arXiv subjects

Ian A. Leahy

Publications and source records attributed to Ian A. Leahy.

13 recordsLinked to original sources

arXiv2026

Field-induced magnetic phase transition driven by a ground state level-crossing in CsErSe$_2$

We report a comprehensive study of the low-temperature magnetic properties of the insulating rare-earth triangular magnet CsErSe$_2$. We uncover a field-induced level crossing at the crystal electric field (CEF) ground state, which gives rise to a first order phase transition as well as to distinctive magnetic properties. This crossing is identified by the accurate determination of the single-ion Hamiltonian, the reliability of which is substantially enhanced by field-dependent optical spectroscopy that directly tracks the Zeeman splittings of Kramers doublets. We also observe spontaneous antiferromagnetic ordering in CsErSe$_2$ below $T_N \approx 110$ mK, and resolve the corresponding magnetic structure using elastic neutron scattering. We discuss how the rich magnetic behavior of CsErSe$_2$ arises from the interplay of non-trivial field-dependent single-ion physics and spontaneous ordering, and highlight the implications of these results for understanding magnetic phenomena across a wide range of insulating rare-earth magnets.

cond-mat.str-el↗

arXiv2025

Interplay of Quasi-Quantum Hall Effect and Coulomb Disorder in Semimetals

Low carrier densities in topological semimetals (TSMs) enable the exploration of novel magnetotransport in the quantum limit (QL). Recent findings consistent with 3D quasi-quantum Hall effect (QQHE) have positioned TSMs as promising platforms for exploring 3D quantum Hall transport, but the lack of tunability in the Fermi level has thus far limited the ability to observe a QQHE signal. Here, we tune the defect concentrations in the Dirac semimetal Cd${}_3$As${}_2$ to achieve ultra-low carrier concentrations at 2 K around $2.9\times10^{16}$cm${}^{-3}$, giving way to QQHE signal at modest fields near 10 T. At low carrier densities, where QQHE is most accessible, we find that clear QQHE is obscured by a carrier density dependent background originating from Coulomb disorder from charged point defects and Landau level broadening. Our results highlight the interplay between QQHE and Coulomb disorder, demonstrating that clear observation of QQHE in TSMs intricately depends on Fermi level and disorder magnitudes. We find that Coulomb disorder, as theoretically predicted, is an essential ingredient for understanding the magnetoresistivity for a spectrum of Fermi levels in Cd${}_3$As${}_2$, anchoring the role of defects and charged disorder in TSM applications. We discuss future constraints and opportunities in exploring 3D QQHE and quantum Hall effects in TSMs.

cond-mat.mtrl-sci↗

arXiv2025

Chirality-induced magnetoresistance in hybrid organic-inorganic perovskite semiconductors

The combination of semiconducting properties and synthetically tunable chirality in chiral metal halide semiconductors (CMHS) offer a compelling platform for room temperature control over electronic spin properties, leveraging effects such as chirality-induced spin selectivity (CISS) for the development of new opto-spintronic functionalities. We report room-temperature CISS-induced magnetoresistance (CISS-MR) exceeding 100% for spin valves in a configuration consisting of a ferromagnet (FM), tunneling barrier, and CMHS. The high CISS-MR is attributed to interfacial spin-selective tunneling barrier induced by the chirality, which can produce current dissymmetry factors that surpass the limit imposed by the Jullière model governed by the intrinsic spin polarization of the adjacent FM contact. The CISS-MR exhibits a strong dependence on the CMHS composition, revealing a structure-property relationship between CISS and structural chirality. The observed exceptionally large tunneling MR response differentiates from a subtle anisotropic MR arising from the proximity effect at the FM/CMHS interface in the absence of a tunneling barrier. Our study provides insights into charge-to-spin interconversion in chiral semiconductors, offering materials design principles to control and enhance CISS response and utilize it in functional platforms.

cond-mat.mtrl-sci↗

arXiv2025

Structural stability, elemental ordering, and transport properties of layered ScTaN2

