arXiv subjects

N. Marzari

Publications and source records attributed to N. Marzari.

At least 19 recordsLinked to original sources

arXiv2025

The Interoperability Challenge in DFT Workflows Across Implementations

Interoperability and cross-validation remains a significant challenge in the computational materials discovery community. In this context, we introduce a common input/output standard designed for internal translation by various workflow managers (AiiDA, PerQueue, Pipeline Pilot, and SimStack) to produce results in a unified schema. This standard aims to enable engine-agnostic workflow execution across multiple density functional theory (DFT) codes, including CASTEP, GPAW, Quantum ESPRESSO, and VASP. As a demonstration, we have implemented a workflow to calculate the open-circuit voltage across several battery cathode materials using the proposed universal input/output schema. We analyze and resolve the challenges of reconciling energetics computed by different DFT engines and document the code-specific idiosyncrasies that make straightforward comparisons difficult. Motivated by these challenges, we outline general design principles for robust automated DFT workflows. This work represents a practical step towards more reproducible and interoperable workflows for high-throughput materials screening, while highlighting challenges of aligning electronic properties, especially for non-pristine structures.

cond-mat.mtrl-sci↗

arXiv2025

Spin structures and phase diagrams of the spin-$\frac{5}{2}$ triangular-lattice antiferromagnet Na$_2$BaMn(PO$_4$)$_2$ under magnetic field

We combine single-crystal neutron diffraction studies and Monte Carlo simulations to determine the spin structures and finite-temperature phase diagram of the spin-5/2 triangular-lattice antiferromagnet Na$_2$BaMn(PO$_4$)$_2$ in magnetic field. With the application of a magnetic field in two different directions, namely along the $c$-axis and in the $ab$-plane of the trigonal symmetry, we track the evolution of the spin structure through changes of the magnetic propagation vector. We account for these results with a minimal Heisenberg Hamiltonian that includes easy-axis anisotropy and weak, frustrated interlayer couplings in addition to intralayer exchange. Guided by representation analysis, we refine symmetry-allowed modes to the measured intensities and obtain the spin structures for all field-induced phases, which we compare quantitatively with simulated configurations. Taken together, our measurements and simulations show that frustrated interlayer exchange -- rather than purely 2D physics -- organizes the unexpectedly rich field-induced phases of Na$_2$BaMn(PO$_4$)$_2$.

cond-mat.str-el↗

arXiv2023

Topological magnons driven by the Dzyaloshinskii-Moriya interaction in the centrosymmetric ferromagnet Mn$_5$Ge$_3$

The phase of the quantum-mechanical wave function can encode a topological structure with wide-ranging physical consequences, such as anomalous transport effects and the existence of edge states robust against perturbations. While this has been exhaustively demonstrated for electrons, properties associated with the elementary quasiparticles in magnetic materials are still underexplored. Here, we show theoretically and via inelastic neutron scattering experiments that the bulk ferromagnet Mn$_5$Ge$_3$ hosts gapped topological Dirac magnons. Although inversion symmetry prohibits a net Dzyaloshinskii-Moriya interaction in the unit cell, it is locally allowed and is responsible for the gap opening in the magnon spectrum. This gap is predicted and experimentally verified to close by rotating the magnetization away from the $c$-axis with an applied magnetic field. Hence, Mn$_5$Ge$_3$ realizes a gapped Dirac magnon material in three dimensions. Its tunability by chemical doping or by thin film nanostructuring defines an exciting new platform to explore and design topological magnons. More generally, our experimental route to verify and control the topological character of the magnons is applicable to bulk centrosymmetric hexagonal materials, which calls for systematic investigation.

cond-mat.str-el↗

arXiv2023

An overview of the spin dynamics of antiferromagnetic Mn$_5$Si$_3$

The metallic compound Mn$_5$Si$_3$ hosts a series of antiferromagnetic phases which can be controlled by external stimuli such as temperature and magnetic field. In this work, we investigate the spin-excitation spectrum of bulk Mn$_5$Si$_3$ by combining inelastic neutron scattering measurements and density functional theory calculations. We study the evolution of the dynamical response under external parameters and demonstrate that the spin dynamics of each phase is robust against any combination of temperature and magnetic field. In particular, the high-energy spin dynamics is very characteristic of the different phases consisting of either spin waves or broad fluctuations patterns.

