arXiv subjects

Graeme J Ackland

Publications and source records attributed to Graeme J Ackland.

At least 19 recordsLinked to original sources

arXiv2026

Phase Stability and Anisotropic Superconductivity in Ternary M2B4C2 (M=Ca, Mg) Monolayer

In this work, we investigate the phase stability, electronic structure, and superconducting properties of the two-dimensional ternary borocarbides MB$_4$C$_2$ (M = Ca, Mg) using first-principles calculations and fully anisotropic Migdal-Eliashberg theory. Ab initio molecular dynamics, phonon dispersion, and elastic constant calculations confirm that both monolayers are dynamically, thermally, and mechanically stable. Electronic structure analysis reveals an intrinsic metallic nature with a multiband Fermi surface, where states near the $Γ$ point are dominated by in-plane B-$p_x$, $p_y$ orbitals, while zone-boundary states are primarily derived from out-of-plane B-$p_z$ orbitals. The electron-phonon coupling is determined to be $λ= 0.64$ for both materials, driven by the rigid covalent B-B and B-C honeycomb networks. By solving the anisotropic Eliashberg equations, we predict that CaB$_4$C$_2$ and MgB$_4$C$_2$ are nodeless two-gap superconductors with critical temperatures ($T_c$) of 33.4 K and 33.8 K, respectively, at a Coulomb pseudopotential of $μ= 0.10$. Furthermore, the superconducting state remains robust under increased Coulomb repulsion ($μ= 0.13$), retaining elevated $T_c$ values of 31.2 K and 30.9 K, respectively. These findings establish MB$_4$C$_2$ monolayers as promising candidates for nanoscale superconducting applications and enrich the family of two-dimensional multigap superconductors.

cond-mat.supr-con↗

arXiv2026

Noble-Gas Solubility in Solid and Fluid Metallic Hydrogen

Metallic hydrogen dominates the deep interiors of giant planets, where trace elements interact with dense quantum matter under extreme pressure. We investigate the thermodynamic stability of noble-gas impurities (He, Ne, Ar, Kr, Xe) in metallic hydrogen at 500 GPa using ab initio molecular dynamics combined with first-principles free-energy calculations. In the solid metallic phase, all noble gases exhibit positive formation free energies, driven by unfavorable electronic enthalpy and zero-point vibrational contributions. By contrast, heavier noble gases (Ar, Kr, Xe) appear soluble in liquid hydrogen, while He and Ne phase separate. This crossover reflects a competition between electronic repulsion and disorder-driven stabilization intrinsic to the liquid phase. Our results reveal noble-gas retention in metallic hydrogen, providing a microscopic mechanism for noble-gas fractionation in giant-planet interiors.

cond-mat.mtrl-sci↗

arXiv2026

Competition between Charge Density Wave and Superconductivity in a Janus MXene Mo2NF2

Charge-density-wave (CDW) order and superconductivity often compete in low-dimensional materials, yet their interplay in Janus MXenes remains largely unexplored. Here, we present a comprehensive first-principles investigation of the structural, vibrational, and electronic properties of Mo2NF2. Phonon calculations reveal an unstable soft phonon mode at the M point in the high-symmetry structure, signaling a CDW instability. Analysis of phonon linewidths and the real and imaginary parts of the bare electronic susceptibility demonstrates that the CDW is not driven by simple Fermi-surface nesting but instead originates from strong momentum-dependent electron-phonon coupling. Structural relaxation yields a commensurate CDW phase characterized by bond-length modulations involving the Mo, N, and F sublattices. We further show that charge doping alone is insufficient to stabilize the soft phonon, whereas compressive biaxial strain exceeding -3 percent completely suppresses the CDW instability. Electron-phonon coupling calculations indicate that the CDW phase exhibits a reduced coupling constant lambda = 0.40 and logarithmic phonon frequency omega_log = 219 K, leading to a low superconducting transition temperature Tc about 1 K. In contrast, the strain-stabilized high-symmetry phase shows enhanced coupling (lambda = 0.53, omega_log = 272 K) and a higher Tc about 4 K. Our results establish Mo2NF2 as a strain-tunable platform where superconductivity emerges upon suppression of a competing CDW phase, highlighting the crucial role of lattice control in Janus MXenes.

