arXiv subjects

Sinéad M. Griffin

Publications and source records attributed to Sinéad M. Griffin.

At least 19 recordsLinked to original sources

arXiv2026

Atomic-scale control of substrate-spin coupling via vertical manipulation of a 2D metal-organic framework

Two-dimensional (2D) materials with frustrated crystal geometries can host strongly correlated electrons, potentially leading to a range of exotic many-body quantum phases such as Mott insulators, quantum spin-liquids, and Kondo lattices. The ability to control exchange-coupling within these systems is therefore highly desirable. Here, we use an atomically sharp scanning tunneling microscope probe to vertically manipulate a 2D Mott insulating kagome metal-organic framework (MOF) featuring Kondo-screened local magnetic moments on Ag(111). We show that by controlling the adsorption height of the MOF, we can also controllably and reversibly change the strength of Kondo coupling between the MOF's local spins and the substrate's conduction electrons. This mechanical control of Kondo coupling could be extended to other forms of interlayer exchange coupling, potentially allowing for atomic-scale design or control of spintronics technologies.

cond-mat.str-el↗

arXiv2026

Relativistic and nonrelativistic spin splitting above and below the Fermi level in a $g$-wave altermagnet

Nonrelativistic spin splitting (NRSS) challenges conventional wisdom about antiferromagnets by allowing spin-split electronic bands even in collinear orders with zero net magnetization. This sub-class of antiferromagnets, recently dubbed "altermagnets," enforces distinctive spin textures via spin-group symmetries in the crystal. However, direct experimental evidence for such symmetry-driven magnetism remains scarce, and distinguishing it from relativistic spin splitting presents additional challenges. Here, we combine first-principles calculations, symmetry analysis, and two spin-resolved spectroscopies--angle-resolved photoemission (spin-ARPES) and our newly developed spin- and angle-resolved electron reflection spectroscopy (spin-ARRES)--to achieve the first complete momentum-resolved mapping of relativistic (RSS) and nonrelastivistic (NRSS) spin splitting in CoNb$_4$Se$_8$. By probing both the occupied (spin-ARPES) and unoccupied (spin-ARRES) electronic states in a single experiment, we uncover a series of momentum-dependent spin splitting phenomena each of which switch sign under sixfold rotations and persists far above and below the Fermi level. Crucially, distinct nodal planes in momentum space distinguish NRSS from RSS features. Additionally, the observed collapse of NRSS and the persistence of RSS above the Néel temperature, distinguishes a genuine magnetic phase transition from inversion symmetry breaking. Our work demonstrates, for the first time, the combined power of spin-ARPES and spin-ARRES in capturing the full spin texture across an extended energy range, positioning CoNb$_4$Se$_8$ as a prototype for exploring spin-group-based phenomena. These findings open new routes for engineering spin-based functionalities ranging from neuromorphic computing to unconventional superconductivity in layered antiferromagnets.

cond-mat.mtrl-sci↗

arXiv2026

Discovery of a new weberite-type antiferroelectric: La3NbO7

Antiferroelectrics are antipolar materials which possess an electric field-induced phase transition to a polar, ferroelectric phase and offer significant potential for sensing/actuation and energy-storage applications. Known antiferroelectrics are relatively scarce and mainly based on a limited set of perovskite materials and their alloys (e.g., PbZrO$_3$, AgNbO$_3$, NaNbO$_3$). Here, a new family of lead-free, weberite-type antiferroelectrics, identified through a large-scale, first-principles computational search is introduced. The screening methodology, which connects lattice dynamics to antipolar distortions, predicted that La$_3$NbO$_7$ could exhibit antiferroelectricity. We confirm the prediction through the synthesis and characterization of epitaxial La$_3$NbO$_7$ thin films, which display the signature double hysteresis loops of an antiferroelectric material as well as clear evidence of an antipolar ground state structure from transmission electron microscopy. The antiferroelectricity in La$_3$NbO$_7$ is simpler than most known antiferroelectrics and can be explained by a Kittel-type mechanism involving the movement of niobium atoms in an oxygen octahedron through a single phonon mode which results in a smaller change in the volume during the field-induced phase transition. Additionally, it is found that La$_3$NbO$_7$ combines a high threshold field with a high breakdown field ($\approx$ 6MV/cm) - which opens up opportunities for energy-storage applications. This new weberite-type family of materials offers many opportunities to tune electrical and temperature response especially through substitutions on the rare-earth site. Ultimately, this work demonstrates a successful data-driven theory-to-experiment discovery of an entirely new family of antiferroelectrics and provides a blueprint for the future design of ferroic materials.

