arXiv subjects

Matthieu J. Verstraete

Publications and source records attributed to Matthieu J. Verstraete.

At least 19 recordsLinked to original sources

arXiv2026

Beyond Allen-Heine-Cardona: non-perturbative electron-phonon interactions in the linewidths and lineshifts of diamond

The temperature-dependent band gap of solids is usually computed from the perturbative Allen-Heine-Cardona (AHC) electron-phonon self-energy evaluated on-shell. Extending AHC to arbitrary frequency $ω$ to determine the full spectral function via the Dyson equation is known to fail, misplacing satellites and yielding no broadening at band extrema, while non-perturbative supercell (SC) methods have focused on eigenvalue averages rather than lineshapes, and approaches based on special displacements cannot describe the full lineshape, or the lineshift at degenerate bands. Here we use a non-perturbative Green's function method (NPG), stochastically sampling distorted SC configurations, from which the spectral function, including lineshift, linewidth, and asymmetry, follows directly, and we recover finite spectral weight at the renormalized band extrema. We prove that the perturbative self-energy, computed to any order with the bare propagator and introduced into the Dyson equation, has an imaginary part that vanishes within the bare gap, giving incorrect spectral functions: self-consistency of the propagator is essential to broaden the band edges. NPG satisfies this property by construction, and contains all non-bubble diagrams. We also give a simple explanation of why SC methods converge with much smaller SCs than the corresponding $\mathbf{q}$-grids required by perturbation theory. For the band gap shift itself, the NPG and on-shell AHC results are found to be comparable, demonstrating that higher-order terms do not significantly alter the resulting renormalization in diamond. When it comes to the spectral function though, our results show that going beyond bare perturbation theory is not merely more accurate, but necessary, and NPG provides a robust framework to capture spectral broadening and higher-order effects from first principles.

cond-mat.mtrl-sci↗

arXiv2026

Temperature dependence of the charge density from first principles: application to the (222) forbidden reflection in silicon

Forbidden reflections (FRs) in X-ray diffraction have inherently weak intensity and have long been studied, in particular in semiconductors like silicon. They serve as sensitive probes of symmetry breaking, local strain, impurities, and weak charge redistribution. Despite extensive experimental work, the theory of their temperature dependence has typically relied on simplified models. While atomic Debye-Waller factors work well on allowed reflections, their applicability to the valence charge between atoms, which determines the intensity of FRs such as Si (222), is questionable, and previous agreement between theory and experiment relied on ad-hoc Debye-Waller corrections. We compute the temperature-dependent valence charge density $ρ(\mathbf{r},T)$ of silicon from first principles, using two methods: (i) perturbation theory, and (ii) averaging over thermally distorted supercells in a non-perturbative approach. The perturbative expression for the charge density is far more demanding than that for electronic energies, since it depends on the wavefunctions themselves and requires an explicit sum over unoccupied bands. We use an acoustic sum rule to express the second derivatives of the potential in terms of first derivatives, making the expression tractable within existing frameworks. The (222) FR then follows directly from the Fourier transform of $ρ(\mathbf{r},T)$, with no ad-hoc factors. Both methods give similar results, in reasonable agreement with experiment, with thermal expansion noticeably affecting the temperature dependence. The charge density answers a question the measured intensities could not settle: how the valence charge actually redistributes with temperature. Relative to the rigid model, we find more charge in the bonds and less in the core regions, a redistribution that shows up in the intensity as a somewhat weaker temperature dependence of the (222) FR.

cond-mat.mtrl-sci↗

arXiv2026

Theory of phonon-magnon hybridization and angular momentum in CrI$_3$ and CrBr$_3$

In magnetic materials angular momentum can be mediated by different carriers, including electrons, magnons, and phonons. The magnons can interact with circularly polarized phonons which are close in energy, provided specific symmetry conditions are met. If the interaction is strong enough the phonons and magnons shift in frequency and start to mix to form hybrid magneto-elastic quasi-particles. In this paper, we develop a constrained Hamiltonian framework which incorporates hybrid stiffness matrices and Berry curvatures. We quantify the degree of hybridization between phonons and magnons (up to 8% in CrI$_3$ and 25% in CrBr$_3$) using a decomposition of the total energy, which is a generalization of the norm decomposition for atomic contributions to phonons used in the literature. We also explore how the total angular momentum is conserved but shared between the phononic and magnonic subsystems upon hybridization.

