arXiv subjects

Jennifer Coulter

Publications and source records attributed to Jennifer Coulter.

At least 19 recordsLinked to original sources

arXiv2026

High-quality single crystals of the kagome metals Ni$_3$In and Ni$_3$Sn grown from Pb flux

The bilayer kagome metal Ni$_3$In has recently attracted attention due to the presence of a flat band located near the Fermi level, which has been associated with unconventional thermodynamic and electronic transport properties [Ye et al., Nat. Phys. 20, 610-614 (2024)]. However, further investigation of the intrinsic properties of this system has been hindered by the lack of large, high-quality single crystals. Here, we report the successful growth of Ni$_3$(In, Sn) single crystals using a Pb-flux technique. By optimizing the growth conditions, competing binary phases can be effectively suppressed, enabling the synthesis of single crystals with dimensions reaching several millimeters. We compare the physical properties of our Pb-flux-grown crystals to previously reported samples prepared by iodine-assisted chemical vapor transport and molecular beam epitaxy as well as to first-principles resistivity calculations. We find a significantly lower electrical resistivity in our crystals, in excellent agreement with calculations of resistivity from electron-phonon scattering, a sizeable non-saturating magnetoresistance, and a reduced Sommerfeld coefficient and magnetic susceptibility compared to previous experimental findings, which are likely related to differences in the Fermi level position. Our results establish Pb-flux growth as a reliable route for obtaining large single crystals of the bilayer kagome metals Ni$_3$(In, Sn) that are suitable for further thermodynamic and spectroscopic investigations of their intrinsic electronic and magnetic properties.

cond-mat.mtrl-sci↗

arXiv2025

Equivalence of charged and neutral density functional formulations for correcting the many-body self-interaction of polarons

The electron self-interaction problem in density functional theory affects the accurate modeling of polarons, particularly their localization and formation energy. Charged and neutral density functional formulations have been developed to address this issue, yet their relationship remains unclear. Here, we demonstrate their equivalence in treating the many-body self-interaction of the polaron state. In particular, we connect with each other piecewise-linear functionals based on adding an extra charge to the supercell, the pSIC approach derived from the energetics of the neutral defect with polaronic distortions in a supercell, and the unit-cell method for polarons based on electron-phonon couplings. We show that these approaches lead to the same formal expression of the self-interaction corrected energy, which is fully defined by the energetics of the neutral charge state of the charged polaronic structure. Residual differences between these methods solely arise from the achieved polaronic structure, which is affected by different treatments of electron-screening and finite-size effects. We apply these methods to a set of prototypical small hole and electron polarons, including the hole polaron in MgO, the hole polaron in $\beta$-Ga$_2$O$_3$, the $V_\text{k}$ center in NaI, the electron polaron in BiVO$_4$, and the electron polaron in TiO$_2$. We show that the ground-state properties of polarons obtained using charged and neutral density functional formulations are in excellent agreement.

cond-mat.mtrl-sci↗

arXiv2025

Spatiotemporal Order and Parametric Instabilities from First-Principles

Shaping crystal structure with light is an enduring goal of physics and materials engineering. Here we present calculations in candidate materials selected by symmetry that allow light-induced spatiotemporal parametric instabilities. We demonstrate a theoretical framework that includes a complete symmetry analysis of phonon modes that contribute to parametric instabilities across all non-centrosymmetric point groups, a detailed survey of the materials landscape and finally the computation of nonlinear couplings from first principles. We then showcase detailed results for chiral crystals, ferroelectrics, and layered van der Waals materials. Our results pave the way towards realizing designer time-crystalline order in quantum materials, detectable with time-resolved diffractive probes.

cond-mat.mtrl-sci↗

arXiv2025

Electron-phonon origins of unconventional resistivity in moderately correlated perovskite oxides

Transition-metal perovskite oxides exhibit moderately correlated metallic phases, several of which exhibit a $T^2$ resistivity scaling up to temperatures far exceeding the regime where Fermi-liquid electron-electron scattering is expected to dominate. Some of these materials, such as SrMoO$_3$, also exhibit unexplained ultra-low room-temperature resistivity. We demonstrate that in SrMoO$_3$, SrWO$_3$, SrTaO$_3$, SrNbO$_3$, and SrVO$_3$ electron-phonon scattering results in quadratic-scaling resistivity due to the shape of the Fermi surface and the thermal activation of optical phonons. We also reveal that the origin of the low resistivity of SrMoO$_3$ is an overall low electron-phonon coupling strength, and identify SrWO$_3$ and SrTaO$_3$ as other possible low-resistivity oxides. Additionally, we find that the strength of electron-phonon coupling is sensitive to structural distortions, energies of optical phonons, and the treatment of electronic correlations. This suggests design principles for finding other ultra-high conductivity transition-metal oxides, and has significant implications for theoretical interpretation of direct-current resistivity in transition-metal oxides and beyond.