cond-mat.mtrl-sci↗

arXiv2025

Engineering micromotion in Floquet prethermalization via space-time symmetries

We present a systematic framework for Floquet prethermalization under strong resonant driving, emphasizing the pivotal role of dynamical space-time symmetries. Our approach demonstrates how dynamical space-time symmetries map onto the projective static symmetry group of the prethermal Hamiltonian governing the prethermal regime. We introduce techniques for detecting dynamical symmetries through the time evolution of local observables, facilitating a detailed analysis of micromotion within each period and surpassing the limitations of conventional stroboscopic Floquet prethermal dynamics. To implement this framework, we present a prethermal protocol that preserves order-two dynamical symmetry in a spin-ladder model, confirming the predicted relationships between the expectation values of local observables at distinct temporal points in the Floquet cycle, linked by this symmetry.

quant-ph↗

arXiv2025

Twin-boundary-induced nonrelativistic spin splitting

Nonrelativistic spin splitting (NRSS) in compensated magnetic materials is drawing considerable attention due to its potential impact in next-generation spintronic devices. While NRSS is typically restricted to materials with particular symmetry constraints, here we demonstrate, using density functional theory (DFT) and tight-binding transport calculations, that twin boundaries can induce NRSS in magnetic systems where it is otherwise forbidden. We focus on two representative material systems: the tetragonal perovskite oxide BiCoO$_3$ with $90^{\circ}$ ferroelastic domain walls, and the rhombohedral layered delafossite-type oxide CoO$_2$, supporting $71^{\circ}$, $109^{\circ}$, and $135^{\circ}$ twin boundaries. Our results reveal that, if these boundaries coexist with ferromagnetic domain walls, they consistently produce NRSS similar to that of d-wave altermagnets, with nodal surfaces dictated by the underlying symmetry of the supercell containing the twin boundary. Tight-binding models further elucidate how the NRSS and derived transport properties scale with domain size and density. Our results put forward twin boundary engineering as a versatile route to realize and control spin splitting in a broader class of materials.

cond-mat.mtrl-sci↗

arXiv2025

First High-Throughput Evaluation of Dark Matter Detector Materials

We perform the first high-throughput search and evaluation of materials that can serve as excellent low-mass dark matter detectors. Using properties of close to one thousand materials from the Materials Project database, we project the sensitivity in dark matter parameter space for experiments constructed from each material, including both absorption and scattering processes between dark matter and electrons. Using the anisotropic materials in the dataset, we further compute the level of daily modulation in interaction rates and the resulting directional sensitivities, highlighting materials with prospects to detect the dark matter wind. Our methods provide the basic tools for the data-driven design of dark matter detectors, and our findings lay the groundwork for the next generation of highly optimized direct searches for dark matter as light as the keV scale.

hep-ph↗

arXiv2025

First principles computations of the Stark shift of a defect-bound exciton: the case of the T center in silicon

The T center in silicon has recently drawn a lot of attention for its potential in quantum information science. The sensitivity of the zero-phonon line (ZPL) to electrical field was recently investigated by a combination of different experimental methods but there is still no first principles study on the Stark shift of the T center. Dealing with the defect-bound exciton nature of the excited state is particularly challenging using density functional theory because of the large spatial delocalization associated with the wavefunction. Here, we tackle this issue by performing a convergence study over the supercell size. We obtain an exciton binding energy of 28.5meV, in good agreement with experimental results. We then calculate the Stark shift through the dipole moment change of the ZPL transition of the T center using the modern theory of polarization formalism and find a modest linear coefficient of $Δμ$=0.79D along X and $Δμ$=0.03D along Y. We discuss our results in light of the recent experimental measurements of the Stark shift. Our analysis suggests that bound-exciton defects could be particularly sensitive to local field effect as a result of their large spatial extent.