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arXiv2026

First-Principles Spin-Lattice Coupling from Downfolded Electron-Phonon Interaction

We present a method to calculate spin-phonon coupling parameters from first-principles perturbation theory by downfolding the electron-phonon coupling (EPC). We exploit the localized nature of magnetic moments and atomic displacements by working in the Wannier representation of the electronic Hamiltonian and the EPC matrix. The spin system is mapped to a classical Heisenberg Hamiltonian, whose parameters are obtained by treating local spin rotations as a perturbation within a Green's-function formalism. The spin and phonon perturbations are connected through the EPC parameters, which enter as lattice-induced perturbations to the tight-binding Hamiltonian. By combining these lattice perturbations with local spin rotations, we obtain real-space derivatives of magnetic exchange parameters without performing displaced magnetic supercell calculations. We illustrate the method on SrMnO$_3$ and show that it can be integrated directly into standard workflows.

cond-mat.mtrl-sci↗

arXiv2026

First-principles electronic transport properties of Ti and Ti-6Al-4V for modeling ultrashort-pulse laser ablation

Predictive modeling of ultrashort-pulse laser ablation requires temperature-dependent material parameters derived from the electronic structure, namely the electronic thermal conductivity, electron--phonon coupling, and heat capacity. These parameters are well documented for elemental metals but remain sparsely documented for alloys, apart from application-relevant exceptions such as stainless steels. The technologically important titanium alloy Ti-6Al-4V is a prominent example, which is still modeled using elemental-titanium values. We compute the electronic transport of hcp Ti and Ti-6Al-4V from first principles, using the Kubo--Greenwood formalism within the Korringa--Kohn--Rostoker coherent-potential-approximation framework, treating chemical and thermal disorder on equal footing. For elemental Ti, the calculated electrical resistivity agrees with independent \textsc{abinit} electron--phonon calculations and experiment, and also reproduces the high-temperature saturation near the Mott--Ioffe--Regel limit. Under electron--phonon nonequilibrium, the electronic thermal conductivity saturates and then decreases with electronic temperature, reaching a maximum of about \SI{2.97}{\kilo\watt\per\metre\per\kelvin} in Ti but only \SI{0.47}{\kilo\watt\per\metre\per\kelvin} in Ti-6Al-4V, a factor of 6.4 lower. In two-temperature-model simulations the alloy and elemental parameter sets yield peak lattice temperatures differing by only about 1.4\%, consistent with reported experimental ablation thresholds that differ by about 3\%, well within their measurement uncertainties. Replacing the first-principles thermal conductivity with the low-temperature Drude limit shifts the peak lattice temperature by up to 19\%, showing that the functional form of the transport model is even more important than the elemental vs alloy distinction for predictive accuracy.

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arXiv2026

Effective Gilbert damping in the stochastic Landau-Lifshitz-Gilbert equation

Quasi particle based (e.g. Boltzmann equation) studies of spin wave transport often assume that their scattering rates follow the simple form $η=αω$, with the Gilbert damping $α$ and frequency $ω$. In this work, we examine the effective damping $α_{eff,T}=η/ω$ observed in atomistic spin dynamics, when temperature and spin wave interactions are introduced for a 1D spin chain. We extract the dynamical correlation functions from spin trajectories propagated using the stochastic Landau-Lifshitz-Gilbert equation, and fit the dynamical structure factor, yielding the dispersion and scattering rates for a wide range of temperatures. The resulting effective damping can be very different from the initially constant Gilbert value. It exhibits a temperature and crystal momentum scaling which we explain based on interactions with the Gilbert bath and spin wave scattering by changes in local magnetic order.

cond-mat.mes-hall↗

arXiv2026

Temperature-dependent Raman spectra of 2H-MoS2 from Machine Learning-driven statistical sampling

Molybdenum sulfides are in the spotlight of materials science thanks to their interesting properties for applications in optoelectronics, nanocomposites, lubricants, and catalysis. The structural characterization of Molybdenum sulfides is a crucial step to understand and tune their properties. Vibrational techniques, such as infrared and Raman spectroscopy, can directly link to structural features, but the experimental literature suffers from large variability. Theoretical calculations are a powerful tool complementing and explaining empirical measurements. The reliability of first-principles calculation depends on the level of approximation made, taking into account disorder, doping, or temperature to yield a good description of the phonon statistics and related measurable quantities, such as the infrared and Raman peaks. In this study we calculate the Raman spectrum of crystalline 2H-MoS2, including broadening and shifts due to thermal and anharmonic effects. Our results demonstrate excellent agreement with experimental measurements; notably, the calculated temperature trends in frequencies and linewidths align with empirical observations. These findings establish a robust computational framework, paving the way for similar studies on amorphous Molybdenum sulfides.