cond-mat.mtrl-sci↗

arXiv2025

Electron-phonon coupling in correlated materials: insights from the Hubbard-Holstein model

Dynamical mean-field theory computations of the electron self energy of the Hubbard-Holstein model as a function of electron-phonon and electron-electron interactions are analyzed to gain insight into the dependence of electron-phonon couplings on correlation strength in quantum materials. We find that the electron-phonon interaction is strongly suppressed by electronic correlations, while electron-electron correlation effects at Fermi liquid scales are only weakly modified by coupling to phonons, with phonon-induced modifications most evident at high frequencies on the order of the electronic bandwidth. Implications for beyond-density functional theories of the electron-phonon interaction are discussed.

cond-mat.str-el↗

arXiv2025

Electron-Phonon Coupling in Correlated Metals: A Dynamical Mean-Field Theory Study

Strong electron-electron interactions are known to significantly modify the electron-phonon coupling relative to the predictions of density functional theory, but this effect is challenging to calculate with realistic theories of strongly correlated materials. Here we define and calculate a version of the EPC applicable beyond band theory by combining first principles density functional theory plus dynamical mean-field theory with finite difference phonon perturbations, presenting results for several representative phonon modes in two materials of interest. In the three-orbital correlated metal SrVO$_3$, we find that intra-V-$t_{2g}$ band correlation significantly increases the coupling of these electrons to a Jahn-Teller phonon mode that splits the degenerate orbital energies, while slightly reducing the coupling associated with a breathing phonon that couples to the charge on each V atom. In the infinite layer cuprate CaCuO$_2$, we find that local correlation within the $d_{x^2-y^2}$ orbital derived band has a modest effect on coupling of near-Fermi surface electrons to optical breathing modes. In both cases, the interaction correction to the electron-phonon coupling predicted by dynamical mean-field theory has a significant dependence on the electronic frequency, arising from a lattice-distortion dependence of the correlated electron dynamics, showing the inadequacy of the simple picture in which correlations change static local susceptibilities. We also show that the electron-phonon scattering and phonon lifetimes associated with these phonon modes are modified by the electronic correlation. Our findings shed light on the material- and mode-specific role of dynamical electronic correlation in electron-phonon coupling and highlight the importance of developing efficient computational methods for treating electron-phonon coupling in correlated materials.

cond-mat.str-el↗

arXiv2025

Coupled electron-phonon hydrodynamics and viscous thermoelectric equations

Non-diffusive, fluid-like transport of charge and heat has been observed in several materials, raising the question of whether they can emerge simultaneously and how they are related to bi-component electron-phonon fluids. Here we introduce a first-principles theory and computational framework to quantitatively describe these phenomena from atomistic to continuum scales in complex device geometries. Starting from the microscopic coupled electron-phonon Boltzmann transport equation, we formalize the emergence of composite "relaxon" electron-phonon excitations, show that they determine the viscosity tensors of the two fluids, and quantify the impact of electron-phonon drag on thermoelectric transport coefficients. We then demonstrate that the coupled Boltzmann equation can be coarse-grained into a set of mesoscopic Viscous Thermoelectric Equations, formally unifying Gurzhi's hydrodynamic equation for electrons [Sov. Phys. Usp., 1968] and the recently developed Viscous Heat Equations for phonons [PRX 10, 011019, 2020], while extending them to cover the intermediate regime of mixed electron and phonon fluids. We leverage this framework to elucidate how electron and phonon fluids can coexist or mix, rationalizing pioneering experiments on electron-phonon drag in graphite, and predicting smoking-gun signatures of non-diffusive behavior such as non-harmonic temperature and electric potential fields, and compressible thermoelectric backflow.

