arXiv subjects

C. Walsh

Publications and source records attributed to C. Walsh.

At least 19 recordsLinked to original sources

arXiv2026

Planet formation in chemically diverse and evolving discs II. Chemical fingerprints in planetary atmospheres

Giant planets form in protoplanetary discs, where the coupled dynamical and chemical evolution of gas and solids determines the composition of the material they accrete. We investigate how planet formation and migration shape the primordial elemental makeup of giant-planet atmospheres. Our aim is to link atmospheric compositions to planets' formation pathways and the time-dependent chemical properties of their natal discs. We couple 1D models of viscously evolving discs - incorporating radial dust drift and volatile chemistry - with N-body simulations of planetesimals interacting with a growing and migrating giant planet. Four chemical scenarios and three representative grain sizes (0.1, 20, and 100 micron) are explored. We track the accretion of carbon, oxygen, nitrogen, and sulphur to derive atmospheric elemental ratios normalised to stellar values (* denotes stellar normalisation). We identify three atmospheric classes corresponding to distinct accretion regimes: gas-dominated, characterised by N/O* > C/O* > C/N* and unconstrained or substellar S/N* (near-stellar C/S*); planetesimal-dominated, showing N/O* < C/O* < C/N*, S/N* >= C/N*, and C/S* <= C/O*; and drift-enhanced, exhibiting N/O* < C/O* < C/N* and markedly superstellar volatile-to-refractory ratios. N/O*, C/N*, and S/N* vary systematically with migration extent, although degeneracies arise for planets forming beyond the CO and N2 snowlines; C/O* remains largely insensitive. Metallicity alone does not uniquely trace the solid-to-gas accretion balance in drift-dominated regimes. Variations in the disc's chemical state and dust size imprint distinctive volatile-ratio patterns across these classes, providing complementary constraints on disc properties. This multi-element framework establishes predictive trends to guide the interpretation of atmospheric spectra from facilities like JWST and Ariel.

astro-ph.EP↗

arXiv2025

Dynamics of superconducting pairs in the two-dimensional Hubbard model

The frequency structure of the superconducting correlations in cuprates gives insights on the pairing mechanism. Here we present an exhaustive study of this problem in the two-dimensional Hubbard model with cellular dynamical mean-field theory. To this end, we systematically quantify the dependence on doping $\delta$ and interaction strength $U$ of the superconducting gap, of the frequency scales where $d$-wave pairing occurs, and of their relative contribution to pairing. For all values of $U$ and $\delta$, we find pair-forming processes confined to frequencies set by the superexchange interaction and followed by pair-breaking processes, ruling out both pair-forming and pair-breaking processes on the scale of $U$. This suggests that at high frequencies, the effect of $U$ is eliminated by the $d$-wave paring, and that at small frequencies, $U$ generates the superexchange interaction that leads to low-frequency pair-forming processes providing the net contribution to pairing.

cond-mat.str-el↗

arXiv2025

Molecular Mobility of Extraterrestrial Ices: Surface Diffusion in Astrochemistry and Planetary Science

Molecules are ubiquitous in space. They are necessary component in the creation of habitable planetary systems and can provide the basic building blocks of life. Solid-state processes are pivotal in the formation of molecules in space and surface diffusion in particular is a key driver of chemistry in extraterrestrial environments, such as the massive clouds in which stars and planets are formed and the icy objects within our Solar System. However, for many atoms and molecules quantitative theoretical and experimental information on diffusion, such as activation barriers, are lacking. This hinders us in unraveling chemical processes in space and determining how the chemical ingredients of planets and life are formed. In this article, an astrochemical perspective on diffusion is provided. Described are the relevant adsorbate-surface systems, the methods to model their chemical processes, and the computational and laboratory techniques to determine diffusion parameters, including the latest developments in the field. While much progress has been made, many astrochemically relevant systems remain unexplored. The complexity of ice surfaces, their temperature-dependent restructuring, and effects at low temperatures create unique challenges that demand innovative experimental approaches and theoretical frameworks. This intersection of astrochemistry and surface science offers fertile ground for physical chemists to apply their expertise. We invite the physical chemistry community to explore these systems, where precise diffusion parameters would dramatically advance our understanding of molecular evolution in space - from interstellar clouds to planetary surfaces - with implications on our understanding on the origins of life and planetary habitability.