cond-mat.mtrl-sci↗

arXiv2025

Symmetries of all lines in monolayer crystals

As "2D" materials (i.e. materials just a few atoms thick) continue to gain prominence, understanding their symmetries is critical for unlocking their full potential. In this work, we present comprehensive tables that tabulate the rod group symmetries of all crystallographic lines in all 80 layer groups, which describe the symmetries of 2D materials. These tables are analogous to the scanning tables for space groups found in Volume E of the International Tables for Crystallography, but are specifically tailored for layer groups and their applications to 2D materials. This resource will aid in the analysis of line defects, such as domain walls, which play a crucial role in determining the properties and functionality of 2D materials.

cond-mat.mtrl-sci↗

arXiv2025

Identifying high performance spectrally-stable quantum defects in diamond

Point defects in semiconductors are becoming central to quantum technologies. They can be used as spin qubits interfacing with photons, which are fundamental for building quantum networks. Currently, the most prominent quantum defect in diamond is the nitrogen-vacancy (NV) center. However, it suffers from spectral diffusion that negatively impacts optical coherence and is due to the coupling of the emission energy with uncontrolled electric fields. The group IV vacancy complexes on the other hand have shown to be significantly more spectrally-stable as they are centrosymmetric and thus immune to the linear Stark shift. They however suffer from several issues ranging from low operation temperature to low optical efficiency due to dark states and difficulty in stabilizing the right defect charge state. Here we search for alternative to the group IV vacancy complex in diamond by systematically evaluating all possible vacancy complex using high-throughput first-principles computational screening. We identify the defects that combine centrosymmetry, emission in the visible range, as well as favorable and achievable electronic structure promoting higher operation temperature and defect levels well within the band gap. We find Zn$V^{-2}$ to be especially appealing.

cond-mat.mtrl-sci↗

arXiv2024

Dark Matter-Electron Detectors for Dark Matter-Nucleon Interactions

In a seminal paper now a decade old, it was shown that dark matter detectors geared at probing interactions with nucleons could also be used to probe dark matter interactions with electrons. In this work, we show that new detector concepts designed to probe dark matter-electron interactions at low masses can similarly be used to probe new parameter space for dark matter-nucleon interactions. We demonstrate the power of this approach by using existing data from superconducting detectors to place new limits on the interactions of nuclei with MeV-scale dark matter. Further, we show that advances in detector technology that have been anticipated for electronic interactions will automatically extend sensitivity deep into uncharted territory for nuclear interactions. This doubles the effective science output of future low-threshold experiments.

hep-ph↗

arXiv2024

Controlling topology through targeted composite symmetry manipulation in magnetic systems

The possibility of selecting magnetic space groups by orienting the magnetization direction or tuning magnetic orders offers a vast playground for engineering symmetry protected topological phases in magnetic materials. In this work, we study how selective tuning of symmetry and magnetism can influence and control the resulting topology in a 2D magnetic system, and illustrate such procedure in the ferromagnetic monolayer MnPSe$_3$. Density functional theory calculations reveals a symmetry-protected accidental semimetalic (SM) phase for out-of-plane magnetization which becomes an insulator when the magnetization is tilted in-plane, reaching band gap values close to $100$ meV. We identify an order-two composite antiunitary symmetry and threefold rotational symmetry that induce the band crossing and classify the possible topological phases using symmetry analysis, which we support with tight-binding and $\mathbf{k}\cdot\mathbf{p}$ models. Breaking of inversion symmetry opens a gap in the SM phase, giving rise to a Chern insulator. We demonstrate this explicitly in the isostructural Janus compound Mn$_2$P$_2$S$_3$Se$_3$, which naturally exhibits Rashba spin-orbit coupling that breaks inversion symmetry. Our results map out the phase space of topological properties of ferromagnetic transition metal phosphorus trichalcogenides and demonstrate the potential of the magnetization-dependent metal-to-insulator transition as a spin switch in integrated two-dimensional electronics.

