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Michael R. von Spakovsky

Publications and source records attributed to Michael R. von Spakovsky.

At least 19 recordsLinked to original sources

Modeling Dynamic Magnetic Response of Spinel Soft Ferrites with the Steepest-Entropy-Ascent Quantum Thermodynamics Formalism

Selecting soft ferrites for alternating-field applications requires balancing magnetic response, dissipation, nonlinearity, and heating. We use a field-driven steepest-entropy-ascent quantum thermodynamic (SEAQT) model to compare the electron, phonon, and magnon responses of Fe$_3$O$_4$, MnFe$2$O$4$, and (Mn${0.5}$Zn${0.5}$)Fe$_2$O$_4$ within a common first-principles framework. The model treats spatially uniform longitudinal relaxation and neglects domain-wall motion, transverse rotation, resonance, eddy-current effects, and heat removal. We use $τ_e=0.05$ ps and $τ_p=3$ ps for all three materials, with effective longitudinal magnon relaxation times of 500, 200, and 85 ps, respectively; these literature-motivated values are model inputs, not fits to measured losses. Within this framework, the Mn--Zn ferrite gives the largest peak longitudinal magnetization change, retains its response best at high frequency, and shows the largest work per cycle and peak-to-peak magnon temperature change, whereas MnFe$_2$O$_4$ gives the largest normalized $χ''$ peak. Thus, no single ferrite ranks highest across all metrics: the preferred material depends on the property, frequency, field amplitude, and cation configuration of interest. The model therefore provides a spectrum- and kinetics-resolved screening tool for engineering comparison of ferrites rather than a prediction of total core loss.

cond-mat.mtrl-sci↗

Field-Driven Coupled Magnon--Phonon--Electron Relaxation in Magnetite Using Steepest-Entropy-Ascent Quantum Thermodynamic Formalism

A field-driven steepest-entropy-ascent quantum thermodynamic (SEAQT) formulation is developed for longitudinal nonequilibrium relaxation in magnetite (Fe$_3$O$_4$) with coupled electron, phonon, and magnon populations. Material-specific excitation spectra define the thermodynamic state space, while one relaxation parameter for each population sets its kinetic scale. A longitudinal magnetic field shifts the dressed magnon eigenenergies while the occupation basis remains fixed; irreversible redistribution conserves instantaneous energy and electron number while allowing the magnon population to vary. The formulation yields nonequilibrium subsystem temperatures, entropy production, magnetic-work identities, and a coupled small-signal susceptibility incorporating energy-conservation feedback among all three populations; the one-pole Debye response appears only as a limiting case. Numerical results under sinusoidal driving show a transition from nearly quasistatic behavior to frequency-dependent lag, finite-amplitude departure from the linear-response ellipse, and increasing higher-harmonic content. Relaxational work per cycle increases strongly with field amplitude and frequency, while the complex susceptibility is broader and shifted relative to a Debye reference. Entropy production remains positive, and the electron, phonon, and magnon temperatures show distinct excursions followed by secular heating when positive magnetic work is retained without heat rejection. The calculated work represents longitudinal magnon quasiparticle relaxation in a homogeneous single-domain model, not the total core loss of a finite ferrite specimen.

cond-mat.mtrl-sci↗

Energy Eigenstates of Electrons, Magnons and Phonons in Fe$_3$O$_4$ (magnetite), MnFe$_2$O$_4$ (jacobsite), and mixed Mn-Zn ferrites

We report first-principles calculations of the electronic structure, magnon excitations, and phonons in magnetite (Fe$_3$O$_4$), jacobsite (MnFe$_2$O$_4$), and mixed manganese-zinc ferrites (Mn$_{x}$,Zn$_{1-x}$)Fe$_2$O$_4$ for representative compositions ($0\le x \le 1$) and A/B-site cation arrangements. Electronic structures are computed using density functional theory (DFT) augmented by rotationally invariant DFT+U+J, with on-site Hubbard and Hund's parameters, $U$ and $J$, respectively, determined self-consistently by spin-polarized linear-response perturbations of the chosen correlated subspaces (including, where applied, the ligand $2p$ subspace). A classical Heisenberg spin Hamiltonian is parameterized by mapping DFT+U+J total energies for multiple collinear spin configurations onto nearest-neighbor exchange couplings, which are then used to obtain magnon dispersions and magnon densities of states within linear spin-wave theory. Phonon spectra and densities of states are obtained from finite-displacement force constants and dynamical matrices computed on the same DFT+U+J-relaxed structures. Overall, the workflow provides a consistent, composition- and configuration-aware route to electronic, vibrational, and magnetic excitation spectra across the Mn/Zn ferrite space.