astro-ph.SR↗

arXiv2025

The Response of Planetary Atmospheres to the Impact of Icy Comets II: exo-Earth Analogues

The orbital regime of a terrestrial planet plays a significant role in shaping its atmospheric dynamics, climate, and hence potential habitability. The orbit is also likely to play a role in shaping the response of a planetary atmosphere to the influx of material from an icy cometary impact. To investigate this response, we model the impact of an icy cometary body with an Earth-analogue exoplanet (i.e. an Earth-like planet orbiting a Sun-like star with a diurnal cycle) using a cometary impact and breakup model coupled with the 3D Earth-System-Model WACCM6/CESM2. To quantify the role that the atmospheric dynamics play in setting the response to a cometary impact, we compare our results with a previous study investigating an impact with a tidally-locked terrestrial exoplanet. We find that the circulation regime of the planet plays a key role in shaping the response of the atmosphere to an icy cometary impact. The weak, multi-celled circulation structure that forms on Earth-like planets is efficient at mixing material horizontally but not vertically, limiting the transport of water from the deep break-up site to higher altitudes. In turn, this limits the rate of water photodissociation at low pressures, reducing the magnitude of post-impact changes to composition. It also reduces the potential observability of an impact due to weakened cloud ice formation, and hence scattering, at low pressures. Despite this, small changes to the overall composition of the planet persist to quasi-steady-state, reinforcing the idea that ongoing bombardment may help to shape the composition/habitability of terrestrial worlds.

astro-ph.EP↗

arXiv2025

Planet formation in chemically diverse and evolving discs -- I. Composition of planetary building blocks

Protoplanetary discs are dynamic environments where the interplay between chemical processes and mass transport shapes the composition of gas and dust available for planet formation. We investigate the combined effects of volatile chemistry - including both gas-phase and surface reactions - viscous gas evolution, and radial dust drift on the composition of planetary building blocks. We explore scenarios of chemical inheritance and reset under varying ionisation conditions and for various dust grain sizes in the sub-mm regime. We simulate disc evolution using a semi-analytical 1D model that integrates chemical kinetics with gas and dust transport, accounting for viscous heating, turbulent mixing, and refractory organic carbon erosion. We find that mass transport plays a role in the chemical evolution of even sub-micron grains, especially in discs that have experienced strong heating or are exposed to relatively high levels of ionising radiation. The radial drift of relatively small icy grains can yield significant volatile enrichment in the gas phase within the snowlines, increasing the abundances of key species by up to an order of magnitude. Early planetesimal formation can lead to volatile depletion in the inner disc on timescales shorter than 0.5 Myr, while the erosion of refractory organic carbon can lead to markedly superstellar gas-phase C/O and C/N ratios. Notably, none of the analysed scenarios reproduce the monotonic radial trend of the gas-phase C/O ratio predicted by early models. Our results also show that a pairwise comparison of elemental ratios, in the context of the host star's composition, is key to isolating signatures of different scenarios in specific regions of the disc. We conclude that models of planet formation must concurrently account for the chemical and dynamical evolution of discs, as well as the diversity of their initial chemical and physical conditions.

astro-ph.EP↗

arXiv2024

How Land-Mass Distribution Influences the Atmospheric Dynamics of Tidally Locked Terrestrial Exoplanets