cond-mat.mes-hall↗

arXiv2025

Stabilization of Fermi-liquid behavior by interactions in disordered metals

We study the interplay of electron-electron and electron-disorder scattering in correlated Fermi liquids by the disordered Hubbard model using dynamical mean-field theory with an IPT-CPA solver. We find significant violations of Matthiessen's rule (additivity of scattering mechanisms) which we explain in terms of the screening of the disorder potential by interactions, leading to a protection of the electron-electron inelastic scattering rate against disorder. We also show that large disorder can lead to a surprising enhancement of the electron-electron scattering that contrasts with the competition seen in the elastic channel. Our results compare positively with available resistivity data in the disordered Fermi liquid phase of the correlated organic metals $\kappa$-(ET)$_{2}$X, and rationalize the strong sample dependence of the $T^2$ coefficients observed in the resistivity of correlated perovskite oxides such as SrVO$_3$.

cond-mat.str-el↗

arXiv2025

Energy filtering-induced ultrahigh thermoelectric power factors in Ni$_3$Ge

Traditional thermoelectric materials rely on low thermal conductivity to enhance their efficiency but suffer from inherently limited power factors. Novel pathways to optimize electronic transport are thus crucial. Here, we achieve ultrahigh power factors in Ni$_3$Ge through a new materials design principle. When overlapping flat and dispersive bands are engineered to the Fermi level, charge carriers can undergo intense interband scattering, yielding an energy filtering effect similar to what has long been predicted in certain nanostructured materials. Via a multi-step DFT-based screening method developed herein, we discover a new family of L1$_2$-ordered binary compounds with ultrahigh power factors up to 11 mW m$^{-1}$ K$^{-2}$ near room temperature, which are driven by an intrinsic phonon-mediated energy filtering mechanism. Our comprehensive experimental and theoretical study of these new intriguing materials paves the way for understanding and designing high-performance scattering-tuned metallic thermoelectrics.

cond-mat.mtrl-sci↗

arXiv2024

Alternate cleavage structure and electronic inhomogeneity in Ca-doped YBa$_2$Cu$_3$O$_{7-\delta}$

YBa$_2$Cu$_3$O$_{7-\delta}$ (YBCO) has favorable macroscopic superconducting properties of $T_\mathrm{c}$ up to 93 K and $H_{c2}$ up to 150 T. However, its nanoscale electronic structure remains mysterious because bulk-like electronic properties are not preserved near the surface of cleaved samples for easy access by local or surface-sensitive probes. It has been hypothesized that Ca-doping at the Y site could induce an alternate cleavage plane that mitigates this issue. We use scanning tunneling microscopy (STM) to study both Ca-free and 10% Ca-doped YBCO, and find that the Ca-doped samples do indeed cleave on an alternate plane, yielding a spatially-disordered partial (Y,Ca) layer. Our density functional theory calculations support the increased likelihood of this new cleavage plane in Ca-doped YBCO. On this surface, we image a superconducting gap with average value 24 $\pm$ 3 meV and characteristic length scale 1-2 nm, similar to Bi-based high-$T_\mathrm{c}$ cuprates, but the first map of gap inhomogeneity in the YBCO family.

cond-mat.supr-con↗

arXiv2023

Complexity of Many-Body Interactions in Transition Metals via Machine-Learned Force Fields from the TM23 Data Set

This work examines challenges associated with the accuracy of machine-learned force fields (MLFFs) for bulk solid and liquid phases of d-block elements. In exhaustive detail, we contrast the performance of force, energy, and stress predictions across the transition metals for two leading MLFF models: a kernel-based atomic cluster expansion method implemented using sparse Gaussian processes (FLARE), and an equivariant message-passing neural network (NequIP). Early transition metals present higher relative errors and are more difficult to learn relative to late platinum- and coinage-group elements, and this trend persists across model architectures. Trends in complexity of interatomic interactions for different metals are revealed via comparison of the performance of representations with different many-body order and angular resolution. Using arguments based on perturbation theory on the occupied and unoccupied d states near the Fermi level, we determine that the large, sharp d density of states both above and below the Fermi level in early transition metals leads to a more complex, harder-to-learn potential energy surface for these metals. Increasing the fictitious electronic temperature (smearing) modifies the angular sensitivity of forces and makes the early transition metal forces easier to learn. This work illustrates challenges in capturing intricate properties of metallic bonding with current leading MLFFs and provides a reference data set for transition metals, aimed at benchmarking the accuracy and improving the development of emerging machine-learned approximations.

cond-mat.mtrl-sci↗

arXiv2022

Phoebe: a High-Performance Framework for Solving Phonon and Electron Boltzmann Transport Equations

