arXiv subjects

Alannah M. Hallas

Publications and source records attributed to Alannah M. Hallas.

36 records · Page 2Linked to original sources

arXiv2024

Discovery of Superconductivity and Electron-Phonon Drag in the Non-Centrosymmetric Weyl Semimetal LaRhGe$_3$

We present an exploration of the effect of electron-phonon coupling and broken inversion symmetry on the electronic and thermal properties of the semimetal LaRhGe$_3$. Our transport measurements reveal evidence for electron-hole compensation at low temperatures, resulting in a large magnetoresistance of 3000% at 1.8 K and 14 T. The carrier concentration is on the order of $10^{21}\rm{/cm}^3$ with high carrier mobilities of $2000~\rm{cm}^2/\rm{Vs}$. When coupled to our theoretical demonstration of symmetry-protected $\textit{almost movable}$ Weyl nodal lines, we conclude that LaRhGe$_3$ supports a Weyl semimetallic state. We discover superconductivity in this compound with a $T_{\text c}$ of 0.39(1) K and $B_{\rm{c}}(0)$ of 2.2(1) mT, with evidence from specific heat and transverse-field muon spin relaxation. We find an exponential dependence in the normal state electrical resistivity below $\sim50$ K, while Seebeck coefficient and thermal conductivity measurements each reveal a prominent peak at low temperatures, indicative of strong electron-phonon interactions. To this end, we examine the temperature-dependent Raman spectra of LaRhGe$_3$ and find that the lifetime of the lowest energy $A_1$ phonon is dominated by phonon-electron scattering instead of anharmonic decay. We conclude that LaRhGe$_3$ has strong electron-phonon coupling in the normal state, while the superconductivity emerges from weak electron-phonon coupling. These results open up the investigation of electron-phonon interactions in the normal state of superconducting non-centrosymmetric Weyl semimetals.

cond-mat.supr-con↗

arXiv2024

Physical properties and electronic structure of the two-gap superconductor V$_{2}$Ga$_{5}$

We present a thorough investigation of the physical properties and superconductivity of the binary intermetallic V2Ga5. Electrical resistivity and specific heat measurements show that V2Ga5 enters its superconducting state below Tsc = 3.5 K, with a critical field of Hc2,perp c(Hc2,para c) = 6.5(4.1) kOe. With H perp c, the peak effect was observed in resistivity measurements, indicating the ultrahigh quality of the single crystal studied. The resistivity measurements under high pressure reveal that the Tsc is suppressed linearly with pressure and reaches absolute zero around 20 GPa. Specific heat and muon spin relaxation measurements both indicate that the two-gap s-wave model best describes the superconductivity of V2Ga5. The spectra obtained from angle-resolved photoemission spectroscopy measurements suggest that two superconducting gaps open at the Fermi surface around the Z and Γ points. These results are verified by first-principles band structure calculations. We therefore conclude that V2Ga5 is a phonon-mediated two-gap s-wave superconductor

cond-mat.supr-con↗

arXiv2023

Symmetry-mode analysis for local structure investigations using pair distribution function data

Symmetry-adapted distortion modes provide a natural way to describe distorted structures derived from higher-symmetry parent phases. Structural refinements using symmetry-mode amplitudes as fit variables have been used for at least 10 years in Rietveld refinements of the average crystal structure from diffraction data; more recently, this approach has also been used for investigations of the local structure using real-space pair distribution function (PDF) data. Here, we further demonstrate the value of performing symmetry-mode fits to PDF data through the successful application of this method to two topical materials: TiSe$_2$, where we detect the subtle but long-range structural distortion driven by the formation of a charge density wave, and MnTe, where we characterize a large but highly localized structural distortion in terms of symmetry-lowering displacements of the Te atoms. The analysis is performed using fully open-source code within the DiffPy framework using two packages we developed for this work: isopydistort, which provides a scriptable interface to the ISODISTORT web application for group theoretical calculations, and isopytools, which converts the ISODISTORT output into a DiffPy-compatible format for subsequent fitting and analysis. These developments expand the potential impact of symmetry-adapted PDF analysis by enabling high throughput analysis and removing the need for any commercial software.

