arXiv subjects

Marco Bernardi

Publications and source records attributed to Marco Bernardi.

At least 19 recordsLinked to original sources

arXiv2026

Strain-Tunable Spin Relaxation in Germanium from First Principles

Germanium is a leading platform for semiconductor spin qubits and spintronics. Yet its electron and hole spin dynamics remain understood primarily through phenomenological models. Here, we predict electronic transport and spin relaxation in bulk Ge entirely from first principles, combining hybrid-functional band structures with fully relativistic electron-phonon ($e$-ph) interactions. Without empirical parameters, we predict carrier mobilities, velocity-field curves, and electron and hole spin relaxation times in close agreement with experiments over 100$-$400 K. By resolving spin-flip scattering by valley and phonon mode, we identify the microscopic mechanisms governing spin relaxation and show that spin and momentum relaxation, although both mediated by $e$-ph scattering, are controlled by distinct processes. We further show that compressive biaxial strain enhances the hole spin lifetime by up to two orders of magnitude at 5% strain, through strain-induced valence-band splitting and suppressed spin mixing. This mechanism is directly relevant to Ge-on-Si devices, where strain provides a practical route to engineering long-lived hole spins for quantum technologies.

cond-mat.mtrl-sci↗

arXiv2026

Predicting electron-phonon coupling and electronic transport at the moir\'e scale in twisted bilayer graphene

First-principles calculations can accurately describe electron-phonon (e-ph) interactions and electronic transport in a wide range of materials, but are currently limited to unit cells with up to $\sim$100 atoms due to computational cost. Here, we develop an atomistic electronic potential with Holstein- and Peierls-like terms for modeling e-ph interactions and phonon-limited electronic transport that enables the study of moir\'e systems with thousands of atoms per unit cell. This method can accurately reproduce first-principles e-ph coupling and resistivity in graphene and large-angle twisted bilayer graphene (TBG). Using this approach, we study TBG over a range of twist angles down to 1.6$^\circ$ (5044-atom unit cell), and report the evolution of e-ph interactions and phonon-limited resistivity with twist angle. The predicted resistivity increases by two orders of magnitude between 13.2$^\circ$ and 1.6$^\circ$, driven by the progressive reduction of the electronic energy scale. Our calculations can predict key experimental trends in 2.0$^\circ$ and 1.6$^\circ$ TBG, including the resistivity and its dependence on temperature and band filling. Our work establishes a scalable approach for quantitative studies of e-ph interactions and transport in moir\'e materials and other systems with previously inaccessible length scales.

cond-mat.mtrl-sci↗

arXiv2025

Quantum Period-Finding using One-Qubit Reduced Density Matrices

The quantum period-finding (QPF) algorithm can compute the period of a function exponentially faster than the best-known classical algorithm. In standard QPF, the output state has a primary contribution from $r$ high-probability bit strings, where $r$ is the period. Measurement of this state, combined with continued fraction analysis, reveals the unknown period. Here, we explore a different approach to QPF, where the period is obtained from single-qubit quantities $-$ specifically, the set of one-qubit reduced density matrices (1-RDMs) $-$ rather than the output bit strings of the entire quantum circuit. Using state-vector simulations, we compute the 1-RDMs of the QPF circuit for a generic periodic function. Analysis of these 1-RDMs as a function of period reveals distinctive patterns, which allows us to obtain the unknown period from the 1-RDMs using a numerical root-finding approach. Our results show that the 1-RDMs $-$ a set of $O(n)$ one-qubit marginals $-$ contain enough information to reconstruct the period, which is typically obtained by sampling the space of $O(2^n)$ bit strings. Conceptually, this can be viewed as a "compression" of the information in the QPF algorithm, which enables period-finding from $n$ one-qubit marginals. Our results motivate the development of approximate simulations of reduced density matrices to design novel period-finding algorithms.

quant-ph↗

arXiv2025

Efficient GPU Parallelization of Electronic Transport and Nonequilibrium Dynamics from Electron-Phonon Interactions in the Perturbo Code