Interpretation of the ongoing efforts to simulate the atmospheres of potentially-habitable terrestrial exoplanets requires that we understand the underlying dynamics and chemistry of such objects to a much greater degree than 1D or even simple 3D models enable. Here, for the tidally-locked habitable-zone planet TRAPPIST-1e, we explore one effect which can shape the dynamics and chemistry of terrestrial planets: the inclusion of an Earth-like land-ocean distribution with orography. To do this we use the Earth-system model WACCM6/CESM2 to run a pair of TRAPPIST-1e models with N$_2$-O$_2$ atmospheres and with the sub-stellar point fixed over either land or ocean. The presence of orography shapes atmospheric transport, and in the case of Earth-like orography, breaks the symmetry between the northern and southern hemispheres which was previously found in slab ocean models. For example, peak zonal jet speeds in the southern hemisphere are $50\rightarrow100\%$ faster than similar jets in the northern hemisphere. This also affects the meridional circulation, transporting equatorial material towards the south-pole. As a result we also find significant changes in the atmospheric chemistry, including the accumulation of potentially lethal quantities of ozone at both the south pole and the surface. Future studies which investigate the effects of land-mass distribution on the dynamics of exoplanetary atmospheres should pay close attention to both the day-side land-fraction as well as the orography of the land. Simply modelling a flat land-mass will not give a complete picture of its dynamical impact.

astro-ph.EP↗

arXiv2024

Modelling predicts a molecule-rich disk around the AGB star L2 Puppis

The nearby oxygen-rich AGB star L2 Pup hosts a well-studied nearly edge-on disk. To date, disks around AGB stars have not been chemically studied in detail. By combining a parameterisation commonly used for protoplanetary disks and archival ALMA observations, we retrieved an updated density and temperature structure of this disk. This physical model was then used as input to the first chemical model of an AGB disk. The model shows that the physical structure of the disk has a large impact on its chemistry, with certain species showing large changes in column density relative to a radial outflow, indicating that chemistry could be used as a tracer of disks that cannot be directly imaged. Despite its oxygen-rich nature, the daughter species formed within the disk are surprisingly carbon-rich. Two chemical regimes can be distinguished: cosmic-ray induced chemistry in the midplane and photochemistry induced by the interstellar radiation field in the outer regions. Certain complex organic molecules are formed in the midplane. This occurs via gas-phase chemistry only, as the disk is too warm for dust-gas chemistry. The photochemistry in the outer regions leads to the efficient formation of (long) carbon-chains. The predictions of the model allow us to tentatively put the disk's age $\lesssim 10^5$ yr. Additional observations are necessary to better constrain the physical structure of L2 Pup's disk and are essential to test the predictions made by the chemical model. Our exploratory work paves the way for a more general study of the chemistry of AGB disks.

astro-ph.SR↗

arXiv2024

Lethal surface ozone concentrations are possible on habitable zone exoplanets

Ozone ($\textrm{O}_3$) is important for the survival of life on Earth because it shields the surface from ionising ultraviolet (UV) radiation. However, the existence of $\textrm{O}_3$ in Earth's atmosphere is not always beneficial. Resulting from anthropogenic activity, $\textrm{O}_3$ exists as a biologically harmful pollutant at the surface when it forms in the presence of sunlight and other pollutants. As a strong oxidiser, $\textrm{O}_3$ can be lethal to several different organisms; thus, when assessing the potential habitability of an exoplanet, a key part is determining whether toxic gases could be present at its surface. Using the Whole Atmosphere Community Climate Model version 6 (WACCM6; a three-dimensional chemistry-climate model), twelve atmospheric simulations of the terrestrial exoplanet TRAPPIST-1 e are performed with a variety of $\textrm{O}_2$ concentrations and assuming two different stellar spectra proposed in the literature. Four atmospheric simulations of the exoplanet Proxima Centauri b are also included. Some scenarios for both exoplanets exhibit time-averaged surface $\textrm{O}_3$ mixing ratios exceeding harmful levels of 40 ppbv, with 2200 ppbv the maximum concentration found in the cases simulated. These concentrations are toxic and can be fatal to most life on Earth. In other scenarios $\textrm{O}_3$ remains under harmful limits over a significant fraction of the surface, despite there being present regions which may prove inhospitable. In the case that $\textrm{O}_3$ is detected in a terrestrial exoplanet's atmosphere, determining the surface concentration is an important step when evaluating a planet's habitability.