Some ternary TM nitrides are predicted to adopt layered structures that make them interesting for thermoelectric conversion and quantum materials applications. Synthesis of TM ternary nitride films by physical vapor deposition often favors disordered 3D structures rather than the predicted 2D-like layered structure. In this study, we investigate the structural interplay in the Sc-Ta-N material system, focusing on ScTaN2. We use a two-step combinatorial approach to deposit Sc-Ta-N films by RF co-sputtering and then process the resulting 3D-structured precursor with RTA. Synchrotron GIWAXS on films annealed at 1200 °C for 20 min reveals the nucleation of the layered structure (P63/mmc) within a composition window of x = Sc/(Sc+Ta) = 0.2-0.5. We estimate the long-range order parameter in stoichiometric ScTaN2 films to be 0.86, corresponding to a fraction of antisites of 7%. Interestingly, we find that the structure can accommodate large off-stoichiometry in the Ta-rich region (x < 0.5), facilitated by making an alloy with the nearly isostructural Ta5N6 compound that exists on a composition tie-line. Transport measurements on ScTaN2 reveal a nearly temperature-independent high carrier density (1021 cm-3), suggesting a heavily doped semiconductor or semimetallic character. The carrier mobility is relatively small (9.5 cm2V-1s-1 at 2 K) and the residual-resistivity ratio is small, suggesting that electrical conduction is dominated by defects or disorder. Measured magnetoresistance is indicative of weak antilocalization at low temperatures. We highlight the interplay between ScTaN2 and Ta5N6 in stabilizing layered structures, emphasizes the importance of cation order/disorder for potential tunable alloys, and suggests that ScTaN2 is promising platform for exploring electronic properties in a tie line of stoichiometry.

cond-mat.mtrl-sci↗

arXiv2024

Heat conduction in magnetic insulators via hybridization of acoustic phonons and spin-flip excitations

We present a comprehensive study on the longitudinal magneto-thermal transport in a paramagnetic effective spin-1/2 magnetic insulator CsYbSe$_2$, by introducing a minimal model requiring only Zeeman splitting and magnetoelastic coupling. We use it to argue that hybridized excitations -- formed from acoustic phonons and localized spin-flip-excitations across the Zeeman gap of the crystal electric field ground doublet -- are responsible for a non-monotonic field dependence of longitudinal thermal conductivity. Beyond highlighting a starring role for phonons, our results raise the prospect of universal magneto-thermal transport phenomena in paramagnetic insulators that originate from simple features shared across many systems.

cond-mat.str-el↗

arXiv2023

Spin injection across a III-V/chiral perovskite interface enabling spin accumulation at room temperature

Spin accumulation in semiconductor structures at room temperature and without magnetic fields is key to enable a broader range of opto-electronic functionality. Current efforts are limited due to inherent inefficiencies associated with spin injection into semiconductor structures. Here, we demonstrate spin injection across chiral halide perovskite/III-V interfaces achieving spin accumulation in a standard semiconductor III-V (AlxGa1-x)0.5In0.5P multiple quantum well (MQW) light emitting diode (LED). The spin accumulation in the MQW is detected via emission of circularly polarized light with a degree of polarization of up to ~15%. The chiral perovskite/III-V interface was characterized with X-ray photoemission spectroscopy (XPS), cross sectional scanning Kelvin probe force microscopy, and cross section transmission electron microscopy (TEM) imaging, showing a clean semiconductor/semiconductor interface where the fermi-level can equilibrate. These findings demonstrate chiral perovskite semiconductors can transform well-developed semiconductor platforms to ones that can also control spin.