cond-mat.mtrl-sci↗

arXiv2021

Complex magnetic structure and spin waves of the noncollinear antiferromagnet Mn5Si3

The investigations of the interconnection between micro- and macroscopic properties of materials hosting noncollinear antiferromagnetic ground states are challenging. These forefront studies are crucial for unraveling the underlying mechanisms at play, which may prove beneficial in designing cutting edge multifunctional materials for future applications. In this context, Mn5Si3 has regained scientific interest since it displays an unusual and complex ground state, which is considered to be the origin of the anomalous transport and thermodynamic properties that it exhibits. Here, we report the magnetic exchange couplings of the noncollinear antiferromagnetic phase of Mn5Si3 using inelastic neutron scattering measurements and density functional theory calculations. We determine the ground-state spin configuration and compute its magnon dispersion relations which are in good agreement with the ones obtained experimentally. Furthermore, we investigate the evolution of the spin texture under the application of an external magnetic field to demonstrate theoretically the multiple field-induced phase transitions that Mn5Si3 undergoes. Finally, we model the stability of some of the material's magnetic moments under a magnetic field and we find that very susceptible magnetic moments in a frustrated arrangement can be tuned by the field.

cond-mat.mes-hall↗

arXiv2020

Li4-xGe1-xPxO4 a potential solid-state electrolyte for all-oxide microbatteries

Solid-state electrolytes for Li-ion batteries are attracting growing interest as they allow building safer batteries, also using lithium metal anodes. Here we studied a compound in the lithium superionic conductor (LISICON) family, i.e. Li4-xGe1-xPxO4 (LGPO). Thin films were deposited via pulsed laser deposition and their electrical properties were compared with ceramic pellets. A detailed characterization of the micro structure shows that thin films can be deposited fully crystalline at higher temperatures but also partially amorphous at room temperature. The conductivity is not strongly influenced by the presence of grain boundaries, exposure to air or lithium deficiencies. First-principles molecular dynamics simulations were employed to calculate the lithium ion diffusion profile and the conductivity at various temperatures of the ideal LGPO crystal. Simulations gives the upper limit of conductivity for a defect free crystal, which is in the range of 10-2 S cm-1 at 300 deg. The ease of thin film fabrication, the room-temperature Li-ion conductivity in the range of a few microS cm-1 make LGPO a very appealing electrolyte material for thin film all-solid-state all-oxide microbatteries.

cond-mat.mtrl-sci↗

arXiv2019

Extraordinary high room-temperature carrier mobility in graphene-WSe$_2$ heterostructures

High charge carrier mobilities play a fundamental role for high-frequency electronics, integrated optoelectronics as well as for sensor and spintronic applications, where device performance is directly linked to the magnitude of the carrier mobility. Van der Waals heterostructures formed by graphene and hexagonal boron nitride (hBN) already outperform all known materials in terms of room temperature mobility. Here, we show that the room temperature carrier mobility of today's best graphene/hBN devices can be surpassed by more than a factor of three by heterostructures formed by tungsten diselenide (WSe$_2$), graphene and hBN, which can have mobilities as high as 350,000 cm$^2$/(Vs) and resistivities as low as $15$ Ohm. The resistivity of these devices shows a significantly weaker temperature dependence than the one of graphene on any other known substrate. Notably, the reduced temperature dependence and the resulting mobility enhancement in graphene show an unexpected relation to the thickness of the WSe$_2$ layer and to the minimum conductivity at the charge neutrality point, suggesting a role of increased charge disorder and/or enhanced screening and questioning the current understanding of electron-phonon scattering in graphene-based van der Waals heterostructures.

cond-mat.mes-hall↗

arXiv2019

Bulk and surface electronic structure of the dual-topology semimetal Pt2HgSe3

We report high-resolution angle resolved photoemission measurements on single crystals of Pt2HgSe3 grown by high-pressure synthesis. Our data reveal a gapped Dirac nodal line whose (001)-projection separates the surface Brillouin zone in topological and trivial areas. In the non-trivial $k$-space range we find surface states with multiple saddle-points in the dispersion resulting in two van Hove singularities in the surface density of states. Based on density functional theory calculations, we identify these surface states as signatures of a topological crystalline state which coexists with a weak topological phase.

cond-mat.mtrl-sci↗

arXiv2019

Evidence of large polarons in photoemission band mapping of the perovskite semiconductor CsPbBr$_3$