cond-mat.mtrl-sci↗

arXiv2025

Spectroscopy and transport of nonpolarons in silicon and germanium: the influence of doping and temperature

We perform a first-principles investigation of electron-phonon interactions in silicon and germanium, uncovering distinct non-polaronic spectral and transport fingerprints in these archetypal covalent semiconductors. Using many-body perturbation theory with the retarded cumulant expansion, we compute quasiparticle energies, lifetimes, and phonon satellites beyond the Dyson-Migdal approximation. Short-range crystal fields dominate coupling in both materials, yet their low-temperature spectral fingerprints differ: Si exhibits well-resolved satellites at both band edges, whereas Ge displays strong sidebands mainly at the valence band maximum (VBM) and much weaker features at the conduction band minimum (CBM). Phonon-induced satellites in both materials broaden and merge with the quasiparticle peak at elevated temperatures. Doping broadens peaks and compresses satellite-quasiparticle separation, with n-type carriers affecting the CBM and p-type the VBM. Mobility calculations, combining cumulant-derived phonon scattering with experimentally motivated ionized-impurity scattering models, reproduce measured trends and reveal Ge's consistently higher mobilities than Si, stemming from lighter effective masses and weaker coupling. These results link band-edge asymmetries and phonon energetics to measurable transport differences, providing a unified framework for predicting mobility in nonpolar semiconductors.

cond-mat.mtrl-sci↗

arXiv2025

Abinit 2025: New Capabilities for the Predictive Modeling of Solids and Nanomaterials

Abinit is a widely used scientific software package implementing density functional theory and many related functionalities for excited states and response properties. This paper presents the novel features and capabilities, both technical and scientific, which have been implemented over the past 5 years. This evolution occurred in the context of evolving hardware platforms, high-throughput calculation campaigns, and the growing use of machine learning to predict properties based on databases of first principles results. We present new methodologies for ground states with constrained charge, spin or temperature; for density functional perturbation theory extensions to flexoelectricity and polarons; and for excited states in many-body frameworks including GW, dynamical mean field theory, and coupled cluster. Technical advances have extended abinit high-performance execution to graphical processing units and intensive parallelism. Second principles methods build effective models on top of first principles results to scale up in length and time scales. Finally, workflows have been developed in different community frameworks to automate \abinit calculations and enable users to simulate hundreds or thousands of materials in controlled and reproducible conditions.

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arXiv2025

Thermal Conductivity Of Monolayer Hexagonal Boron Nitride: Four-Phonon Scattering And Quantum Sampling Effects

Monolayer hexagonal boron nitride is a prototypical planar 2-dimensional system material and has been the subject of many investigations of its exceptional vibrational, spectroscopic and transport properties. The lattice thermal conductivity remains quite uncertain, with theoretical and experimental reports varying between 218 and 1060 Wm-1K-1. It has a strong temperature evolution and is sensitive to strain effects and isotope concentrations. While the impact of isotope scattering has been widely studied and is well understood, nuclear quantum effects and 4-phonon scattering have so far been neglected. Monolayer hexagonal boron nitride is composed of light elements, and further has its 3-phonon scattering phase space restricted by mirror plane symmetry, so these effects may be of similar order as isotope scattering, and would lead to a completely different understanding of the fundamental processes limiting the lattice thermal conductivity for this system. In this work, we use both classical and path-integral molecular dynamics, in conjunction with the Temperature Dependent Effective Potential method, to compute temperature-dependent renormalized phonons including isotope scattering, 3-phonon scattering, 4-phonon scattering and nuclear quantum effects. We show the impact of the latter two on the lattice thermal conductivity for a large temperature range, as well as their impact on the phonon lifetimes. Overall, our work provides a robust framework for calculations of the lattice thermal conductivity in solids, providing quantitative improvements and physical understanding that help explain the variety of results found in the literature.