The Boltzmann transport equation (BTE) with electron-phonon (e-ph) interactions computed from first principles is widely used to study electronic transport and nonequilibrium dynamics in materials. Calculating the e-ph collision integral is the most important step in the BTE, but it remains computationally costly, even with current MPI+OpenMP parallelization. This challenge makes it difficult to study materials with large unit cells and to achieve high resolution in momentum space. Here, we show acceleration of BTE calculations of electronic transport and ultrafast dynamics using graphical processing units (GPUs). We implement a novel data structure and algorithm, optimized for GPU hardware and developed using OpenACC, to process scattering channels and efficiently compute the collision integral. This approach significantly reduces the overhead for data referencing, movement, and synchronization. Relative to the efficient CPU implementation in the open-source package Perturbo (v2.2.0), used as a baseline, this approach achieves a speed-up of 40 times for both transport and nonequilibrium dynamics on GPU hardware, and achieves nearly linear scaling up to 100 GPUs. The novel data structure can be generalized to other electron interactions and scattering processes. We released this GPU implementation in the latest public version (v3.0.0) of Perturbo. The new MPI+OpenMP+GPU parallelization enables sweeping studies of e-ph physics and electron dynamics in conventional and quantum materials, and prepares Perturbo for exascale supercomputing platforms.

cond-mat.mtrl-sci↗

arXiv2025

Magnetotransport in Topological Materials and Nonlinear Hall Effect via First-Principles Electronic Interactions and Band Topology

Topological effects arising from the Berry curvature lead to intriguing transport signatures in quantum materials. Two such phenomena are the chiral anomaly and nonlinear Hall effect (NLHE). A unified description of these transport regimes requires a quantitative treatment of both band topology and electron scattering. Here, we show accurate predictions of the magnetoresistance in topological semimetals and NLHE in noncentrosymmetric materials by solving the Boltzmann transport equation (BTE) with electron-phonon ($e$-ph) scattering and Berry curvature computed from first principles. We apply our method to study magnetotransport in a prototypical Weyl semimetal, TaAs, and the NLHE in strained monolayer WSe$_2$, bilayer WTe$_2$ and bulk BaMnSb$_2$. In TaAs, we find a chiral contribution to the magnetoconductance which is positive and increases with magnetic field, consistent with experiments. We show that $e$-ph interactions can significantly modify the Berry curvature dipole and its dependence on temperature and Fermi level, highlighting the interplay of band topology and electronic interactions in nonlinear transport. The computed nonlinear Hall response in BaMnSb$_2$ is in agreement with experiments. By adding the Berry curvature to first-principles transport calculations, our work advances the quantitative analysis of a wide range of linear and nonlinear transport phenomena in quantum materials.

cond-mat.mtrl-sci↗

arXiv2025

Ab initio Maxwell-Bloch Approach for X-Ray Excitations in Two-Dimensional Materials

The combination of Maxwell and X-ray Bloch equations forms an appropriate framework to describe ultrafast time-resolved X-ray experiments on attosecond time scale in crystalline solids. However, broadband experiments such as X-ray absorption near edge spectroscopy or resonant inelastic X-ray scattering require a detailed knowledge of the electronic structure and transition matrix elements. Here, we show how to fill this gap by combining the Maxwell-X-ray Bloch formalism with first-principles calculations treating explicitly the core states. The resulting X-ray absorption spectrum recovers key spectral signatures which were missing in our previous work relying on a semi-empirical tight-binding approach.

cond-mat.mtrl-sci↗

arXiv2025

Tensor Learning and Compression of N-phonon Interactions

Phonon interactions from lattice anharmonicity govern thermal properties and heat transport in materials. These interactions are described by n-th order interatomic force constants (n-IFCs), which can be viewed as high-dimensional tensors correlating the motion of n atoms, or equivalently encoding n-phonon scattering processes in momentum space. Here, we introduce a tensor decomposition to efficiently compress n-IFCs for arbitrary order n. Using tensor learning, we find optimal low-rank approximations of n-IFCs by solving the resulting optimization problem. Our approach reveals the inherent low dimensionality of phonon-phonon interactions and allows compression of the 3 and 4-IFC tensors by factors of up to $10^3-10^4$ while retaining high accuracy in calculations of phonon scattering rates and thermal conductivity. Calculations of thermal conductivity using the compressed n-IFCs achieve a speed-up by nearly three orders of magnitude with >98% accuracy relative to the reference uncompressed solution. These calculations include both 3- and 4-phonon scattering and are shown for a diverse range of materials (Si, HgTe, MgO, TiNiSn and monoclinic ZrO$_2$). In addition to accelerating state-of-the-art thermal transport calculations, the method shown here paves the way for modeling strongly anharmonic materials and higher-order phonon interactions.