cond-mat.supr-con↗

arXiv2026

Frustrated supermolecules: the high-pressure phases of crystalline methane

Methane is the simplest hydrocarbon, yet it exhibits an extraordinarily complicated series of crystal phases. Notably, the non-plastic phases have large unit cells with nearly, but not quite cubic symmetry. Furthermore, although non-polar molecules interact very weakly, their reorganisation across phase transitions is very sluggish. Here, we demonstrate that these complex structures can be understood as simple packing of near-spherical supermolecular clusters of methane molecules: the departure from cubic symmetry arising from the non-spherical nature of the molecules. We use molecular dynamics based on density functional theory calculations to simulate the finite-temperature crystal structures of methane, finding that the complex Phase A is based around a 13-molecule regular icosahedron, with 8 additional molecules forming the 21-molecule unit cell. Similarly, Phase B is based on a body-centred cubic bcc packing of 17-molecule Z16 polyhedra, with the remaining 12 molecules per cell in tetrahedral interstices. We demonstrate that the favored intermolecular separation depends sensitively on molecular orientation, leading to hindered rotation and suppressed entropy. The structures are determined by a trade-off between efficient packing and entropy.

physics.comp-ph↗

arXiv2026

Charge Density Wave Order and Superconductivity in Janus MoXH Monolayers

Two-dimensional Janus hydrogenated transition metal chalcogenides provide an unusual platform where lattice instabilities, electron-phonon coupling, and superconductivity are strongly intertwined. Using first-principles calculations, we demonstrate that Janus 2H and 1T MoXH (X = S, Se) monolayers host an intrinsic, commensurate charge density wave (CDW) ground state originating from soft phonon modes at the Brillouin zone M point. Real-space supercell optimizations confirm that the CDW reconstruction lowers the total energy and fully stabilizes the lattice, eliminating the imaginary phonon modes present in the high-symmetry metallic structures. Analysis of the electronic susceptibility shows that the CDW instability is not driven by Fermi surface nesting, but instead arises from strong electron-phonon coupling. We further reveal a material-dependent interplay between CDW order and superconductivity. In 1T MoSH, CDW formation enhances low-energy phonon contributions and strengthens electron-phonon coupling, leading to an increased superconducting transition temperature. In contrast, for 1T MoSeH and 2H MoSeH, the CDW phase suppresses electron-phonon coupling and reduces superconductivity. Finally, we show that thermal fluctuations, compressive strain, and carrier doping can selectively suppress CDW order and restore superconductivity. These results establish Janus MoXH monolayers as a tunable two-dimensional system for exploring lattice-driven charge ordering and its competition with superconductivity.

cond-mat.supr-con↗

arXiv2026

Enhanced Electron-Phonon Coupling and Superconductivity in Ba-Alloyed A15 LaH5.75

Recent experiments have established rare earth A15 type hydrides as a distinct family of high temperature superconductors that can be stabilized at significantly lower pressures compared to other superconducting hydrides. In particular, A15 type LaH5.75 was recently shown to be a high Tc superconductor. We have investigated a range of ternary substitutions and demonstrate that partial substitution of La by Ba stabilizes the A15 hydride lattice, with La0.75Ba0.25H5.75 identified as a stable compound. We calculate a superconducting transition temperature of approximately 183 K, almost double that of LaH5.75 at similar pressures. Ba typically acts as a 2 plus ion, while La is 3 plus. The reduced electron count disrupts the formation of H2 units and shifts the Fermi surface, leading to strongly enhanced electron phonon coupling. By contrast, substitution with Hf fails to produce any stable compounds. This work extends emerging alloy design principles in A15 hydride superconductors, demonstrating that doping can shift the Fermi level and tune the strength of the electron phonon coupling. These results provide concrete guidance for the experimental realization of new high Tc phases.