physics.app-ph↗

arXiv2023

Structural and Optoelectronic Properties of Thin Film LaWN$_3$

Nitride perovskites are an emerging class of materials that have been predicted to display a range of interesting physics and functional properties, but they are under-explored due to the difficulty of synthesizing oxygen-free nitrides. LaWN3, recently reported as the first oxygen-free nitride perovskite, exhibited polar symmetry and a large piezoelectric coefficient. However, the predicted ferroelectric switching was hindered by large leakage current, which motivates better understanding of its electronic structure and optical properties. Here, we study the structure and optoelectronic properties of thin film LaWN3 in greater detail, employing combinatorial techniques to correlate these properties with cation stoichiometry. We report a two-step synthesis that utilizes a more common RF substrate bias instead of a nitrogen plasma source, yielding nanocrystalline films that are crystallized by ex-situ annealing. We investigate the structure and composition of these films, finding polycrystalline La-rich and highly textured W-rich films. The optical absorption onset and temperature- and magnetic field-dependent resistivity are consistent with semiconducting behavior and are highly sensitive to cation stoichiometry, which may be related to amorphous impurities: metallic W or WNx in W-rich samples and insulating La2O3 in La-rich samples. The fractional magnetoresistance is linear and small, consistent with defect scattering, and a W-rich sample has n-type carriers with high densities and low mobilities. We demonstrate a photoresponse in LaWN3: the resistivity of a La-rich sample is enhanced by 28% at low temperature, likely due to a defect trapping mechanism. The physical properties of LaWN3 are highly sensitive to cation stoichiometry, like many oxide perovskites, which therefore calls for precise composition control to utilize the interesting properties observed in this nitride perovskite.

cond-mat.mtrl-sci↗

arXiv2023

Thin film TaAs: developing a platform for Weyl semimetal devices

MX monopnictide compounds (M=Nb,Ta, X = As,P) are prototypical three-dimensional Weyl semimetals (WSMs) that have been shown in bulk single crystal form to have potential for a wide variety of novel devices due to topologically protected band structures and high mobilities. However, very little is known about thin film synthesis, which is essential to enable device applications. We synthesize TaAs(001) epilayers by molecular beam epitaxy on GaAs(001) and provide an experimental phase diagram illustrating conditions for single phase, single-crystal-like growth. We investigate the relationship between nanoscale defects and electronic structure, using angle-resolved photoemission spectroscopy, Kelvin probe microscopy and transmission electron microscopy. Our results provide a roadmap and platform for developing 3D WSMs for device applications.

cond-mat.mtrl-sci↗

arXiv2022

Field-Induced Magnetic States in the Metallic Rare-Earth Layered Triangular Antiferromagnet TbAuAl$_4$Ge$_2$

Magnetic frustration in metallic rare earth lanthanides ($Ln$) with $4f$-electrons is crucial for producing interesting magnetic phases with high magnetic anisotropy where intertwined charge and spin degrees of freedom lead to novel phenomena. Here we report on the magnetic, thermodynamic, and electrical transport properties of TbAuAl$_4$Ge$_2$. Tb ions form 2-dimensional triangular lattice layers which stack along the crystalline $c$-axis. The magnetic phase diagram reveals multiple nearly degenerate ordered states upon applying field along the magnetically easy $ab$-plane before saturation. The magnetoresistance in this configuration exhibits intricate field dependence that closely follows that of the magnetization while the specific heat reveals a region of highly enhanced entropy, suggesting the possibility of a non-trivial spin textured phase. For fields applied along the $c$-axis (hard axis), we find linear magnetoresistance over a wide range of fields. We compare the magnetic properties and magnetoresistance with an isostructral GdAuAl$_4$Ge$_2$ single crystals. These results identify TbAuAl$_4$Ge$_2$ as an environment for complex quantum spin states and pave the way for further investigations of the broader $Ln$AuAl$_4$Ge$_2$ family of materials.

cond-mat.str-el↗

arXiv2022

Direct link between disorder, mobility and magnetoresistance in topological semimetals

The extent to which disorder influences the properties of topological semimetals remains an open question and is relevant to both the understanding of topological states and the use of topological materials in practical applications. Here, we achieve unmatched and systematic control of point defect concentrations in the prototypical Dirac semimetal Cd$_3$As$_2$ to gain important insight into the role of disorder on electron transport behavior. We find that arsenic vacancies introduce localized states near the Fermi level and strongly influence the electron mobility. Reducing arsenic vacancies by changing the As/Cd flux ratio used during deposition results in an increase in the magnetoresistance from 200%-1000% and an increase in mobility from 5000-18,000 cm$^2$/Vs. However, the degree of linear magnetoresistance, which has previously been linked to disorder, is found here to correlate inversely with measures of disorder, including disorder potential and disorder correlation lengths. This finding yields important new information in the quest to identify the origin of linear magnetoresistance in a wider range of materials.

