radiation in the form of galactic cosmic rays, which may act as an important driver of molecular destruction and synthesis. In this paper, we report the results of a comparative and systematic study of the irradiation of CH4:H2O ice mixtures by 1 MeV protons and 2 keV electrons at 20 K.We demonstrate that our irradiations result in the formation of a number of new products, including both simple and complex daughter molecules such as C2H6, C3H8, C2H2, CH3OH, CO, CO2, and probably also H2CO. A comparison of the different irradiation regimes has also revealed that proton irradiation resulted in a greater abundance of radiolytic daughter molecules compared to electron irradiation, despite a lower radiation dose having been administered. These results are important in the context of the radiation astrochemistry occurring within the molecular cores of dense interstellar clouds, as well as on outer Solar System objects.

astro-ph.GA

Energetic Electron Irradiations of Amorphous and Crystalline Sulphur-Bearing Astrochemical Ices

Laboratory experiments have confirmed that the radiolytic decay rate of astrochemical ice analogues is dependent upon the solid phase of the target ice, with some crystalline molecular ices being more radio-resistant than their amorphous counterparts. The degree of radio-resistance exhibited by crystalline ice phases is dependent upon the nature, strength, and extent of the intermolecular interactions that characterise their solid structure. For example, it has been shown that crystalline CH3OH decays at a significantly slower rate when irradiated by 2 keV electrons at 20 K than does the amorphous phase due to the stabilising effect imparted by the presence of an extensive array of strong hydrogen bonds. These results have important consequences for the astrochemistry of interstellar ices and outer Solar System bodies, as they imply that the chemical products arising from the irradiation of amorphous ices (which may include prebiotic molecules relevant to biology) should be more abundant than those arising from similar irradiations of crystalline phases. In this present study, we have extended our work on this subject by performing comparative energetic electron irradiations of the amorphous and crystalline phases of the sulphur-bearing molecules H2S and SO2 at 20 K. We have found evidence for phase-dependent chemistry in both these species, with the radiation-induced exponential decay of amorphous H2S being more rapid than that of the crystalline phase, similar to the effect that has been previously observed for CH3OH. For SO2, two fluence regimes are apparent: a low-fluence regime in which the crystalline ice exhibits a rapid exponential decay while the amorphous ice possibly resists decay, and a high-fluence regime in which both phases undergo slow exponential-like decays.

physics.chem-ph

Ozone Production in Electron Irradiated CO2:O2 Ices

The detection of ozone (O3) in the surface ices of Ganymede, Jupiters largest moon, and of the Saturnian moons Rhea and Dione, has motivated several studies on the route of formation of this species. Previous studies have successfully quantified trends in the production of O3 as a result of the irradiation of pure molecular ices using ultraviolet photons and charged particles (i.e., ions and electrons), such as the abundances of O3 formed after irradiation at different temperatures or using different charged particles. In this study, we extend such results by quantifying the abundance of O3 as a result of the 1 keV electron irradiation of a series of 14 stoichiometrically distinct CO2:O2 astrophysical ice analogues at 20 K. By using mid-infrared spectroscopy as our primary analytical tool, we have also been able to perform a spectral analysis of the asymmetric stretching mode of solid O3 and the variation in its observed shape and profile among the investigated ice mixtures. Our results are important in the context of better understanding the surface composition and chemistry of icy outer Solar System objects, and may thus be of use to future interplanetary space missions such as the ESA Jupiter Icy Moons Explorer and the NASA Europa Clipper missions, as well as the recently launched NASA James Webb Space Telescope.

astro-ph.EP

Laboratory Experiments on the Radiation Astrochemistry of Water Ice Phases

Water (H2O) ice is ubiquitous component of the universe, having been detected in a variety of interstellar and Solar System environments where radiation plays an important role in its physico-chemical transformations. Although the radiation chemistry of H2O astrophysical ice analogues has been well studied, direct and systematic comparisons of different solid phases are scarce and are typically limited to just two phases. In this article, we describe the results of an in-depth study of the 2 keV electron irradiation of amorphous solid water (ASW), restrained amorphous ice (RAI) and the cubic (Ic) and hexagonal (Ih) crystalline phases at 20 K so as to further uncover any potential dependence of the radiation physics and chemistry on the solid phase of the ice. Mid-infrared spectroscopic analysis of the four investigated H2O ice phases revealed that electron irradiation of the RAI, Ic, and Ih phases resulted in their amorphization (with the latter undergoing the process more slowly) while ASW underwent compaction. The abundance of hydrogen peroxide (H2O2) produced as a result of the irradiation was also found to vary between phases, with yields being highest in irradiated ASW. This observation is the cumulative result of several factors including the increased porosity and quantity of lattice defects in ASW, as well as its less extensive hydrogen-bonding network. Our results have astrophysical implications, particularly with regards to H2O-rich icy interstellar and Solar System bodies exposed to both radiation fields and temperature gradients.