cond-mat.mes-hall↗

arXiv2024

Modeling the Superlattice Phase Diagram of Transition Metal Intercalation in Bilayer 2H-TaS$_2$

Van der Waals hosts intercalated with transition metal (TM) ions exhibit a range of magnetic properties strongly influenced by the structural order of the intercalants. However, predictive computational models for the intercalant ordering phase diagram are lacking, complicating experimental pursuits to target key structural phases. Here we use Density Functional Theory (DFT) to construct a pairwise lattice model and Monte Carlo to determine its associated thermodynamic phase diagram. To circumvent the complexities of modeling magnetic effects, we use the diamagnetic ions Zn$^{2+}$ and Sc$^{3+}$ as computationally accessible proxies for divalent and trivalent species of interest (Fe$^{2+}$ and Cr$^{3+}$), which provide insights into the high-temperature thermodynamic phase diagram well above the paramagnetic transition temperature. We find that electrostatic coupling between intercalants is almost entirely screened, so the pairwise lattice model represents a coarse-grained charge density reorganization about the intercalated sites. The resulting phase diagram reveals that the entropically-favored $\sqrt{3} \times \sqrt{3}$ ordering and coexisting locally ordered $\sqrt{3} \times \sqrt{3}$ and $2 \times 2$ domains persist across a range of temperatures and intercalation densities. This occurs even at quarter filling of interstitial sites (corresponding to bulk stoichiometries of M$_{0.25}$TaS$_2$; M = intercalant ion) where a preference for long-range $2 \times 2$ order is typically assumed.

cond-mat.mtrl-sci↗

arXiv2024

Factors influencing quantum evaporation of helium from polar semiconductors from first principles

While there is much indirect evidence for the existence of dark matter (DM), to date it has evaded detection. Current efforts focus on DM masses over $\sim$GeV -- to push the sensitivity of DM searches to lower masses, new DM targets and detection schemes are needed. In this work, we focus on the latter - a novel detection scheme recently proposed to detect ~10-100 meV phonons in polar target materials. Previous work showed that well-motivated models of DM can interact with polar semiconductors to produce an athermal population of phonons. This new sensing scheme proposes that these phonons then facilitate quantum evaporation of $^3$He from a van der Waals film deposited on the target material. However, a fundamental understanding of the underlying process is still unclear, with several uncertainties related to the precise rate of evaporation and how it can be controlled. In this work, we use \textit{ab initio} density functional theory (DFT) calculations to compare the adsorption energies of helium atoms on a polar target material, sodium iodide (NaI), to understand the underlying evaporation physics. We explore the role of surface termination, monolayer coverage and elemental species on the rate of He evaporation from the target material. Using this, we discuss the optimal target features for He-evaporation experiments and their range of tunability through chemical and physical modifications such as applied field and surface termination.

hep-ph↗

arXiv2024

Pressure-Tunable Targets for Light Dark Matter Direct Detection: The Case of Solid Helium

We propose hydrostatic pressure -- a well-established tool for tuning properties of condensed matter -- as a novel route for optimizing targets for light dark matter direct detection, specifically via phonons. Pressure dramatically affects compressible solids by boosting the speed of sound and phonon frequencies. Focusing on helium -- the most compressible solid -- our ab initio calculations illustrate how high pressure elevates helium from lacking single-phonon reach to rivaling leading candidates. Our work establishes pressure as an unexplored tuning knob for accessing lower dark matter mass regimes.