cond-mat.mtrl-sci↗

arXiv2025

First-principles calculations of transport coefficients in Weyl semimetal TaAs

We study charge and heat transport from first-principles in the topological Weyl semimetal TaAs. Electron-phonon coupling matrix elements are calculated using density functional perturbation theory and used to derive the thermo-electric transport coefficients, including the electrical conductivity, Seebeck coefficient, electronic thermal conductivity and the Peltier coefficient. We compare the self-energy and momentum relaxation time approximations to the iterative solution of the Boltzmann Transport Equation, finding they give similar results for TaAs provided the chemical potential is treated accurately. For the iterative method, we derive an additional equation, which is needed to fully solve for transport under both thermal and an electrical potential gradients. Interestingly, the Onsager reciprocity between $S$ and $Π$ is no longer imposed, and we can deal with systems breaking time-reversal symmetry, in particular magnetic materials. We compare our results with the available experimental data for TaAs: the agreement is excellent for $σ_{xx}$, while $σ_{zz}$ is overestimated, probably due to differences in experimental carrier concentrations. The Seebeck coefficient is of the same order of magnitude in theory and experiments, and we find that its low-T behavior also strongly depends on the doping level.

cond-mat.mtrl-sci↗

arXiv2025

Fluctuation-dissipation and virtual processes in interacting phonon systems

Phonon-phonon interactions are fundamental to understanding a wide range of material properties, including thermal transport and vibrational spectra. In conventional perturbative approaches, energy conservation during each microscopic phonon interaction is enforced using delta functions. We demonstrate that these delta functions stem from an incomplete treatment, that violates the fluctuation-dissipation theorem governing systems at equilibrium. By replacing delta functions with convolutions and introducing a self-consistency condition for the phonon spectral function, we provide a more accurate and physically consistent framework. For systems where phonon dynamics can be approximated as Markovian, we simplify this approach, reducing the dissipative component to a single parameter tied to phonon lifetimes. Applying this method to boron arsenide, we find that self-consistent linewidths better capture the phonon scattering processes, significantly improving agreement with experimental thermal conductivity values. These results also challenge the conventional view of four-phonon processes as dominant in BAs, demonstrating the adequacy of a three-phonon description, provided it is self-consistent. With this method we address critical limitations of perturbative approaches, offering new insights into dissipation and phonon-mediated processes, and enabling more accurate modeling of anharmonic materials.

cond-mat.mtrl-sci↗

arXiv2025

Electron-mediated anharmonicity and its role in the Raman spectrum of graphene

The Raman active G mode in graphene exhibits strong coupling to electrons, yet the comprehensive treatment of this interaction in the calculation of its temperature-dependent Raman spectrum remains incomplete. In this study, we calculate the temperature dependence of the G mode frequency and linewidth, and successfully explain the experimental trend, by accounting for the contributions arising from the first-order electron-phonon coupling, electron-mediated phonon-phonon coupling, and standard lattice anharmonicity. The generality of our approach enables its broad applicability to study phonon dynamics in materials where both electron-phonon coupling and anharmonicity are important.

cond-mat.mtrl-sci↗

arXiv2025

Mode-coupling formulation of heat transport in anharmonic materials

The temperature-dependent phonons are a generalization of interatomic force constants varying in T, which as found widespread use in computing the thermal transport of materials. A formal justification for using this combination to access thermal conductivity in anharmonic crystals, beyond the harmonic approximation and perturbation theory, is still lacking. In this work, we derive a theory of heat transport of anharmonic crystals, using the mode-coupling theory of anharmonic lattice dynamics. Starting from the Green-Kubo formula, we develop the thermal conductivity tensor based on the system's dynamical susceptibility, or spectral function. Our results account for both the diagonal and off-diagonal contributions of the heat current, with and without collective effects. We implement our theory in the TDEP package, and have notably introduced a Monte Carlo scheme to compute phonon scattering due to third- and fourth-order interactions, achieving a substantial reduction in computational cost which enables full convergence of such calculations for the first time. We apply our methodology to systems with varying regimes of anharmonicity and thermal conductivity to demonstrate its universality. These applications highlight the importance of the phonon renormalizations and their interactions beyond the harmonic order. Overall, our work advances the understanding of thermal conductivity in anharmonic crystals and provides a theoretically robust framework for predicting heat transport in complex materials.

cond-mat.mtrl-sci↗

arXiv2024

Roadmap on Quantum Magnetic Materials

Fundamental research on two-dimensional (2D) magnetic systems based on van der Waals materials has been gaining traction rapidly since their recent discovery. With the increase of recent knowledge, it has become clear that such materials have also a strong potential for applications in devices that combine magnetism with electronics, optics, and nanomechanics. Nonetheless, many challenges still lay ahead. Several fundamental aspects of 2D magnetic materials are still unknown or poorly understood, such as their often-complicated electronic structure, optical properties, and magnetization dynamics, and their magnon spectrum. To elucidate their properties and facilitate integration in devices, advanced characterization techniques and theoretical frameworks need to be developed or adapted. Moreover, developing synthesis methods which increase critical temperatures and achieve large-scale, high-quality homogeneous thin films is crucial before these materials can be used for real-world applications. Therefore, the field of 2D magnetic materials provides many challenges and opportunities for the discovery and exploration of new phenomena, as well as the development of new applications. This Roadmap presents the background, challenges, and potential research directions for various relevant topics in the field on the fundamentals, synthesis, characterization, and applications. We hope that this work can provide a strong starting point for young researchers in the field and provide a general overview of the key challenges for more experienced researchers.