cond-mat.mtrl-sci↗

arXiv2025

Magnons in chromium trihalides from \emph{ab initio} Bethe-Salpeter equation

Chromium trihalides (CrX$_3$, with $\rm{X=I,Br,Cl}$) are layered ferromagnetic materials with rich physics and possible applications. Their structure consists of magnetic Cr atoms positioned between two layers of halide atoms. The choice of halide results in distinct magnetic properties, but their effect on spin-wave (magnon) excitations is not fully understood. Here we present first-principles calculations of magnon dispersions and wave functions for monolayer Cr trihalides using the finite-momentum Bethe-Salpeter equation (BSE) to describe collective spin-flip excitations. % We study the dependence of magnon dispersions on the halide species and resolve the small topological gap at the Dirac point in the magnon spectrum by including spin-orbit coupling. Analysis of magnon wave functions reveals that magnons are made up of electronic transitions with a wider energy range than excitons in CrX$_3$ monolayers, providing insight into magnon states in real and reciprocal space. We discuss Heisenberg exchange parameters extracted from the BSE and discuss the convergence of BSE magnon calculations. Our work advances the quantitative modeling of magnons in two-dimensional materials, providing the starting point for studying magnon interactions in a first-principles BSE framework.

cond-mat.mtrl-sci↗

arXiv2025

Magnon-phonon interactions from first principles

Modeling spin-wave (magnon) dynamics in novel materials is important to advance spintronics and spin-based quantum technologies. The interactions between magnons and lattice vibrations (phonons) limit the length scale for magnon transport. However, quantifying these interactions remains challenging. Here we show many-body calculations of magnon-phonon (mag-ph) coupling based on the ab initio Bethe-Salpeter equation. We derive expressions for mag-ph coupling matrices and compute them in 2D ferromagnets, focusing on hydrogenated graphene and monolayer CrI3. Our analysis shows that electron-phonon (e-ph) and mag-ph interactions differ significantly, where modes with weak e-ph coupling can exhibit strong mag-ph coupling (and vice versa), and reveals which phonon modes couple more strongly with magnons. In both materials studied here, the inelastic magnon relaxation time is found to decrease abruptly above the threshold for emission of strongly coupled phonons, thereby defining a low-energy window for efficient magnon transport. By averaging in this window, we compute the temperature-dependent magnon mean-free path, a key figure of merit for spintronics, entirely from first principles. The theory and computational tools shown in this work enable studies of magnon interactions, scattering, and dynamics in generic materials, advancing the design of magnetic systems and magnon- and spin-based devices.

cond-mat.mtrl-sci↗

arXiv2024

Advancing Simulations of Coupled Electron and Phonon Nonequilibrium Dynamics Using Adaptive and Multirate Time Integration

Electronic structure calculations in the time domain provide a deeper understanding of nonequilibrium dynamics in materials. The real-time Boltzmann equation (rt-BTE), used in conjunction with accurate interactions computed from first principles, has enabled reliable predictions of coupled electron and lattice dynamics. However, the timescales and system sizes accessible with this approach are still limited, with two main challenges being the different timescales of electron and phonon interactions and the cost of computing collision integrals. As a result, only a few examples of these calculations exist, mainly for two-dimensional (2D) materials. Here we leverage adaptive and multirate time integration methods to achieve a major step forward in solving the coupled rt-BTEs for electrons and phonons. Relative to conventional (non-adaptive) time-stepping, our approach achieves a 10x speedup for a given target accuracy, or greater accuracy by 3-6 orders of magnitude for the same computational cost, enabling efficient calculations in both 2D and bulk materials. This efficiency is showcased by computing the coupled electron and lattice dynamics in graphene up to $\sim$100 ps, as well as modeling ultrafast lattice dynamics and thermal diffuse scattering maps in a bulk material (silicon). These results open new opportunities for quantitative studies of nonequilibrium physics in materials.

cond-mat.mtrl-sci↗

arXiv2024

Deep-ultraviolet transparent conducting SrSnO3 via heterostructure design

Exploration and advancements in ultra-wide bandgap (UWBG) semiconductors are pivotal for next-generation high-power electronics and deep-ultraviolet (DUV) optoelectronics. A critical challenge lies in finding a semiconductor that is highly transparent to DUV wavelengths yet conductive with high mobility at room temperature. Here, we achieved both high transparency and high conductivity by employing a thin heterostructure design. The heterostructure facilitated high conductivity by screening phonons using free carriers, while the atomically thin films ensured high transparency. We utilized a heterostructure comprising SrSnO3/La:SrSnO3/GdScO3 (110) and applied electrostatic gating to effectively separate electrons from their dopant atoms. This led to a modulation of carrier density from 1018 cm-3 to 1020 cm-3, with room temperature mobilities ranging from 40 to 140 cm2V-1s-1. The phonon-limited mobility, calculated from first principles, closely matched experimental results, suggesting that room-temperature mobility could be further increased with higher electron density. Additionally, the sample exhibited 85% optical transparency at a 300 nm wavelength. These findings highlight the potential of heterostructure design for transparent UWBG semiconductor applications, especially in deep-ultraviolet regime.