cond-mat.mtrl-sci↗

arXiv2023

Phase stability of entropy stabilized oxides with the $α$-PbO$_2$ structure

The prediction of new high entropy oxides (HEOs) remains a profound challenge due to their inherent chemical complexity. In this work, we combine experimental and computational methods to search for new HEOs in the tetravalent $A$O$_2$ family, using exclusively $d^0$ and $d^{10}$ cations, and to explain the observed phase stability of the $α$-PbO$_2$ structure, as found for the medium entropy oxide (Ti, Zr, Hf, Sn)O$_2$. Using a pairwise approach to approximate the mixing enthalpy, we confirm that $α$-PbO$_2$ is the expected lowest energy structure for this material above other candidates including rutile, baddeleyite, and fluorite structures. We also show that no other five-component compound composed of the tetravalent cations considered here is expected to form under solid state synthesis conditions, which we verify experimentally. Ultimately, we conclude that the flexible geometry of the $α$-PbO$_2$ structure can be used to understand its stability among tetravalent HEOs.

cond-mat.mtrl-sci↗

arXiv2023

Direct confirmation of long-range magnetic order and evidence for multipoles in Ce$_{2}$O$_{3}$

The sesquioxide, Ce$_{2}$O$_{3}$, has been a material of intense interest in recent years due to reports of an anomalous giant magnetodielectric effect and emergent mixed crystal field-phonon (vibronic) excitations below a putative antiferromagnetic transition at T$_{N}$ = 6.2 K. The claim of long-range magnetic order in this material is based on heat capacity and temperature-dependent susceptibility measurements; however, multiple neutron diffraction studies have been unable to distinguish any magnetic Bragg peaks. In this article, we present the results of a comprehensive investigation of the low-temperature phase in symmetry-broken polycrystalline Ce$_{2}$O$_{3}$ using a combination of magnetic susceptibility, heat capacity, neutron diffraction, triple-axis and time-of-flight (TOF) inelastic neutron scattering (INS), and muon spin rotation ($μ$SR). Our measurements and subsequent analysis confirm that the transition at T$_{N}$ can be associated with the ordering of moments on the Ce$^{3+}$ site. Both a spontaneous magnetic order observed with $μ$SR and a dispersive spin-wave spectrum observed with inelastic neutron scattering suggest a model wherein planar dipoles order antiferromagnetically. Notable inconsistencies between $μ$SR and neutron scattering data within the dipole picture provide strong evidence for the ordering of higher-order moments.

cond-mat.str-el↗

arXiv2023

Understanding the role of entropy in high entropy oxides

The field of high entropy oxides (HEOs) flips traditional materials science paradigms on their head by seeking to understand what properties arise in the presence of profound configurational disorder. This disorder, which originates from multiple elements sharing a single lattice site, can take on a kaleidoscopic character due to the vast numbers of possible elemental combinations. High configurational disorder appears to imbue some HEOs with functional properties that far surpass their non-disordered analogs. While experimental discoveries abound, efforts to characterize the true magnitude of the configurational entropy and understand its role in stabilizing new phases and generating superior functional properties have lagged behind. Understanding the role of configurational disorder in existing HEOs is the crucial link to unlocking the rational design of new HEOs with targeted properties. In this Perspective, we attempt to establish a framework for articulating and beginning to address these questions in pursuit of a deeper understanding of the true role of entropy in HEOs.