Lead-halide perovskite (LHP) semiconductors are emergent optoelectronic materials with outstanding transport properties which are not yet fully understood. We find signatures of large polaron formation in the electronic structure of the inorganic LHP CsPbBr$_3$ by means of angle-resolved photoelectron spectroscopy. The experimental valence band dispersion shows a hole effective mass $0.26\pm0.02\,\,m_e$, 50% heavier than the bare mass $m_0 =0.17 m_e$ predicted by density functional theory. Calculations of electron-phonon coupling indicate that phonon dressing of the carriers mainly occurs via distortions of the Pb-Br bond with a Fröhlich coupling parameter $α=1.82$. A good agreement with our experimental data is obtained within the Feynmann polaron model, validating a viable theorical method to predict the carrier effective mass of LHPs ab-initio.

cond-mat.mtrl-sci↗

arXiv2017

Advanced capabilities for materials modelling with Quantum ESPRESSO

Quantum ESPRESSO is an integrated suite of open-source computer codes for quantum simulations of materials using state-of-the art electronic-structure techniques, based on density-functional theory, density-functional perturbation theory, and many-body perturbation theory, within the plane-wave pseudo-potential and projector-augmented-wave approaches. Quantum ESPRESSO owes its popularity to the wide variety of properties and processes it allows to simulate, to its performance on an increasingly broad array of hardware architectures, and to a community of researchers that rely on its capabilities as a core open-source development platform to implement theirs ideas. In this paper we describe recent extensions and improvements, covering new methodologies and property calculators, improved parallelization, code modularization, and extended interoperability both within the distribution and with external software.

cond-mat.mtrl-sci↗

arXiv2015

A generalized Poisson and Poisson-Boltzmann solver for electrostatic environments

The computational study of chemical reactions in complex, wet environments is critical for applications in many fields. It is often essential to study chemical reactions in the presence of applied electrochemical potentials, taking into account the non-trivial electrostatic screening coming from the solvent and the electrolytes. As a consequence the electrostatic potential has to be found by solving the generalized Poisson and the Poisson-Boltzmann equation for neutral and ionic solutions, respectively. In the present work solvers for both problems have been developed. A preconditioned conjugate gradient method has been implemented to the generalized Poisson equation and the linear regime of the Poisson-Boltzmann, allowing to solve iteratively the minimization problem with some ten iterations of a ordinary Poisson equation solver. In addition, a self-consistent procedure enables us to solve the non-linear Poisson-Boltzmann problem. Both solvers exhibit very high accuracy and parallel efficiency, and allow for the treatment of different boundary conditions, as for example surface systems. The solver has been integrated into the BigDFT and Quantum-ESPRESSO electronic-structure packages and will be released as an independent program, suitable for integration in other codes.

cond-mat.mtrl-sci↗

arXiv2014

Projector augmented-wave and all-electron calculations across the periodic table: a comparison of structural and energetic properties

We construct a reference database of materials properties calculated using density-functional theory in the local or generalized-gradient approximation, and an all-electron or a projector augmented-wave (PAW) formulation, for verification and validation of first-principles simulations. All-electron calculations use the full-potential linearised augmented-plane wave method, as implemented in the \texttt{Elk} open-source code, while PAW calculations use the datasets developed by some of us in the open-source \texttt{PSlibrary} repository and the \texttt{Quantum ESPRESSO} distribution. We first calculate lattice parameters, bulk moduli, and energy differences for alkaline metals, alkaline earths, and $3d$ and $4d$ transition metals in three ideal, reference phases (simple cubic, fcc, and bcc), representing a standardized crystalline monoatomic solid-state test. Then, as suggested by K. Lejaeghere {\it et al.}, [Critical Reviews in Solid State and Material Sciences 39, p 1 (2014)], we compare the equations of state for all elements, except lanthanides and actinides, in their experimental phase (or occasionally a simpler, closely related one). PAW and all-electron energy differences and structural parameters agree in most cases within a few meV/atom and a fraction of a percent, respectively. This level of agreement, comparable with the previous study, includes also other PAW and all-electron data from the electronic-structure codes \texttt{VASP} and \texttt{WIEN2K}, and underscores the overall reliability of current, state-of-the-art electronic-structure calculations. At the same time, discrepancies that arise even within the same formulation for simple, fundamental structural properties point to the urgent need of establishing standards for verification and validation, reference data sets, and careful refinements of the computational approaches used.