Understanding the electrical and thermal transport properties of materials is critical to the design of electronics, sensors and energy conversion devices. Computational modeling can accurately predict materials properties but, in order to be reliable, require accurate descriptions of electron and phonon states and their interactions. While first-principles methods are capable of describing the energy spectrum of each carrier, using them to compute transport properties is still a formidable task, both computationally demanding and memory intensive, requiring integration of fine microscopic scattering details for estimation of macroscopic transport properties. To address this challenge, we present Phoebe - a newly developed software package that includes the effects of electron-phonon, phonon-phonon, boundary, and isotope scattering in computations of electrical and thermal transport properties of materials with a variety of available methods and approximations. This open source C++ code combines MPI-OpenMP hybrid parallelization with GPU acceleration and distributed memory structures to manage computational cost, allowing Phoebe to effectively take advantage of contemporary computing infrastructures. We demonstrate that Phoebe accurately and efficiently predicts a wide range of transport properties, opening avenues for accelerated computational analysis of complex crystals.

cond-mat.mtrl-sci↗

arXiv2022

Engineering ideal helical topological networks in stanene via Zn decoration

The xene family of topological insulators plays a key role in many proposals for topological electronic, spintronic, and valleytronic devices. These proposals rely on applying local perturbations, including electric fields and proximity magnetism, to induce topological phase transitions in xenes. However, these techniques lack control over the geometry of interfaces between topological regions, a critical aspect of engineering topological devices. We propose adatom decoration as a method for engineering atomically precise topological edge modes in xenes. Our first-principles calculations show that decorating stanene with Zn adatoms exclusively on one of two sublattices induces a topological phase transition from the quantum spin Hall (QSH) to quantum valley Hall (QVH) phase and confirm the existence of spin-valley polarized edge modes propagating at QSH/QVH interfaces. We conclude by discussing technological applications of these edge modes that are enabled by the atomic precision afforded by recent advances in adatom manipulation technology.

cond-mat.mes-hall↗

arXiv2020

Relative importance of nonlinear electron-phonon coupling and vertex corrections in the Holstein model

Determining the range of validity of Migdal's approximation for electron-phonon ($e$-ph) coupled systems is a long-standing problem. Many attempts to answer this question employ the Holstein Hamiltonian, where the electron density couples linearly to local lattice displacements. When these displacements are large, however, nonlinear corrections to the interaction must also be included, which can significantly alter the physical picture obtained from this model. Using determinant quantum Monte Carlo and the self-consistent Migdal approximation, we compared superconducting and charge-density-wave correlations in the Holstein model with and without second-order nonlinear interactions. We find a disagreement between the two cases, even for relatively small values of the $e$-ph coupling strength, and, importantly, that this can occur in the same parameter regions where Migdal's approximation holds. Our results demonstrate that questions regarding the validity of Migdal's approximation go hand in hand with questions of the validity of a linear $e$-ph interaction.

cond-mat.supr-con↗

arXiv2020

Effects of Structural Distortions on the Electronic Structure of T-type Transition Metal Dichalcogenides

Single-layer transition metal dichalcogenides (TMDCs) can adopt two distinct structures corresponding to different coordination of the metal atoms. TMDCs adopting the T-type structure exhibit a rich and diverse set of phenomena, including charge density waves (CDW) in a $\sqrt{13}\times\sqrt{13}$ supercell pattern in TaS$_2$ and TaSe$_2$, and a possible excitonic insulating phase in TiSe$_2$. These properties make the T-TMDCs desirable components of layered heterostructure devices. In order to predict the emergent properties of combinations of different layered materials, one needs simple and accurate models for the constituent layers which can take into account potential effects of lattice mismatch, relaxation, strain, and structural distortion. Previous studies have developed ab initio tight-binding Hamiltonians for H-type TMDCs [arXiv:1709.07510]. Here we extend this work to include T-type TMDCs. We demonstrate the capabilities of our model using three example systems: a 1-dimensional sinusoidal ripple, the 2$\times$2 CDW in TiSe$_2$, and the $\sqrt{13}\times\sqrt{13}$ CDW in TaS$_2$. Using the technique of band unfolding we compare the electronic structure of the distorted crystals to the pristine band structure and find excellent agreement with direct DFT calculations, provided the magnitude of the distortions remains in the linear regime.

