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Luke Allen Myers

Publications and source records attributed to Luke Allen Myers.

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Recursive entropy in thermodynamics: expounding the statistical-physics basis of the zentropy approach

The recursive property of entropy is well known in information theory; however, the concept is underutilized in thermodynamics, despite being the field where the concept of entropy originated. The zentropy approach is built on this idea, and it has emerged as a useful framework for describing thermodynamic systems across multiple scales, yet its statistical-physics foundation has not been fully articulated. In this work, we establish that foundation by showing that the recursive property allows us to coarse-grain thermodynamic systems into the most useful groups, and deriving the Helmholtz energy and partition function by maximizing entropy in its recursive form. This derivation clarifies the thermodynamic meaning of so-called "states that depend on temperature" as coarse-grained configurations, and maintains a clear distinction between the physical and statistical aspects of statistical mechanics. We then illustrate the usefulness of the approach through two representative applications: magnetic materials, where configurations are defined by spin arrangements, and liquids, where configurations are defined by nearest-neighbor environments. In both cases, the framework enables physically meaningful coarse-graining and captures emergent behavior arising from probability redistribution among configurations. These results position zentropy as an exact and flexible multiscale framework for thermodynamics and statistical mechanics, particularly for systems that admit a natural hierarchical grouping of states.

cond-mat.stat-mech

pyzentropy: A Python package implementing recursive entropy for first-principles thermodynamics

While the recursive property of entropy is well known in information theory, it is rarely utilized in thermodynamics, despite entropy originating in this field. Moreover, computational tools to implement this concept within first-principles thermodynamics remain lacking. In this work, we introduce an open-source Python package, pyzentropy, to implement this approach. We demonstrate its effectiveness using $Fe_3Pt$ as a case study, considering a 12-atom supercell with multiple magnetic configurations. By applying the recursive formulation of entropy to compute the total entropy of the system, we reproduce the Invar behavior, along with the anomalous temperature dependence of the linear coefficient of thermal expansion (LCTE), heat capacity $C_P$, and bulk modulus $B$. We also construct the $T$-$V$ and $P$-$T$ phase diagrams in good agreement with experimental observations. Finally, we highlight the importance of determining key high-probability configurations to accurately capture material properties.

cond-mat.mtrl-sci

Density Functional Theory ToolKit (DFTTK) to Automate First-Principles Thermodynamics via the Quasiharmonic Approximation

The Helmholtz energy is a key thermodynamic quantity representing available energy to do work at a constant temperature and volume. Despite a well-established methodology from first-principles calculations, a comprehensive tool and database are still lacking. To address this gap, we developed an open-source Density Functional Theory Tool Kit (DFTTK), which automates first-principles thermodynamics using the quasiharmonic approximation (QHA) for Helmholtz energy predictions. This Python-based package provides a solution for automating the calculation and analysis of various contributions to Helmholtz energy, including the static total energy contributions at 0 K in terms of DFT-based energy-volume curves, vibrational contributions from the Debye-Gruneisen model and phonons, and thermal electronic contributions via the electronic density of states. The QHA is also implemented to calculate the Gibbs energy and associated properties at constant temperature and pressure. The present work demonstrates DFTTK's capabilities through case studies on a simple FCC Al and various collinear magnetic configurations of Invar Fe3Pt, where DFTTK enumerates all unique configurations and their associated multiplicities. DFTTK is freely available on GitHub, and its modular design allows for the easy addition of new workflows.

cond-mat.mtrl-sci