astro-ph.EP↗

arXiv2023

Measurements of Extended Magnetic Fields in Laser-Solid Interaction

Magnetic fields generated from a laser-foil interaction are measured with high fidelity using a proton radiography scheme with in situ x-ray fiducials. In contrast to prior findings under similar experimental conditions, this technique reveals the self-generated, Biermann-battery fields extend beyond the edge of the expanding plasma plume to a radius of over 3.5 mm by t=+1.4 ns, a result not captured in state-of-the-art magneto-hydrodynamics simulations. An analysis of two mono-energetic proton populations confirms that proton deflection is dominated by magnetic fields far from the interaction (>2 mm) and electric fields are insignificant. Comparisons to prior work suggest a new physics mechanism for the magnetic field generation and transport in laser-solid interactions.

physics.plasm-ph↗

arXiv2023

Superconductivity in the two-dimensional Hubbard model with cellular dynamical mean-field theory: a quantum impurity model analysis

Doping a Mott insulator gives rise to unconventional superconducting correlations. Here we address the interplay between d-wave superconductivity and Mott physics using the two-dimensional Hubbard model with cellular dynamical mean-field theory on a $2\times2$ plaquette. Our approach is to study superconducting correlations from the perspective of a cluster quantum impurity model embedded in a self-consistent bath. At the level of the cluster, we calculate the probabilities of the possible cluster electrons configurations. Upon condensation we find an increased probability that cluster electrons occupy a four-electron singlet configuration, enabling us to identify this type of short-range spin correlations as key to superconducting pairing. The increased probability of this four-electron singlet comes at the expense of a reduced probability of a four-electron triplet with no significant probability redistribution of fluctuations of charges. This allows us to establish that superconductivity at the level of the cluster primarily involves a reorganisation of short-range spin correlations rather than charge correlations. We gain information about the bath by studying the spectral weight of the hybridization function. Upon condensation, we find a transfer of spectral weight leading to the opening of a superconducting gap. We use these insights to interpret the signatures of superconducting correlations in the density of states of the system and in the zero-frequency spin susceptibility.

cond-mat.str-el↗

arXiv2022

Prediction of anomalies in the velocity of sound for the pseudogap of hole-doped cuprates

We predict sound anomalies at the doping $\delta_{p}$ where the pseudogap ends in the normal state of hole-doped cuprates. Our prediction is based on the two-dimensional compressible Hubbard model using cluster dynamical mean-field theory. We find sharp anomalies (dips) in the velocity of sound as a function of doping and interaction. These dips are a signature of supercritical phenomena, stemming from an electronic transition without symmetry breaking below the superconducting dome. If experimentally verified, these signatures may help to solve the fundamental question of the nature of the pseudogap -- pinpointing its origin as due to Mott physics and resulting short-range correlations.

cond-mat.str-el↗

arXiv2022

Surface astrochemistry: a computational chemistry perspective

Molecules in space are synthesized via a large variety of gas-phase reactions, and reactions on dust-grain surfaces, where the surface acts as a catalyst. Especially, saturated, hydrogen-rich molecules are formed through surface chemistry. Astrochemical models have developed over the decades to understand the molecular processes in the interstellar medium, taking into account grain surface chemistry. However, essential input information for gas-grain models, such as binding energies of molecules to the surface, have been derived experimentally only for a handful of species, leaving hundreds of species with highly uncertain estimates. Moreover, some fundamental processes are not well enough constrained to implement these into the models. The proceedings gives three examples how computational chemistry techniques can help answer fundamental questions regarding grain surface chemistry.

astro-ph.GA↗

arXiv2021

Information-theoretic measures of superconductivity in a two-dimensional doped Mott insulator

A key open issue in condensed matter physics is how quantum and classical correlations emerge in an unconventional superconductor from the underlying normal state. We study this problem in a doped Mott insulator with information theory tools on the two-dimensional Hubbard model at finite temperature with cluster dynamical mean-field theory. We find that the local entropy detects the superconducting state and that the difference in the local entropy between the superconducting and normal states follows the same difference in the potential energy. We find that the thermodynamic entropy is suppressed in the superconducting state and monotonically decreases with decreasing doping. The maximum in entropy found in the normal state above the overdoped region of the superconducting dome is obliterated by superconductivity. The total mutual information, which quantifies quantum and classical correlations, is amplified in the superconducting state of the doped Mott insulator for all doping levels, and shows a broad peak versus doping, as a result of competing quantum and classical effects.