cond-mat.supr-con↗

arXiv2025

The distinction between Ice phases VII, VIII and X

Ice phases VII, VIII and X are all based on a body-centered cubic arrangement of molecules, the differences coming from molecular orientation. There is some debate as to whether these should even be considered distinct phases. The standard definition of a transition between distinct phases involves a discontinuity in any derivative of the free energy. This can be hard to prove experimentally, and most previous theoretical works have been based on models which either have continuously differentiable free energies, or no straightforward way to determine the free energy. Here we build a free energy model based on the common definitions of the phases ; ordered ice-VIII, orientationally disordered ice VII and proton-disordered ice X. All transitions in this model might or might not be associated with a discontinuity in the specific heat, depending on paramaterization. By comparing with data, we find that a VII-X transition line exists, but it ends in a critical point hidden within the stability field of phase VIII. If the model is correct, there is a discontinuity between VII and X, so they are separate phases. We propose that the hidden phase boundary might be demonstrated experimentally by compression of supercooled ice VII.

cond-mat.stat-mech↗

arXiv2024

Solid Solubility in Metallic Hydrogen

Hydrogen in its metallic form is the most common material in our solar system, found under the extreme pressure and temperature conditions found in giant planets. Such conditions are inaccessible to experiment and consequently, theoretical work has typically led experiment. Many remarkable properties are proposed for metallic hydrogen, which is expected to exist in solid form down to low temperatures. Relevant here is that solid metallic hydrogen is not expected to have a close-packed structure, even at extreme pressures. The predicted crystal structure has a packing fraction of only 0.44 compared with 0.74 for fcc. Alloying with other metallic elements can form compounds with atomic hydrogen and much reduced metallization pressure. Here, we investigate the possible solid solubility of a representative range of elements (Be, B, Mg, S, Fe, La) in metallic atomic hydrogen near 500GPa. Zero point energy is highly significant in all cases. The metallic elements Be, Mg, Fe, and La have a well-defined clathrate-style first neighbour shell at 300K, while the non-metallic B and S have more open arrangements. All the elements considered are soluble, in sites substituting for more than one hydrogen atom. The solid solubility of such a wide range of ambient bonding types: simple metals, covalent materials, transition metals, lanthanides, which gives a strong indication that most elements will dissolve in solid metallic hydrogen.

cond-mat.mtrl-sci↗

arXiv2024

Superconductivity and strain-enhanced phase stability of Janus tungsten chalcogenide hydride monolayers

Janus transition metal-dichalcogenide (JTMD) materials have attracted a great deal of attention due to their remarkable physical properties arising from the two-dimensional geometry and the breakdown of the out-of-plane symmetry. Using first-principles density functional theory, we investigated the phase stability, strain-enhanced phase stability, and superconductivity of Janus WSeH and WSH. In addition, we investigated the contribution of the phonon linewidths from the phonon energy spectrum responsible for the superconductivity, and the electron-phonon coupling as a function of phonon wave vectors and modes. Previous work has examined hexagonal 2H and tetragonal 1T structures, but we found that neither is a ground state structure. The metastable 2H phase of WSeH is dynamically stable with Tc around 11.60K, similar to WSH. Compressive biaxial strain - the 2D equivalent of pressure - can stabilize the 1T structures of WSeH and WSH with Tc around 9.23K and 10.52K, respectively.

cond-mat.supr-con↗

arXiv2023

Compression and information entropy of binary strings from the collision history of three hard balls

We investigate how to measure and define the entropy of a simple chaotic system, three hard spheres on a ring. A novel approach is presented, which does not assume the ergodic hypothesis. It consists of transforming the particles collision history into a sequence of binary digits. We then investigate three approaches which should demonstrate the non-randomness of these collision-generated strings compared with random number generator created strings: Shannon entropy, diehard randomness tests and compression percentage. We show that the Shannon information entropy is unable to distinguish random from deterministic strings. The Diehard test performs better, but for certain mass-ratios the collision-generated strings are misidentified as random with high confidence. The zlib and bz2 compression algorithms are efficient at detecting non-randomness and low information content, with compression efficiencies that tend to 100% in the limit of infinite strings. Thus compression algorithm entropy is non-extensive for this chaotic system, in marked contrast to the extensive entropy determined from phase-space integrals by assuming ergodicity.