cond-mat.mtrl-sci↗

Optimizing QAOA circuit transpilation with parity twine and SWAP network encodings

Mapping quantum approximate optimization algorithm (QAOA) circuits with non-trivial connectivity in fixed-layout quantum platforms, such as superconducting quantum processing units (QPUs), requires a transpilation process to match the circuit to the hardware layout. This step is critical for reducing error rates on noisy QPUs. Two approaches that improve the resources required for such transpilation are the SWAP network and parity twine chains (PTC), which reduce the two-qubit gate count and circuit depth needed to represent fully connected circuits. In this work, we introduce a simulated annealing-based method that further reduces the encoding overhead of PTC and SWAP networks for QAOA circuits with non-fully connected two-qubit interactions. The method is benchmarked against various transpilers, including the Qiskit SAT mapper, demonstrating that beyond specific connectivity thresholds it achieves significant reductions in both two-qubit gate count and circuit depth. For example, for a 120-qubit QAOA instance with 25% connectivity, our method achieves an 87\% reduction in depth and a 29% reduction in two-qubit gates compared to the Qiskit transpiler. Finally, the practical impact of PTC encoding is validated by benchmarking QAOA on the ibm_fez and ibm_kingston devices, showing improved performance for systems of up to 20 qubits.

quant-ph↗

Evolution of Hypoequilibrium States in Steepest Entropy Ascent Models for Nonequilibrium Quantum Thermodynamics

A formal development of the hypoequilibrium (HE) state concept within the Steepest-Entropy-Ascent Quantum Thermodynamics (SEAQT) framework is presented, emphasizing its rigorous mathematical formulation. Using a general decomposition of the Hilbert space, HE states are defined in operator language and the reduced evolution of the associated intensive parameters for the regime where the dissipative dynamics commutes with the Hamiltonian is derived. It is proved that the $M$-th order HE family (where $M$ is the number of spectral sectors) constitutes an invariant manifold under the SEAQT equation of motion, ensuring that states initially representing a ``mixture of canonicals'' maintain this structure throughout their evolution. Furthermore, a formal connection is established between the HE ansatz and the rate-controlled constrained equilibrium (RCCE) method, identifying HE variables as constraint potentials. Finally, the model is extended to non-Hamiltonian SEAQT (NH-SEAQT) interactions to describe thermodynamically consistent energy and entropy exchanges between subsystems and heat baths. This work provides the formal foundation for reduced-order modeling of far-from-equilibrium relaxation and transport processes, and supports a methodology previously applied across various physical and chemical systems.

quant-ph↗

Diagnosing crosstalk in large-scale QPUs using zero-entropy classical shadows

As quantum processing units (QPUs) scale toward hundreds of qubits, diagnosing noise-induced correlations (crosstalk) becomes critical for reliable quantum computation. In this work, we introduce Zero-Entropy Classical Shadows (ZECS), a diagnostic tool that uses information of a rank-one quantum state tomography (QST) reconstruction from classical shadow (CS) information to make a crosstalk diagnosis. We use ZECS on trapped ion and superconductive QPUs, including ionq_forte (36 qubits), ibm_brisbane (127 qubits), and ibm_fez (156 qubits), using from 1,000 to 6,000 samples. With these samples, we use the ZECS to characterize crosstalk among disjoint qubit subsets across the full hardware. This information is then used to select low-crosstalk qubit subsets on ibm_fez for executing the Quantum Approximate Optimization Algorithm (QAOA) on a 20-qubit problem. Compared to the best qubit selection via Qiskit transpilation, our method improves solution quality by 10% and increases algorithmic coherence by 33%. ZECS offers a scalable and measurement-efficient approach to diagnosing crosstalk in large-scale QPUs.

quant-ph↗

Steepest-Entropy-Ascent Framework for Predicting Arsenic Adsorption on Graphene Oxide Surfaces -- A Case Study