cond-mat.str-el↗

arXiv2020

Chemical modelling of dust-gas chemistry within AGB outflows III. Photoprocessing of the ice and return to the ISM

To explain the properties of dust in the interstellar medium (ISM), the presence of a refractory organic mantle is necessary. The outflows of AGB stars are among the main contributors of stellar dust to the ISM. We present the first study of the refractory organic contribution of AGB stars to the ISM. Based on laboratory experiments, we included a new reaction in our extended chemical kinetics model: the photoprocessing of volatile complex ices into inert refractory organic material. The refractory organic feedback of AGB outflows to the ISM is estimated using observationally motivated parent species and grids of models of C-rich and O-rich outflows. Refractory organic material is mainly inherited from the gas phase through accretion onto the dust and subsequent photoprocessing. Grain-surface chemistry, initiated by photodissociation of ices, produces only a minor part and takes place in a sub-monolayer regime in almost all outflows. The formation of refractory organic material increases with outflow density and depends on the initial gas-phase composition. While O-rich dust is negligibly covered by refractory organics, C-rich dust has an average coverage of $3-9\%$, but can be as high as $8-22\%$. Although C-rich dust does not enter the ISM bare, its average coverage is too low to influence its evolution in the ISM or significantly contribute to the coverage of interstellar dust. This study opens up questions on the coverage of other dust-producing environments. It highlights the need for an improved understanding of dust formation and for models specific to density structures within the outflow.

astro-ph.SR↗

arXiv2020

Entanglement and classical correlations at the doping-driven Mott transition in the two-dimensional Hubbard model

Tools of quantum information theory offer a new perspective to characterize phases and phase transitions in interacting many-body quantum systems. The Hubbard model is the archetypal model of such systems and can explain rich phenomena of quantum matter with minimal assumptions. Recent measurements of entanglement-related properties of this model using ultracold atoms in optical lattices hint that entanglement could provide the key to understanding open questions of the doped Hubbard model, including the remarkable properties of the pseudogap phase. These experimental findings call for a theoretical framework and new predictions. Here we approach the doped Hubbard model in two dimensions from the perspective of quantum information theory. We study the local entropy and the total mutual information across the doping-driven Mott transition within plaquette cellular dynamical mean-field theory. We find that upon varying doping these two entanglement-related properties detect the Mott insulating phase, the strongly correlated pseudogap phase, and the metallic phase. Imprinted in the entanglement-related properties we also find the pseudogap to correlated metal first-order transition, its finite temperature critical endpoint, and its supercritical crossovers. Through this footprint we reveal an unexpected interplay of quantum and classical correlations. Our work shows that sharp variation in the entanglement-related properties and not broken symmetry phases characterizes the onset of the pseudogap phase at finite temperature.

cond-mat.str-el↗

arXiv2020

Chemical modelling of dust-gas chemistry within AGB outflows -- II. Effect of the dust-grain size distribution

AGB stars are, together with supernovae, the main contributors of stellar dust to the interstellar medium (ISM). Dust grains formed by AGB stars are thought to be large. However, as dust nucleation and growth within their outflows are still not understood, the dust-grain size distribution (GSD) is unknown. This is an important uncertainty regarding our knowledge of the chemical and physical history of interstellar dust, as AGB dust forms $\sim$ 70% of the starting point of its evolution. We expand on our chemical kinetics model, which uniquely includes a comprehensive dust-gas chemistry. The GSD is now allowed to deviate from the commonly assumed canonical Mathis et al. (1977) distribution. We find that the specific GSD can significantly influence the dust-gas chemistry within the outflow. Our results show that the level of depletion of gas-phase species depends on the average grain surface area of the GSD. Gas-phase abundance profiles and their possible depletions can be retrieved from observations of molecular emission lines when using a range of transitions. Due to degeneracies within the prescription of GSD, specific parameters cannot be retrieved, only (a lower limit to) the average grain surface area. Nonetheless, this can discriminate between dust composed of predominantly large or small grains. We show that when combined with other observables such as the spectral energy distribution and polarised light, depletion levels from molecular gas-phase abundance profiles can constrain the elusive GSD of the dust delivered to the ISM by AGB outflows.