physics.comp-ph↗

arXiv2023

Breaking the H2 chemical bond in a crystalline environment

Through density functional theory and molecular dynamics calculations, we have analysed various metal polyhydrides to understand whether hydrogen is present in its molecular or atomic form - tetrahydrides of Ba,Sr,Ra, Cs and La; Ba$_8$H$_{46}$ and BaH$_{12}$. We show that, in experimentally reported binary barium hydrides (BaH$_x$), molecular H$_2$ and atomic H$^-$ can coexist with the metallic cations. In this thorough study of differences between BaH$_4$, higher barium hydrides, and other binary tetrahydrides we find the number of atomic hydrogens is equal to the formal charge of the cations. The remaining hydrogen forms molecules in proportions yielding, e.g. BaH$_2$(H$_2)_x$, at pressures as high as 200 GPa. At room temperature these are highly dynamic structures with the hydrogens switching between H$^-$ and H$_2$ while retaining the 2:x ratio. We find some qualitative differences between our static DFT calculations and previously reported structural and spectroscopic experimental results. Two factors allow us to resolve such discrepancies: Firstly, in static relaxation H$_2$ must be regarded as a non-spherical object, which breaks symmetry in a way invisible to X-rays; Secondly the required number of molecules $x$ may be incompatible with the experimental space group (e.g. $BaH_2(H_2)_5$). In molecular dynamics, bond-breaking transitions between various structural symmetry configurations happen on a picosecond timescale via an H$_3^-$ intermediate. Rebonding is slow enough to allow a spectroscopic signal but frequent enough to average out over the lengthscale involved in diffraction.

cond-mat.mtrl-sci↗

arXiv2023

On the existence of an intermediate phase in the antiferromagnetic Ising model on an face-centered cubic lattice

We use Monte Carlo simulation to determine the stable structures in the second-neighbour Ising model on the face-centred cubic lattice. Those structures are L1_1 for strongly antiferromagnetic second neighbour interactions and L1_0 for ferromagnetic and weakly antiferromagnetic second neighbours. We find a third stable "intermediate" antiferromagnetic phase with I4_1/amd symmetry, and calculate the paramagnetic transition temperature for each. The transition temperature depends strongly on second neighbour interactions which are not frustrated. Our results contradict a recent paper, which also reported two different AFM structures and a new "intermediate" phase exists in this system. Here we show that the assumed sublattice structure in is inconsistent with the ground state. We determine a sublattice structure suitable for solving this problem with mean field theory.

cond-mat.stat-mech↗

arXiv2019

The Observed Vibron Shift in Helium-Hydrogen Mixtures are due to Quantum Nuclear and Localisation Effects, not bonding

The vibrational frequency of hydrogen molecules has been observed to increase strongly with He concentration in helium hydrogen fluid mixtures. This has been associated with He-H interactions, either directly through chemical bonding, or indirectly through increased local pressure. Here, we demonstrate that the increase in the Raman frequency of the hydrogen molecule vibron is due to the number of H$_2$ molecules participating in the mode. There is no chemical bonding between He and H$_2$, helium acts only to separate the molecules. The variety of possible environments for H$_2$ gives rise to many Raman active modes, which causes broadening the vibron band. As the Raman active modes tend to be the lower frequency vibrons, these effects work together to produce the majority of the shift seen in experiment. We used Density Functional Theory (DFT) methods in both solid and fluid phases to demonstrate this effect. DFT also reveals that the pressure in these H$_2$-He mixture is primarily due to quantum nuclear effects, again the weak chemical bonding makes it a secondary effect.