Water contamination by arsenic(V) constitutes a major public-health concern, underscoring the need for models that capture both equilibrium and transient adsorption behaviour. A framework that can do so is the steepest-entropy-ascent quantum thermodynamic (SEAQT) framework, which is used here to describe the uptake of As(V) on graphene oxide (GO) across pollutant concentrations of 25-350 mg/L. A non-equilibrium equation of motion derived from the steepest-entropy-ascent principle for a five-component system (water, arsenic, two GO functional groups, and protons is solved with an energy eigenstructure generated by a Replica-Exchange Wang-Landau algorithm and then extrapolated to relevant contaminant concentrations via an artificial neural network. Without recourse to empirical rate laws, the model predicts the time-dependent adsorption capacity, the stable-equilibrium arsenic concentration, and the pH dependence of removal efficiency. Equilibrium capacities are reproduced within 5 % of experimental isotherms, and the characteristic adsorption time aligns with the reported kinetics. These results indicate that SEAQT framework provides a thermodynamically consistent, fully predictive tool for designing and optimising adsorbent-based water-treatment technologies.

physics.chem-ph↗

Model for Predicting Adsorption Isotherms and the Kinetics of Adsorption via Steepest-Entropy-Ascent Quantum Thermodynamics

This work outlines the foundations for being able to do a first-principle study of the adsorption process using the steepest-entropy-ascent quantum thermodynamic (SEAQT) framework, a framework able to predict the unique non-equilibrium path taken by a system from some initial state to stable equilibrium. To account for the process of multi-component adsorption, the SEAQT framework incorporates the particle number operator for each absorbed species directly into its equation of motion. The theoretical models developed are validated via some initial comparisons with experimental data found in the literature, demonstrating good agreement. The findings reveal that this framework can be an effective tool for describing the adsorption process out of equilibrium. It is able to do so without $a \; priori$ knowledge of the specific adsorption mechanism(s) involved. It also aligns well with the anticipated predictions of equilibrium models. In addition, within this framework, all intensive thermodynamic properties are characterized by out-of-equilibrium fluctuations, highlighting the significance of non-equilibrium thermodynamics in predicting measurable physical quantities.

physics.chem-ph↗

Predicting Ion Sequestration in Charged Polymers with the Steepest-Entropy-Ascent Quantum Thermodynamic Framework

The steepest-entropy-ascent quantum thermodynamic framework is used to investigate the effectiveness of multi-chain polyethyleneimine-methylenephosphonic acid in sequestering rare-earth ions (Eu$^{+3}$) from aqueous solutions. The framework applies a thermodynamic equation of motion to a discrete energy eigenstructure to model the binding kinetics of europium ions to reactive sites of the polymer chains. The energy eigenstructure is generated using a non-Markovian Monte Carlo model that estimates energy level degeneracies. The equation of motion is used to determine the occupation probability of each energy level, describing the unique path through thermodynamic state space by which the polymer system sequesters rare-earth ions from solution. A second Monte Carlo simulation is conducted to relate the kinetic path in state space to physical descriptors associated with the polymer, including the radius of gyration, tortuosity, and Eu-neighbor distribution functions. These descriptors are used to visualize the evolution of the polymer during the sequestration process. The fraction of sequestered Eu$^{+3}$ ions depends upon the total energy of the system, with lower energy resulting in higher sequestration. The kinetics of the overall sequestration are dependent on the steepest-entropy-ascent principle used by the equation of motion to generate a unique kinetic path from an initial non-equilibrium state.

cond-mat.soft↗

Predicting Polymer Brush Behavior in Solvents using the Steepest-Entropy-Ascent Quantum Thermodynamic Framework

The steepest-entropy-ascent quantum thermodynamic (SEAQT) framework is utilized to study the effects of temperature on polymer brushes. The brushes are represented by a discrete energy spectrum and energy degeneracies obtained through the Replica-Exchange Wang-Landau algorithm. The SEAQT equation of motion is applied to the density of states to establish a unique kinetic path from an initial thermodynamic state to a stable equilibrium state. The kinetic path describes the brush's evolution in state space as it interacts with a thermal reservoir. The predicted occupation probabilities along the kinetic path are used to determine expected thermodynamic and structural properties. The polymer density profile of a polystyrene brush in cyclohexane solvent is predicted using the equation of motion, and it agrees qualitatively with experimental density profiles. The Flory-Huggins parameter chosen to describe brush-solvent interactions affects the solvent distribution in the brush but has minimal impact on the polymer density profile. Three types of non-equilibrium kinetic paths with differing amounts of entropy production are considered: a heating path, a cooling path, and a heating-cooling path. Properties such as tortuosity, radius of gyration, brush density, solvent density, and brush chain conformations are calculated for each path.

cond-mat.soft↗

Predicting Non-Equilibrium Folding Behavior of Polymer Chains using the Steepest-Entropy-Ascent Quantum Thermodynamic Framework