astro-ph.SR↗

arXiv2019

Dust-gas chemistry in AGB outflows: Chemical modelling of dust-gas chemistry within AGB outflows I. Effect on the gas-phase chemistry

Chemical modelling of AGB outflows is typically focused on either non-thermodynamic equilibrium chemistry in the inner region or photon-driven chemistry in the outer region. We include, for the first time, a comprehensive dust-gas chemistry in our AGB outflow chemical kinetics model, including both dust-gas interactions and grain-surface chemistry. The dust is assumed to have formed in the inner region, and follows an interstellar-like dust-size distribution. Using radiative transfer modelling, we obtain dust temperature profiles for different dust types in an O-rich and a C-rich outflow. We calculate a grid of models, sampling different outflow densities, drift velocities between the dust and gas, and dust types. Dust-gas chemistry can significantly affect the gas-phase composition, depleting parent and daughter species and increasing the abundance of certain daughter species via grain-surface formation followed by desorption/sputtering. Its influence depends on four factors: outflow density, dust temperature, initial composition, and drift velocity. The largest effects are for higher density outflows with cold dust and O-rich parent species, as these species generally have a larger binding energy. At drift velocities larger than $\sim 10$ km s$^{-1}$, ice mantles undergo sputtering; however, they are not fully destroyed. Models with dust-gas chemistry can better reproduce the observed depletion of species in O-rich outflows. When including colder dust in the C-rich outflows and adjusting the binding energy of CS, the depletion in C-rich outflows is also better reproduced. To best interpret high-resolution molecular line observations from AGB outflows, dust-gas interactions are needed in chemical kinetics models.

astro-ph.SR↗

arXiv2019

VLA cm-wave survey of young stellar objects in the Oph A cluster: constraining extreme UV- and X-ray-driven disk photo-evaporation -- A pathfinder for Square Kilometre Array studies

Observations of young stellar objects (YSOs) in centimeter bands can probe the continuum emission from growing dust grains, ionized winds, and magnetospheric activity, which are intimately connected to the evolution of protoplanetary disks and the formation of planets. We have carried out sensitive continuum observations toward the Ophiuchus A star-forming region using the Karl G. Jansky Very Large Array (VLA) at 10 GHz over a field-of-view of 6$'$ with a spatial resolution of $\theta_{maj}$ $\times$ $\theta_{min}$ $\sim$ 0.4$''$ $\times$ 0.2$''$. We achieved a 5 $\mu$Jy beam$^{-1}$ root-mean-square noise level at the center of our mosaic field of view. Among the eighteen sources we detected, sixteen are YSOs (three Class 0, five Class I, six Class II, and two Class III) and two are extragalactic candidates. We find that thermal dust emission generally contributes less that 30% of the emission at 10 GHz. The radio emission is dominated by other types of emission such as gyro-synchrotron radiation from active magnetospheres, free-free emission from thermal jets, free-free emission from the outflowing photo-evaporated disk material, and/or synchrotron emission from accelerated cosmic-rays in jet or protostellar surface shocks. These different types of emission could not be clearly disentangled. Our non-detections towards Class II/III disks suggest that extreme UV-driven photoevaporation is insufficient to explain the disk dispersal, assuming that the contribution of UV photoevaporating stellar winds to radio flux does not evolve with time. The sensitivity of our data cannot exclude photoevaporation due to X-ray photons as an efficient mechanism for disk dispersal. Deeper surveys with the Square Kilometre Array will be able to provide strong constraints on disk photoevaporation.

astro-ph.SR↗