arXiv subjects

Hubert J. Naguszewski

Publications and source records attributed to Hubert J. Naguszewski.

6 recordsLinked to original sources

arXiv2026

Formation of $\mathrm{L}1_2$-ordered $γ'$-$\mathrm{Ni}_3\mathrm{Al}$ precipitates in ternary Cu-Ni-Al alloys modelled using an ab initio concentration wave theory and atomistic simulations

Precipitation-strengthened Cu-Ni-Al alloys are of interest for technological applications because coherent, $\mathrm{L}1_2$-ordered $γ'$-$\mathrm{Ni}_3\mathrm{Al}$ precipitates can confer high mechanical strength while allowing the material to retain many of the good transport properties characteristic of elemental Cu. In this work, we study the thermodynamics and phase stability of the pseudobinary $\textrm{Cu}_x (\textrm{Ni}_{3/4} \textrm{Al}_{1/4})_{1-x}$ system, $0 \leq x \leq 1$. We use a computational modelling framework combining first-principles electronic structure calculations with a concentration wave analysis from which atom-atom effective pair interactions are extracted for use in atomistic Monte Carlo simulations. Our modelling reveals three distinct, composition-dependent regimes of phase behaviour, in qualitative agreement with the experimentally determined phase diagram. At low Cu content, Cu is soluble in the $\mathrm{L}1_2$-ordered $\mathrm{Ni}_3\mathrm{Al}$ phase, with a single identifiable phase transition corresponding to chemical ordering between Ni and Al. At intermediate compositions, this high-temperature ordering is followed at lower temperatures by phase separation of Cu and $\mathrm{L}1_2$-ordered $\mathrm{Ni}_3\mathrm{Al}$. Finally, at high Cu content, $\mathrm{L}1_2$-ordered $\mathrm{Ni}_3\mathrm{Al}$ precipitates directly from the solid solution, with no clearly identifiable secondary transition. We relate these phase transformations to features of the underlying electronic structures of the considered alloys. Overall, this work demonstrates a computationally efficient workflow capturing both chemical ordering and coherent precipitation in multicomponent substitutional alloys, with relevance to the study of phenomena such as precipitation strengthening.

cond-mat.mtrl-sci↗

arXiv2026

Learned Committors as Reaction Coordinates for Nucleation Rates

A central challenge in the analysis of first-order phase transitions is the identification of optimal reaction coordinates. In principle, the committor is the ideal choice; however, its computational cost has historically made it intractable. Here, we train a convolutional neural network ($p_B$-NN) as a proxy for the committor on brute-force committor labels and use it directly as the coordinate of a Markov state model. Applied to magnetisation reversal in the two-dimensional Ising model, $p_B$-NN reproduces brute-force nucleation rates across a range of thermodynamic conditions. The largest geometric cluster size also recovers accurate rates despite providing a poor pointwise predictor of the committor. These results demonstrate that an effective reaction coordinate for nucleation rate calculation must reliably separate the metastable and stable basins, but need not preserve the committor pointwise for every microstate. We stress that this distinction has direct implications for the choice of collective variable in rare-event simulations of nucleation more broadly.

physics.comp-ph↗

arXiv2026

Optimal parallelisation strategies for flat histogram Monte Carlo sampling

Flat histogram methods, such as Wang--Landau sampling, provide a means for high-throughput calculation of phase diagrams of atomistic/lattice model systems. Many parallelisation schemes with varying degrees of complexity have been proposed to accelerate such sampling simulations. In this study, several widely used schemes are benchmarked -- both in isolation and in combination -- to establish best practice. The schemes studied include energy domain decomposition with both static sizing of energy sub-domains, as well as a dynamic sub-domain sizing scheme which we propose. We also assess the benefits both of replica exchange and of including multiple random walkers per sub-domain, to determine which factors have the largest impact on parallel efficiency. Additionally, the influence of energy sub-domain overlap regions is discussed. As illustrative test cases, we implement and apply the aforementioned strategies to a lattice-based model describing the internal energy of a substitutional alloy, studying the AlTiCrMo refractory high-entropy superalloy as well as the binary CuZn system, both of which crystallographically order into a B2 (CsCl) structure with decreasing temperature. We find that -- while all of the proposed strategies confer a non-negligible speedup -- parallelisation across energy domains which are non-uniform in size offers the most appreciable performance improvements. This work offers concrete recommendations for which parallelisation strategies should be prioritised to optimally accelerate flat-histogram Monte Carlo simulations.