cond-mat.mtrl-sci↗

arXiv2024

Respective Roles of Electron-Phonon and Electron-Electron Interactions in the Transport and Quasiparticle Properties of SrVO$_3$

The spectral and transport properties of strongly correlated metals, such as SrVO$_3$ (SVO), are widely attributed to electron-electron ($e$-$e$) interactions, with lattice vibrations (phonons) playing a secondary role. Here, using first-principles electron-phonon ($e$-ph) and dynamical mean field theory calculations, we show that $e$-ph interactions play an essential role in SVO: they govern the electron scattering and resistivity in a wide temperature range above 30 K, and induce an experimentally observed kink in the spectral function. In contrast, the $e$-$e$ interactions control quasiparticle renormalizations and low temperature transport, and enhance the $e$-ph coupling. We clarify the origin of the near $T^2$ temperature dependence of the resistivity by analyzing the $e$-$e$ and $e$-ph limited transport regimes. Our work disentangles the electronic and lattice degrees of freedom in a prototypical correlated metal, revealing the dominant role of $e$-ph interactions in SVO.

cond-mat.mtrl-sci↗

arXiv2024

First-principles electron-phonon interactions and electronic transport in large-angle twisted bilayer graphene

Twisted bilayer graphene (tBLG) has emerged as an exciting platform for novel condensed matter physics. However, electron-phonon ($e$-ph) interactions in tBLG and their effects on electronic transport are not completely understood. Here we show first-principles calculations of $e$-ph interactions and resistivity in commensurate tBLG with large twist angles of 13.2 and 21.8 degrees. These calculations overcome key technical barriers, including large unit cells of up to 76 atoms, Brillouin-zone folding of the $e$-ph interactions, and unstable lattice vibrations due to the AA-stacked domains. We show that $e$-ph interactions due to layer-breathing (LB) phonons enhance intervalley scattering in large-angle tBLG. This interaction effectively couples the two layers, which are otherwise electronically decoupled at such large twist angles. As a result, the phonon-limited resistivity in tBLG deviates from the temperature-linear trend characteristic of monolayer graphene and tBLG near the magic angle. Taken together, our work quantifies $e$-ph interactions and scattering mechanisms in tBLG, revealing subtle interlayer coupling effects at large twist angles.

cond-mat.mtrl-sci↗

arXiv2024

Data-driven compression of electron-phonon interactions

First-principles calculations of electron interactions in materials have seen rapid progress in recent years, with electron-phonon (e-ph) interactions being a prime example. However, these techniques use large matrices encoding the interactions on dense momentum grids, which reduces computational efficiency and obscures interpretability. For e-ph interactions, existing interpolation techniques leverage locality in real space, but the high dimensionality of the data remains a bottleneck to balance cost and accuracy. Here we show an efficient way to compress e-ph interactions based on singular value decomposition (SVD), a widely used matrix / image compression technique. Leveraging (un)constrained SVD methods, we accurately predict material properties related to e-ph interactions - including charge mobility, spin relaxation times, band renormalization, and superconducting critical temperature - while using only a small fraction (1-2%) of the interaction data. These findings unveil the hidden low-dimensional nature of e-ph interactions. Furthermore, they accelerate state-of-the-art first-principles e-ph calculations by about two orders of magnitudes without sacrificing accuracy. Our Pareto-optimal parametrization of e-ph interactions can be readily generalized to electron-electron and electron-defect interactions, as well as to other couplings, advancing quantitative studies of condensed matter.

cond-mat.mtrl-sci↗

arXiv2024

First-Principles Electron-Phonon Interactions and Polarons in the Parent Cuprate La$_2$CuO$_4$

Understanding electronic interactions in high-temperature superconductors is an outstanding challenge. In the widely studied cuprate materials, experimental evidence points to strong electron-phonon ($e$-ph) coupling and broad photoemission spectra. Yet, the microscopic origin of this behavior is not fully understood. Here we study $e$-ph interactions and polarons in a prototypical parent (undoped) cuprate, La$_2$CuO$_4$ (LCO), by means of first-principles calculations. Leveraging parameter-free Hubbard-corrected density functional theory, we obtain a ground state with band gap and Cu magnetic moment in nearly exact agreement with experiments. This enables a quantitative characterization of $e$-ph interactions. Our calculations reveal two classes of longitudinal optical (LO) phonons with strong $e$-ph coupling to hole states. These modes consist of Cu-O plane bond-stretching and bond-bending as well as vibrations of apical O atoms. The hole spectral functions, obtained with a cumulant method that can capture strong $e$-ph coupling, exhibit broad quasiparticle peaks with a small spectral weight ($Z\approx0.25$) and pronounced LO-phonon sidebands characteristic of polaron effects. Our calculations predict features observed in photoemission spectra, including a 40-meV peak in the $e$-ph coupling distribution function not explained by existing models. These results show that the universal strong $e$-ph coupling found experimentally in lanthanum cuprates is an intrinsic feature of the parent compound, and elucidates its microscopic origin.