The Replica Exchange Wang-Landau Method is used to estimate the energy landscape of a polymer composed of a simple hydrophobic and polar sequence using the HP protein model. Calculations of state transitions between the energy levels of the derived energy landscape are made using an equation of motion from the steepest-entropy-ascent quantum thermodynamic (SEAQT) framework. The SEAQT framework makes it possible to determine the unique kinetic paths from an arbitrary quasi-equilibrium or non-equilibrium initial state to stable equilibrium. Calculations performed with SEAQT require significantly reduced computational time versus comparable Monte Carlo simulations while providing otherwise unavailable thermodynamic and structural properties. Expected values for state averaged structural parameters are used to produce representative reconstructions of the calculated state-based evolution. Results show continuous transitions between states with no distinct folding phases. Changes in chain conformations during heating and cooling are more drastic along non-equilibrium paths than along quasi-equilibrium paths. In addition, SEAQT-derived kinetics are compared to experimentally derived intensity profiles describing the kinetics of the cytochrome c protein using Rouse dynamic relations.

cond-mat.soft↗

Predicting Defect Stability and Annealing Kinetics in Two-Dimensional PtSe$_2$ Using Steepest Entropy Ascent Quantum Thermodynamics

The steepest-entropy-ascent quantum thermodynamic (SEAQT) framework was used to calculate the stability of a collection of point defects in 2D PtSe$_2$ and predict the kinetics with which defects rearrange during thermal annealing. The framework provides a non-equilibrium, ensemble-based framework with a self-consistent link between mechanics (both quantum and classical) and thermodynamics. It employs an equation of motion derived from the principle of steepest entropy ascent (maximum entropy production) to predict the time evolution of a set of occupation probabilities that define the states of a system undergoing a non-equilibrium process. The system is described by a degenerate energy landscape of eigenvalues, and the entropy is found from the occupation probabilities and the eigenlevel degeneracies. Scanning tunneling microscopy was used to identify the structure and distribution of point defects observed experimentally in a 2D PtSe$_2$ film. A catalog of observed defects included six unique point defects (vacancies and anti-site defects on Pt and Se sublattices) and twenty combinations of multiple point defects in close proximity. The defect energies were estimated with density functional theory (DFT), while the degeneracies, or density of states, for the 2D film with all possible combinations or arrangements of cataloged defects was constructed using a non-Markovian Monte-Carlo approach (i.e., the Replica-Exchange-Wang-Landau algorithm) with a q-state Potts model. The energy landscape and associated degeneracies were determined for a 2D PtSe$_2$ film two molecules thick and $30 \times 30$ unit cells in area (total of 5400 atoms). The SEAQT equation of motion was applied to the energy landscape to determine how an arbitrary density and arrangement of the six defect types evolve during annealing.

cond-mat.mtrl-sci↗

Entropy-Driven Microstructure Evolution Predicted with the Steepest-Entropy-Ascent Quantum Thermodynamic Framework

A Potts model and the Replica Exchange Wang-Landau algorithm are used to construct an energy landscape for a crystalline solid containing surfaces and grain boundaries. The energy landscape is applied to an equation of motion from the steepest-entropy-ascent quantum thermodynamic (SEAQT) framework to explore the kinetics of three distinct kinds of microstructural evolution: polycrystalline sintering, precipitate coarsening, and grain growth. The steepest entropy ascent postulate predicts unique kinetic paths for these non-equilibrium processes without needing any detailed information about the underlying physical mechanisms of the processes. A method is also proposed for associating the kinetic path in state space to a set of smoothly evolving microstructural descriptors. The SEAQT-predicted kinetics agree well with available experimental kinetics for ZrO2 sintering, Al3Li precipitate coarsening, and grain growth in nanocrystalline Pd. The computational cost associated with calculating the energy landscape needed by the approach is comparable to a Monte Carlo simulation. However, the subsequent kinetic calculations from the SEAQT equation of motion are quite modest and save considerable computational resources by obviating the need for averaging multiple kinetic Monte Carlo runs.

cond-mat.mtrl-sci↗

Method for Generating Randomly Perturbed Density Operators Subject to Different Sets of Constraints