cond-mat.mes-hall↗

arXiv2020

Metamaterials for Active Colloid Transport

Transport phenomena in out-of-equilibrium systems is immensely important in a myriad of applications in biology, engineering and physics. Complex environments, such as the cytoplasm or porous media, can substantially affect the transport properties of such systems. In particular, recent interest has focused on how such environments affect the motion of active systems, such as colloids and organisms propelled by directional driving forces. Nevertheless, the transport of active matter with non-directional (rotational) activity is yet to be understood, despite the ubiquity of rotating modes of motion in synthetic and natural systems. Here, we report on the discovery of spatiotemporal metamaterial systems that are able to dictate the transport of spinning colloids in exquisite ways based on solely two parameters: frequency of spin modulation in time and the symmetry of the metamaterial. We demonstrate that dynamic modulations of the amplitude of spin on a colloid in lattices with rotational symmetry give rise to non-equilibrium ballistic transport bands, reminiscent of those in Floquet-Bloch systems. By coupling these temporal modulations with additional symmetry breaking in the lattice, we show selective control from 4-way to 2-way to unidirectional motion. Our results provide critical new insights into the motion of spinning matter in complex (biological) systems. Furthermore, our work can also be used for designing systems with novel and unique transport properties for application in, for example, smart channel-less microfluidics, micro-robotics, or colloidal separations.

cond-mat.soft↗

arXiv2019

Optoelectronic Response of Type-I Weyl Semimetals TaAs and NbAs from First Principles

Weyl semimetals are materials with topologically nontrivial band structure both in the bulk and on the surface, hosting chiral nodes which are sinks and sources of Berry curvature. Weyl semimetals have been predicted, and recently measured, to exhibit large nonlinear optical responses. This discovery, along with their high mobilities, makes Weyl semimetals relevant to a broad spectrum of applications in optoelectronic, nanophotonic and quantum optical devices. While there is growing interest in understanding and characterizing the linear and nonlinear behavior of Weyl semimetals, an ab initio calculation of the linear optical and optoelectronic responses at finite temperature remains largely unexplored. Here, we specifically address the temperature dependence of the linear optical response in type-I Weyl semimetals TaAs and NbAs. We evaluate from first principles the scattering lifetimes due to electron-phonon and electron-electron interaction and incorporate these lifetimes in evaluating an experimentally relevant frequency-, polarization- and temperature-dependent complex dielectric function for each semimetal. From these calculations we present linear optical conductivity predictions which agree well where experiment exists (for TaAs) and guide the way for future measurements of type-I Weyl semimetals. Importantly, we also examine the optical conductivity's dependence on the chemical potential, a crucial physical parameter which can be controlled experimentally and can elucidate the role of the Weyl nodes in optoelectronic response. Through this work, we present design principles for Weyl optoelectronic devices that use photogenerated carriers in type-I Weyl semimetals.

cond-mat.mtrl-sci↗

arXiv2019

A Theoretical Investigation of Charge Density Wave Instability in CuS$_2$

The existence of a charge density wave (CDW) in transition metal dichalcogenide CuS$_2$ has remained undetermined since its first experimental synthesis nearly 50 years ago. Despite conflicting experimental literature regarding its low temperature structure, there exists no theoretical study of the phonon properties and lattice stability of this material. By studying the first-principles electronic structure and phonon properties of CuS$_2$ at various electronic temperatures, we identify temperature-sensitive soft phonon modes which unveil a previously unreported Kohn anomaly at approximately 100K. Variation of the electronic temperature shows the presence of two distinct phases, characterized at low temperature by a $2\times2\times2$ periodic charge modulation associated with the motion of the S$_2$ dimers. Investigation of the Fermi surface presents a potential Fermi surface nesting vector related to the location of the Kohn anomaly and observed band splittings in the unfolded bandstructure. The combination of these results suggests a strong possibility of CDW order in CuS$_2$. Further study of CuS$_2$ in monolayer form finds no evidence of a CDW phase, as the identified bulk periodic distortions cannot be realized in 2D. This behavior sets this material apart from other transition metal dichalcogenide materials, which exhibit a charge density wave phase down to the 2D limit. As CDW in TMDC materials is considered to compete with superconductivity, the lack of CDW in monolayer CuS$_2$ suggests the possibility of enhanced superconductivity relative to other transition metal dichalcogenides. Overall, our work identifies CuS$_2$ as a previously unrealized candidate to study interplay of superconductivity, CDW order, and dimensionality.

cond-mat.mes-hall↗