astro-ph.GA

2022 Review of Data-Driven Plasma Science

Data science and technology offer transformative tools and methods to science. This review article highlights latest development and progress in the interdisciplinary field of data-driven plasma science (DDPS). A large amount of data and machine learning algorithms go hand in hand. Most plasma data, whether experimental, observational or computational, are generated or collected by machines today. It is now becoming impractical for humans to analyze all the data manually. Therefore, it is imperative to train machines to analyze and interpret (eventually) such data as intelligently as humans but far more efficiently in quantity. Despite the recent impressive progress in applications of data science to plasma science and technology, the emerging field of DDPS is still in its infancy. Fueled by some of the most challenging problems such as fusion energy, plasma processing of materials, and fundamental understanding of the universe through observable plasma phenomena, it is expected that DDPS continues to benefit significantly from the interdisciplinary marriage between plasma science and data science into the foreseeable future.

physics.plasm-ph

Comparative Electron Irradiations of Amorphous and Crystalline Astrophysical Ice Analogues

Laboratory studies of the radiation chemistry occurring in astrophysical ices have demonstrated the dependence of this chemistry on a number of experimental parameters. One experimental parameter which has received significantly less attention is that of the phase of the solid ice under investigation. In this present study, we have performed systematic 2 keV electron irradiations of the amorphous and crystalline phases of pure CH3OH and N2O astrophysical ice analogues. Radiation-induced decay of these ices and the concomitant formation of products were monitored in situ using FT-IR spectroscopy. A direct comparison between the irradiated amorphous and crystalline CH3OH ices revealed a more rapid decay of the former compared to the latter. Interestingly, a significantly lesser difference was observed when comparing the decay rates of the amorphous and crystalline N2O ices. These observations have been rationalised in terms of the strength and extent of the intermolecular forces present in each ice. The strong and extensive hydrogen-bonding network that exists in crystalline CH3OH (but not in the amorphous phase) is suggested to significantly stabilise this phase against radiation-induced decay. Conversely, although alignment of the dipole moment of N2O is anticipated to be more extensive in the crystalline structure, its weak attractive potential does not significantly stabilise the crystalline phase against radiation-induced decay, hence explaining the smaller difference in decay rates between the amorphous and crystalline phases of N2O compared to those of CH3OH. Our results are relevant to the astrochemistry of interstellar ices and icy Solar System objects, which may experience phase changes due to thermally-induced crystallisation or space radiation-induced amorphisation.

astro-ph.GA

Molecular dynamics characterisation of radiosensitising coated gold nanoparticles in aqueous environment

Functionalized metal nanoparticles (NPs) have been proposed as promising radiosensitizing agents for more efficient radiotherapy treatment using photons and ion beams. Radiosensitizing properties of NPs may depend on many different parameters (such as size, composition and density) of the metal core, organic coatings and the molecular environment. A systematic exploration of each of these parameters on the atomistic level remains a costly experimental task but it can be addressed by means of advanced computational modeling. This paper outlines a detailed computational procedure for the construction and atomistic-level characterization of radiosensitizing metal NPs in explicit molecular media. The procedure is general and extensible to many different combinations of the core, coating and environment. As an illustrative and experimentally relevant case study, we consider nanometre-sized gold NPs coated with thiol-poly(ethylene glycol)-amine molecules of different length and surface density and solvated in water at ambient conditions. Radial distribution of different atoms in the coatings as well as distribution and structural properties of water around the coated NPs are analyzed and linked to radiosensitizing properties of the NPs. It is revealed that the structure of the coating layer on the solvated NPs depends strongly on the surface density of ligands. At surface densities below $\sim$3 molecules/nm$^{2}$ the coating represents a mixture of different conformation states, whereas elongated "brush"-like structures are formed at higher densities of ligands. The water content in denser coatings is significantly lower at distances from 1 to 3 nm from the gold surface depending on the length of ligands. Such dense and thick coatings may suppress the production of hydroxyl radicals by low-energy electrons emitted from the metal NPs and thus diminish their radiosensitizing properties.

physics.atm-clus