cond-mat.mtrl-sci↗

arXiv2024

Hard X-ray Generation and Detection of Nanometer-Scale Localized Coherent Acoustic Wave Packets in SrTiO$_3$ and KTaO$_3$

We demonstrate that the absorption of femtosecond x-ray pulses can excite quasi-spherical high-wavevector coherent acoustic phonon wavepackets using an all x-ray pump and probe scattering experiment. The time- and momentum-resolved diffuse scattering signal is consistent with strain pulses induced by the rapid electron cascade dynamics following photoionization at uncorrelated excitation centers. We quantify key parameters of this process, including the localization size of the strain wavepacket and the energy absorption efficiency, which are determined by the photoelectron and Auger electron cascade dynamics, as well as the electron-phonon interaction. In particular, we obtain the localization size of the observed strain wave packet to be 1.5 and 2.5 nm for bulk SrTiO$_3$ and KTaO$_3$ single crystals, even though there are no nanoscale structures or light-intensity patterns that would ordinarily be required to generate acoustic waves of wavelengths much shorter than the penetration depth. Whereas in GaAs and GaP we do not observe a signal above background. The results provide crucial information on x-ray matter interactions, which sheds light on the mechanism of x-ray energy deposition, and the study of high wavevector acoustic phonons and thermal transport at the nanoscale.

cond-mat.mtrl-sci↗

arXiv2023

Dynamic mode decomposition of nonequilibrium electron-phonon dynamics: accelerating the first-principles real-time Boltzmann equation

Nonequilibrium dynamics governed by electron-phonon (e-ph) interactions plays a key role in electronic devices and spectroscopies and is central to understanding electronic excitations in materials. The real-time Boltzmann transport equation (rt-BTE) with collision processes computed from first principles can describe the coupled dynamics of electrons and atomic vibrations (phonons). Yet, a bottleneck of these simulations is the calculation of e-ph scattering integrals on dense momentum grids at each time step. Here we show a data-driven approach based on dynamic mode decomposition (DMD) that can accelerate the time propagation of the rt-BTE and identify dominant electronic processes. We apply this approach to two case studies, high-field charge transport and ultrafast excited electron relaxation. In both cases, simulating only a short time window of ~10% of the dynamics suffices to predict the dynamics from initial excitation to steady state using DMD extrapolation. Analysis of the momentum-space modes extracted from DMD sheds light on the microscopic mechanisms governing electron relaxation to steady state or equilibrium. The combination of accuracy and efficiency makes our DMD-based method a valuable tool for investigating ultrafast dynamics in a wide range of materials.

cond-mat.mtrl-sci↗

arXiv2023

Combining Electron-Phonon and Dynamical Mean-Field Theory Calculations of Correlated Materials: Transport in the Correlated Metal Sr$_2$RuO$_4$

Electron-electron ($e$-$e$) and electron-phonon ($e$-ph) interactions are challenging to describe in correlated materials, where their joint effects govern unconventional transport, phase transitions, and superconductivity. Here we combine first-principles $e$-ph calculations with dynamical mean field theory (DMFT) as a step toward a unified description of $e$-$e$ and $e$-ph interactions in correlated materials. We compute the $e$-ph self-energy using the DMFT electron Green's function, and combine it with the $e$-$e$ self-energy from DMFT to obtain a Green's function including both interactions. This approach captures the renormalization of quasiparticle dispersion and spectral weight on equal footing. Using our method, we study the $e$-ph and $e$-$e$ contributions to the resistivity and spectral functions in the correlated metal Sr$_2$RuO$_4$. In this material, our results show that $e$-$e$ interactions dominate transport and spectral broadening in the temperature range we study (50$-$310~K), while $e$-ph interactions are relatively weak and account for only $\sim$10\% of the experimental resistivity. We also compute effective scattering rates, and find that the $e$-$e$ interactions result in scattering several times greater than the Planckian value $k_BT$, whereas $e$-ph interactions are associated with scattering rates lower than $k_BT$. Our work demonstrates a first-principles approach to combine electron dynamical correlations from DMFT with $e$-ph interactions in a consistent way, advancing quantitative studies of correlated materials.

cond-mat.mtrl-sci↗