physics.comp-ph↗

arXiv2026

Electronic structure, phase stability, and transport properties of the AlTiVCr lightweight high-entropy alloy: A computational study

We investigate the thermodynamics and phase stability of the AlTiVCr lightweight high-entropy alloy using a combination of ab initio electronic structure calculations, a concentration wave analysis, and atomistic Monte Carlo simulations. In alignment both with experimental data and with results obtained using other computational approaches, we predict a $\textrm{B2}$ (CsCl) chemical ordering emerging in this alloy at comparatively high temperatures, which is driven by Al and Ti moving to separate sublattices, while V and Cr express weaker site preferences. The impact of this $\textrm{B2}$ chemical ordering on the electronic transport properties of the alloy is investigated within a Kubo-Greenwood linear response framework and it is found that, counter-intuitively, the alloy's residual resistivity increases as the material transitions from the $\textrm{A2}$ (disordered bcc) phase to our predicted $\textrm{B2}$ (partially) ordered structure. This is understood to result primarily from a reduction in the density of electronic states at the Fermi level induced by the chemical ordering. At low temperatures, our atomistic Monte Carlo simulations then reveal subsequent sublattice orderings, with the ground-state configuration predicted to be a fully-ordered, single-phase structure with vanishing associated residual resistivity. These results give fresh, insight into the atomic-scale structure and consequent physical properties of this well-studied, technologically relevant material.

cond-mat.mtrl-sci↗

arXiv2025

BraWl: Simulating the thermodynamics and phase stability of multicomponent alloys using conventional and enhanced sampling techniques

We present BraWl, a Fortran package implementing a range of conventional and enhanced sampling algorithms for exploration of the phase space of the Bragg-Williams model, facilitating study of diffusional solid-solid transformations in binary and multicomponent alloys. These sampling algorithms include Metropolis-Hastings Monte Carlo, Wang-Landau sampling, and Nested Sampling. We demonstrate the capabilities of the package by applying it to some prototypical binary and multicomponent alloys, including high-entropy alloys.

physics.comp-ph↗

arXiv2025

Emergent B2 chemical orderings in the AlTiVNb and AlTiCrMo refractory high-entropy superalloys studied via first-principles theory and atomistic modelling

We study the thermodynamics and phase stability of the AlTiVNb and AlTiCrMo refractory high-entropy superalloys using a combination of \textit{ab initio} electronic structure theory -- namely a concentration wave analysis -- and atomistic Monte Carlo simulations. Our multiscale approach is suitable both for examining atomic short-range order in the solid solution, as well as for studying the emergence of long-range crystallographic order with decreasing temperature. In both alloys considered in this work, in alignment with experimental observations, we predict a B2 (CsCl) chemical ordering emerging at high temperatures, which is driven primarily by Al and Ti, with other elements expressing weaker site preferences. The predicted B2 ordering temperature for AlTiVNb is higher than that for AlTiCrMo. These chemical orderings are discussed in terms of the alloys' electronic structure, with hybridisation between the $sp$ states of Al and the $d$ states of the transition metals understood to play an important role. Within our modelling, the chemically ordered B2 phases for both alloys have an increased predicted residual resistivity compared to the A2 (disordered bcc) phases. These increased resistivity values are understood to originate in a reduction in the electronic density of states at the Fermi level, in conjunction with qualitative changes to the alloys' smeared-out Fermi surfaces. These results highlight the close connections between composition, structure, and physical properties in this technologically relevant class of materials.

cond-mat.mtrl-sci↗