hep-ph↗

arXiv2024

Electron-phonon coupling in copper-substituted lead phosphate apatite

Recent reports of room-temperature, ambient pressure superconductivity in copper-substituted lead phosphate apatite, commonly referred to as LK99, have prompted numerous theoretical and experimental studies into its properties. As the electron-phonon interaction is a common mechanism for superconductivity, the electron-phonon coupling strength is an important quantity to compute for LK99. In this work, we compare the electron-phonon coupling strength among the proposed compositions of LK99. The results of our study are in alignment with the conclusion that LK99 is not a likely candidate for room-temperature superconductivity if electron-phonon interaction is to serve as the mechanism.

cond-mat.supr-con↗

arXiv2024

Local atomic stacking and symmetry in twisted graphene trilayers

Moiré superlattices formed from twisting trilayers of graphene are an ideal model for studying electronic correlation, and offer several advantages over bilayer analogues, including more robust and tunable superconductivity and a wide range of twist angles associated with flat band formation. Atomic reconstruction, which strongly impacts the electronic structure of twisted graphene structures, has been suggested to play a major role in the relative versatility of superconductivity in trilayers. Here, we exploit an inteferometric 4D-STEM approach to image a wide range of trilayer graphene structures. Our results unveil a considerably different model for moiré lattice relaxation in trilayers than that proposed from previous measurements, informing a thorough understanding of how reconstruction modulates the atomic stacking symmetries crucial for establishing superconductivity and other correlated phases in twisted graphene trilayers.

cond-mat.mes-hall↗

arXiv2024

Realistic non-collinear ground states of solids with source-free exchange correlation functional

In this work, we extend the source-free (SF) exchange correlation (XC) functional developed by Sangeeta Sharma and co-workers to plane-wave density functional theory (DFT) based on the projector augmented wave (PAW) method. This constraint is implemented by the current authors within the VASP source code, using a fast Poisson solver that capitalizes on the parallel three-dimensional fast Fourier transforms (FFTs) implemented in VASP. Using this modified XC functional, we explore the improved convergence behavior that results from applying this constraint to the GGA-PBE+$U$+$J$ functional. In the process, we compare the non-collinear magnetic ground state computed by each functional and their SF counterpart for a select number of magnetic materials in order to provide a metric for comparing with experimentally determined magnetic orderings. We observe significantly improved agreement with experimentally measured magnetic ground state structures after applying the source-free constraint. Furthermore, we explore the importance of considering probability current densities in spin polarized systems, even under no applied field. We analyze the XC torque as well, in order to provide theoretical and computational analyses of the net XC magnetic torque induced by the source-free constraint. Along these lines, we highlight the importance of properly considering the real-space integral of the source-free local magnetic XC field. Our analysis on probability currents, net torque, and constant terms draws additional links to the rich body of previous research on spin-current density functional theory (SCDFT), and paves the way for future extensions and corrections to the SF corrected XC functional.

cond-mat.mtrl-sci↗

arXiv2024

Discovery of T center-like quantum defects in silicon

Quantum technologies would benefit from the development of high performance quantum defects acting as single-photon emitters or spin-photon interface. Finding such a quantum defect in silicon is especially appealing in view of its favorable spin bath and high processability. While some color centers in silicon have been emerging in quantum applications, there is still a need to search and develop new high performance quantum emitters. Searching a high-throughput computational database of more than 22,000 charged complex defects in silicon, we identify a series of defects formed by a group III element combined with carbon ((A-C)$\rm _{Si}$ with A=B,Al,Ga,In,Tl) and substituting on a silicon site. These defects are analogous structurally, electronically and chemically to the well-known T center in silicon ((C-C-H)$\rm_{Si}$) and their optical properties are mainly driven by an unpaired electron in a carbon $p$ orbital. They all emit in the telecom and some of these color centers show improved properties compared to the T center in terms of computed radiative lifetime or emission efficiency. We also show that the synthesis of hydrogenated T center-like defects followed by a dehydrogenation annealing step could be an efficient way of synthesis. All the T center-like defects show a higher symmetry than the T center making them easier to align with magnetic fields. Our work motivates further studies on the synthesis and control of this new family of quantum defects, and also demonstrates the use of high-throughput computational screening to detect new complex quantum defects.

cond-mat.mtrl-sci↗