cond-mat.mtrl-sci↗

arXiv2013

Playing quantum hide-and-seek with the muon: localizing muon stopping sites

One of the most fundamental limitations of a muon-spin relaxation experiment can be the lack of knowledge of the implantation site of the muon and the uncertainty about the muon's perturbation of its host. Here we review some of the work done on the `muon site problem' in the solid state and highlight some recent applications of electronic structure calculations that have successfully characterized the quantum states of muons in a number of insulating compounds containing fluorine, in a number of pnictide superconductors, and in ZnO.

cond-mat.str-el↗

arXiv2013

Quantum states of muons in fluorides

Muon-spin relaxation (μSR) is a sensitive probe of magnetism, but its utility can be severely limited by the lack of knowledge of the muon implantation site and the extent to which the muon perturbs its host. We demonstrate systematically that these problems can be addressed accurately using electronic-structure calculations. We show that diamagnetic muons introduce significant short-ranged distortions in ionic insulators that would lead to systematic errors on magnetic moments determined by μSR, and quantify these. The F--μ--F complex formed by muons in many fluorides can be understood as an exotic molecule-in-a-crystal defect with a zero-point energy larger than that of any naturally-occurring triatomic molecule.

cond-mat.str-el↗

arXiv2011

The Shear Mode of Multi-Layer Graphene

We uncover the interlayer shear mode of multi-layer graphene samples, ranging from bilayer-graphene (BLG) to bulk graphite, and show that the corresponding Raman peak measures the interlayer coupling. This peak scales from~43cm-1 in bulk graphite to~31cm-1 in BLG. Its low energy makes it a probe of near-Dirac point quasi-particles, with a Breit-Wigner-Fano lineshape due to resonance with electronic transitions. Similar shear modes are expected in all layered materials, providing a direct probe of interlayer interactions

cond-mat.mes-hall↗

arXiv2010

Towards First-principles Electrochemistry

Chemisorbed molecules at a fuel cell electrode are a very sensitive probe of the surrounding electrochemical environment, and one that can be accurately monitored with different spectroscopic techniques. We develop a comprehensive electrochemical model to study molecular chemisorption at either constant charge or fixed applied voltage, and calculate from first principles the voltage dependence of vibrational frequencies -- the vibrational Stark effect -- for CO adsorbed on close-packed platinum electrodes. The predicted vibrational Stark slopes are found to be in very good agreement with experimental electrochemical spectroscopy data, thereby resolving previous controversies in the quantitative interpretation of in-situ experiments and elucidating the relation between canonical and grand-canonicaldescriptions of vibrational surface phenomena.

cond-mat.mtrl-sci↗

arXiv2010

An ab-initio converse NMR approach for pseudopotentials

We extend the recently developed converse NMR approach [T. Thonhauser, D. Ceresoli, A. Mostofi, N. Marzari, R. Resta, and D. Vanderbilt, J. Chem. Phys. \textbf{131}, 101101 (2009)] such that it can be used in conjunction with norm-conserving, non-local pseudopotentials. This extension permits the efficient ab-initio calculation of NMR chemical shifts for elements other than hydrogen within the convenience of a plane-wave pseudopotential approach. We have tested our approach on several finite and periodic systems, finding very good agreement with established methods and experimental results.

cond-mat.mtrl-sci↗

arXiv2009

NMR shifts for polycyclic aromatic hydrocarbons from first-principles

We present first-principles, density-functional theory calculations of the NMR chemical shifts for polycyclic aromatic hydrocarbons, starting with benzene and increasing sizes up to the one- and two-dimensional infinite limits of graphene ribbons and sheets. Our calculations are performed using a combination of the recently developed theory of orbital magnetization in solids, and a novel approach to NMR calculations where chemical shifts are obtained from the derivative of the orbital magnetization with respect to a microscopic, localized magnetic dipole. Using these methods we study on equal footing the $^1$H and $^{13}$C shifts in benzene, pyrene, coronene, in naphthalene, anthracene, naphthacene, and pentacene, and finally in graphene, graphite, and an infinite graphene ribbon. Our results show very good agreement with experiments and allow us to characterize the trends for the chemical shifts as a function of system size.

cond-mat.mtrl-sci↗