This paper presents a general method for producing randomly perturbed density operators subject to different sets of constraints. The perturbed density operators are a specified "distance" away from the state described by the original density operator. This approach is applied to a bipartite system of qubits and used to examine the sensitivity of various entanglement measures on the perturbation magnitude. The constraint sets used include constant energy, constant entropy, and both constant energy and entropy. The method is then applied to produce perturbed random quantum states that correspond with those obtained experimentally for Bell states on the IBM quantum device ibmq_manila. The results show that the methodology can be used to simulate the outcome of real quantum devices where noise, which is important both in theory and simulation, is present.

quant-ph↗

Loss-of-entanglement prediction of a controlled-PHASE gate in the framework of steepest-entropy-ascent quantum thermodynamics

As has been shown elsewhere, a reasonable model of the loss of entanglement or correlation that occurs in quantum computations is one which assumes that they can effectively be predicted by a framework that presupposes the presence of irreversibilities internal to the system. It is based on the steepest-entropy-ascent principle and is used here to reproduce the behavior of a controlled-PHASE gate in good agreement with experimental data. The results show that the loss of entanglement predicted is related to the irreversibilities in a nontrivial way, providing a possible alternative approach that warrants exploration to that conventionally used to predict the loss of entanglement. The results provide a means for understanding this loss in quantum protocols from a nonequilibrium thermodynamic standpoint. This framework permits the development of strategies for extending either the maximum fidelity of the computation or the entanglement time.

quant-ph↗

Low-temperature Atomistic Spin Relaxation and Non-equilibrium Intensive Properties Using Steepest-Entropy-Ascent Quantum-Inspired Thermodynamics Modeling

The magnetization of body-centered cubic iron at low temperatures is calculated with the steepest-entropy-ascent quantum thermodynamics (SEAQT) framework. This framework assumes that a thermodynamic property in an isolated system traces the path through state space with the greatest entropy production. Magnetization is calculated from the expected value of a thermodynamic ensemble of quantized spin waves based on the Heisenberg spin model applied to an ensemble of coupled harmonic oscillators. A realistic energy landscape is obtained from a magnon dispersion relation calculated using spin-density-functional-theory. The equilibrium magnetization as well as the evolution of magnetization from a non-equilibrium state to equilibrium are calculated from the path of steepest entropy ascent determined from the SEAQT equation of motion in state space. The framework makes it possible to model the temperature- and time-dependence of magnetization without a detailed description of magnetic damping. The approach is also used to define intensive properties (temperature and magnetic field strength) that are fundamentally, i.e., canonically or grand canonically, valid for any non-equilibrium state. Given the assumed magnon dispersion relation, the SEAQT framework is used to calculate the equilibrium magnetization at different temperatures and external magnetic fields and the results are shown to closely agree with experiment for temperatures less than 500 K. The time-dependent evolution of magnetization from different initial states and interactions with a reservoir is also predicted.

cond-mat.mtrl-sci↗

Steepest-Entropy-Ascent Quantum Thermodynamics Models in Materials Science

Steepest-entropy-ascent quantum thermodynamics, or SEAQT, is a unified approach of quantum mechanics and thermodynamics that avoids many of the inconsistencies that can arise between the two theories. Given a set of energy levels, i.e., energy eigenstructure, accessible to a given physical system, SEAQT predicts the unique kinetic path from any initial non-equilibrium state to stable equilibrium by solving a master equation that directs the system along the path of steepest entropy ascent. There are no intrinsic limitations on the length and time scales the method can treat so it is well-suited for calculations where the dynamics over multiple spacial scales need to be taken into account within a single framework. In this paper, the theoretical framework and its advantages are described, and several applications are presented to illustrate the use of the SEAQT equation of motion and the construction of a simplified, reduced-order, energy eigenstructure.

cond-mat.mtrl-sci↗

Kinetic Pathways of Phase Decomposition Using Steepest-Entropy-Ascent Quantum Thermodynamics Modeling. Part II: Phase Separation and Ordering

The kinetics of ordering and concurrent ordering and clustering is analyzed with an equation of motion initially developed to account for dissipative processes in quantum systems. A simplified energy eigenstructure, or pseudo-eigenstructure, is constructed from a static concentration wave method to describe the configuration-dependent energy for atomic ordering and clustering in a binary alloy. This pseudo-eigenstructure is used in conjunction with an equation of motion that follows steepest entropy ascent to calculate the kinetic path that leads to ordering and clustering in a series of hypothetical alloys. By adjusting the thermodynamic solution parameters, it is demonstrated that the model can predict the stable equilibrium state as well as the unique thermodynamic path and kinetics of continuous/discontinuous ordering and concurrent processes of simultaneous ordering and phase separation.

cond-mat.mtrl-sci↗