cond-mat.mtrl-sci↗

arXiv2018

On the Diffusion of Sticky Particles in 1D

The 1D Ising model is the simplest Hamiltonian-based model in statistical mechanics. The sim- plest interacting particle process is the Symmetric Exclusion Process (SEP), a 1D lattice gas of particles that hop symmetrically and cannot overlap. Combining the two gives a model for sticky particle diffusion, SPM, which is described here. SPM dynamics are based on SEP with short-range interaction, allowing flow due to non-equilibrium boundary conditions. We prove that SPM is also a detailed-balance respecting, particle-conserving, Monte Carlo (MC) description of the Ising model. Neither the Ising model nor SEP have a phase transition in 1D, but the SPM exhibits a non-equilibrium transition from a diffusing to a blocked state as stickiness increases. This transition manifests in peaks in the MC density fluctuation, a change in the dependency of flow-rate on stickiness, and odd structure in the eigenspectrum of the transition rate matrix. We derive and solve a fully non-linear, analytic, mean-field solution, which has a crossover from a positive to a negative diffusion constant where the MC shows the transition. The negative diffusion constant in fact indicates a breakdown of the mean-field approximation, with close to zero flow and breaking into a two-phase mixture, and thus the mean field theory successfully predicts its own demise. We also present an analytic solution for the flow via direct analysis of the transition rate matrix. The simplicity of the model suggest a wide range of possible applications.

cond-mat.stat-mech↗

arXiv2018

MIST: A Simple and Efficient Molecular Dynamics Abstraction Library for Integrator Development

We present MIST, the Molecular Integration Simulation Toolkit, a lightweight and efficient software library written in C++ which provides an abstract in- terface to common molecular dynamics codes, enabling rapid and portable development of new integration schemes for molecular dynamics. The initial release provides plug-in interfaces to NAMD-Lite, GROMACS and Amber, and includes several standard integration schemes, a constraint solver, tem- perature control using Langevin Dynamics, and two tempering schemes. We describe the architecture and functionality of the library and the C and For- tran APIs which can be used to interface additional MD codes to MIST. We show, for a range of test systems, that MIST introduces negligible overheads for serial, shared-memory parallel, and GPU-accelerated cases, except for Amber where the native integrators run directly on the GPU itself. As a demonstration of the capabilities of MIST, we describe a simulated tempering simulation used to study the free energy landscape of Alanine-12 in both vacuum and detailed solvent conditions.

physics.comp-ph↗

arXiv2017

Stability of Metallic Hydrogen at Ambient Conditions

The possibility of metallic hydrogen was first mooted by Wigner and Huntington in 1935. Here it is show that the calculations from that paper are in remarkably good agreement with modern density functional theory results. The possibility that metallic hydrogen could be recovered to ambient pressure is often attributed to papers by Brovman, although in fact they only say it would be metastable with undetermined lifetime. Density functional theory calculations presented here show that reasonable candidate structures for metallic hydrogen are wildly unstable at ambient conditions, and molecular dynamics calculations show that the lifetime to which Brovman et al refer is considerably less than a picosecond. It is concluded that the prospects of using recovered metallic hydrogen as rocket fuel or for electricity distribution may have been overstated.

cond-mat.mtrl-sci↗

arXiv2017

A simple thermodynamic model for the hydrogen phase diagram

We describe a classical thermodynamic model that reproduces the main features of the solid hydrogen phase diagram. In particular, we show how the general structure types that are found by electronic structure calculations and the quantum nature of the protons can also be understood from a classical viewpoint. The model provides a picture not only of crystal structure, but also for the anomalous melting curve and insights into isotope effects, liquid metallisation and InfraRed activity. The existence of a classical picture for this most quantum of condensed matter systems provides a surprising extension of the correspondence principle of quantum mechanics, in particular the equivalent effects of classical and quantum uncertainty.

cond-mat.dis-nn↗

arXiv2016

Shear Melting and High Temperature Embrittlement: Theory and Application to Machining Titanium

We show that alloying with rare earth metals (REMs) can dramatically improve the machineability of a range of titanium alloys, even though the REM is not incorporated in the alloy matrix. The mechanism for this is that under cutting, shear bands are formed within which the nano-precipitates of REM are shear mixed. This lowers the melting point such that the mechanism of deformation changes from dislocation mechanism to localised amorphisation and shear softening. The material then fractures along the thin, amorphous shear-band. Outside the shear band, the REM remains as precipitates. The new alloys have similar mechanical properties and biocompatibility to conventional materials.

cond-mat.mtrl-sci↗