cond-mat.mtrl-sci↗

arXiv2019

Giant thermal magnetoconductivity in CrCl$_3$ and a general model for spin-phonon scattering

Insulating quantum magnets lie at the forefront both of fundamental research into quantum matter and of technological exploitation in the increasingly applied field of spintronics. In this context, the magnetic thermal transport is a particularly sensitive probe of the elementary spin and exotic topological excitations in unconventional magnetic insulators. However, magnetic contributions to heat conduction are invariably intertwined with lattice contributions, and thus the issue of spin-phonon coupling in determining the spin and thermal transport properties becomes more important with emergent topological magnetic system. Here we report the observation of an anomalously strong enhancement of the thermal conductivity, occurring at all relevant temperatures, in the layered honeycomb material CrCl$_3$ in the presence of an applied magnetic field. Away from the magnetically ordered phase at low temperatures and small fields, there is no coherent spin contribution to the heat conduction, and hence the effect must be caused by a strong suppression of the phonon thermal conductivity due to magnetic fluctuations, which are in turn suppressed by the field. We build an empirical model for the thermal conductivity of CrCl$_3$ within a formalism assuming an independently determined number of spin-flip processes and an efficiency of the phonon scattering events they mediate. By extracting the intrinsic phonon thermal conductivity we obtain a quantitative description at all fields and temperatures and demonstrate that the scattering efficiency is entirely independent of the field. In this way we use CrCl$_3$ as a model system to understand the interactions between spin and phonon excitations in the context of thermal transport. We anticipate that the completely general framework we introduce will have broad implications for the interpretation of transport phenomena in magnetic quantum materials.

cond-mat.str-el↗

arXiv2018

Non-saturating large magnetoresistance in semimetals

The rapidly expanding class of quantum materials known as {\emph{topological semimetals}} (TSM) display unique transport properties, including a striking dependence of resistivity on applied magnetic field, that are of great interest for both scientific and technological reasons. However, experimental signatures that can identify or discern the dominant mechanism and connect to available theories are scarce. Here we present the magnetic susceptibility ($χ$), the tangent of the Hall angle ($\tanθ_H$) along with magnetoresistance in four different non-magnetic semimetals with high mobilities, NbP, TaP, NbSb$_2$ and TaSb$_2$, all of which exhibit non-saturating large MR. We find that the distinctly different temperature dependences, $χ(T)$ and the values of $\tanθ_H$ in phosphides and antimonates serve as empirical criteria to sort the MR from different origins: NbP and TaP being uncompensated semimetals with linear dispersion, in which the non-saturating magnetoresistance arises due to guiding center motion, while NbSb$_2$ and TaSb$_2$ being {\it compensated} semimetals, with a magnetoresistance emerging from nearly perfect charge compensation of two quadratic bands. Our results illustrate how a combination of magnetotransport and susceptibility measurements may be used to categorize the increasingly ubiquitous non-saturating large magnetoresistance in TSMs.

cond-mat.str-el↗

arXiv2017

Anomalous thermal conductivity and magnetic torque response in the honeycomb magnet $α$-RuCl$_3$

We report on the unusual behavior of the in-plane thermal conductivity ($κ$) and torque ($τ$) response in the Kitaev-Heisenberg material $α$-RuCl$_3$. $κ$ shows a striking enhancement with linear growth beyond H = 7 T, where magnetic order disappears, while $τ$ for both of the in-plane symmetry directions shows an anomaly at the same field. The temperature- and field-dependence of $κ$ are far more complex than conventional phonon and magnon contributions, and require us to invoke the presence of unconventional spin excitations whose properties are characteristic of a field-induced spin-liquid phase related to the enigmatic physics of the Kitaev model in an applied magnetic field

cond-mat.str-el↗