cond-mat.mtrl-sci↗

arXiv2024

Impact of spin-entropy on the thermoelectric properties of a 2D magnet

Heat-to-charge conversion efficiency of thermoelectric materials is closely linked to the entropy per charge carrier. Thus, magnetic materials are promising building blocks for highly efficient energy harvesters, as their carrier entropy is boosted by a spin degree of freedom. In this work, we investigate how this spin entropy impacts heat-to-charge conversion in A-type antiferromagnet CrSBr. We perform simultaneous measurements of electrical conductance and thermocurrent while changing magnetic order using temperature and magnetic field as tuning parameters. We find a strong enhancement of the thermoelectric power factor around the Néel temperature. We further reveal that the power factor at low temperature can be increased by up to 600% upon applying a magnetic field. Our results demonstrate that the thermoelectric properties of 2D magnets can be optimized by exploiting the sizeable impact of spin entropy and confirm thermoelectric measurements as a sensitive tool to investigate subtle magnetic phase transitions in low-dimensional magnets.

cond-mat.mes-hall↗

arXiv2023

Mode-coupling theory of lattice dynamics for classical and quantum crystals

The dynamical properties of nuclei, carried by the concept of phonon quasiparticles (QP), are central to the field of condensed matter. While the harmonic approximation can reproduce a number of properties observed in real crystals, the inclusion of anharmonicity in lattice dynamics is essential to accurately predict properties such as heat transport or thermal expansion. For highly anharmonic systems, non perturbative approaches are needed, which result in renormalized theories of lattice dynamics. In this article, we apply the Mori-Zwanzig projector formalism to derive an exact generalized Langevin equation describing the quantum dynamics of nuclei in a crystal. By projecting this equation on quasiparticles in reciprocal space, and with results from linear response theory, we obtain a formulation of vibrational spectra that fully accounts for the anharmonicity. Using a mode-coupling approach, we construct a systematic perturbative expansion in which each new order is built to minimize the following ones. With a truncation to the lowest order, we show how to obtain a set of self-consistent equations that can describe the lineshapes of quasiparticles. The only inputs needed for the resulting set of equations are the static Kubo correlation functions, which can be computed using (fully quantum) path-integral molecular dynamics or approximated with (classical or ab initio) molecular dynamics. We illustrate the theory with an application on fcc 4He, an archetypal quantum crystal with very strong anharmonicity.

cond-mat.mtrl-sci↗

arXiv2023

Effects of Pressure on the Electronic and Magnetic Properties of Bulk NiI$_{2}$

Transition metal dihalides have recently garnered interest in the context of two-dimensional van der Waals magnets as their underlying geometrically frustrated triangular lattice leads to interesting competing exchange interactions. In particular, NiI$_{2}$ is a magnetic semiconductor that has been long known for its exotic helimagnetism in the bulk. Recent experiments have shown that the helimagnetic state survives down to the monolayer limit with a layer-dependent magnetic transition temperature that suggests a relevant role of the interlayer coupling. Here, we explore the effects of hydrostatic pressure as a means to enhance this interlayer exchange and ultimately tune the electronic and magnetic response of NiI$_{2}$. We study first the evolution of the structural parameters as a function of external pressure using first-principles calculations combined with x-ray diffraction measurements. We then examine the evolution of the electronic structure and magnetic exchange interactions via first-principles calculations and Monte Carlo simulations. We find that the leading interlayer coupling is an antiferromagnetic second-nearest neighbor interaction that increases monotonically with pressure. The ratio between isotropic third- and first-nearest neighbor intralayer exchanges, which controls the magnetic frustration and determines the magnetic propagation vector $\mathbf{q}$ of the helimagnetic ground state, is also enhanced by pressure. As a consequence, our Monte Carlo simulations show a monotonic increase in the magnetic transition temperature, indicating that pressure is an effective means to tune the magnetic response of NiI$_{2}$.

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