cond-mat.mtrl-sci↗

arXiv2022

Entropy engineering and tunable magnetic order in the spinel high entropy oxide

Spinel oxides are an ideal setting to explore the interplay between configurational entropy, site selectivity, and magnetism in high entropy oxides. In this work we characterize the magnetic properties of the spinel (Cr,Mn,Fe,Co,Ni)$_3$O$_4$ and study the evolution of its magnetism as a function of non-magnetic gallium substitution. Across the range of compositions studied here, from 0% to 40% Ga, magnetic susceptibility and powder neutron diffraction measurements show that ferrimagnetic order is robust in the spinel HEO. However, we also find that the ferrimagnetic order is highly tunable, with the ordering temperature, saturated and sublattice moments, and magnetic hardness all varying significantly as a function of Ga concentration. Through x-ray absorption and magnetic circular dichroism, we are able to correlate this magnetic tunability with strong site selectivity between the various cations and the tetrahedral and octahedral sites in the spinel structure. In particular, we find that while Ni and Cr are largely unaffected by the substitution with Ga, the occupancies of Mn, Co, and Fe are each significantly redistributed. Ga substitution also requires an overall reduction in the transition metal valence, and this is entirely accommodated by Mn. Finally, we show that while site selectivity has an overall suppressing effect on the configurational entropy, over a certain range of compositions, Ga substitution yields a striking increase in the configurational entropy and may confer additional stabilization. Spinel oxides can be tuned seamlessly from the low-entropy to the high-entropy regime, making this an ideal platform for entropy engineering.

cond-mat.mtrl-sci↗

arXiv2022

Tutorial: A Beginner's Guide to Interpreting Magnetic Susceptibility Data with the Curie-Weiss Law

Magnetic susceptibility measurements are often the first characterization tool that researchers turn to when beginning to assess the magnetic nature of a newly discovered material. Breakthroughs in instrumentation have made the collection of high quality magnetic susceptibility data more accessible than ever before. However, the analysis of susceptibility data remains a common challenge for newcomers to the field of magnetism. While a comprehensive treatment of the theoretical aspects of magnetism are found in numerous excellent textbooks, there is a gap at the point of practical application. We were inspired by this obstacle to put together this guide to the analysis and interpretation of magnetic susceptibility data, with an emphasis on materials that exhibit Curie-Weiss paramagnetism.

cond-mat.mtrl-sci↗

arXiv2022

Nonsymmorphic Symmetry-Protected Band Crossings in a Square-Net Metal PtPb$_4$

Topological semimetals with symmetry-protected band crossings have emerged as a rich landscape to explore intriguing electronic phenomena. Nonsymmorphic symmetries in particular have been shown to play an important role in protecting the crossings along a line (rather than a point) in momentum space. Here we report experimental and theoretical evidence for Dirac nodal line crossings along the Brillouin zone boundaries in PtPb$_4$, arising from the nonsymmorphic symmetry of its crystal structure. Interestingly, while the nodal lines would remain gapless in the absence of spin-orbit coupling (SOC), the SOC in this case plays a detrimental role to topology by lifting the band degeneracy everywhere except at a set of isolated points. Nevertheless, the nodal line is observed to have a bandwidth much smaller than that found in density functional theory (DFT). Our findings reveal PtPb$_4$ to be a material system with narrow crossings approximately protected by non-symmorhpic crystalline symmetries.

cond-mat.mtrl-sci↗

arXiv2022

Field-induced quantum critical point in the new itinerant antiferromagnet Ti$_3$Cu$_4$

New phases of matter emerge at the edge of magnetic instabilities. In local moment systems, such as heavy fermions, the magnetism can be destabilized by pressure, chemical doping, and, rarely, by magnetic field, towards a zero-temperature transition at a quantum critical point (QCP). Even more rare are instances of QCPs induced by pressure or doping in itinerant moment systems, with no known examples of analogous field-induced \textit{T} = 0 transitions. Here we report the discovery of a new itinerant antiferromagnet with no magnetic constituents, in single crystals of Ti$_3$Cu$_4$ with $T_N$ = 11.3 K. Band structure calculations point to an orbital-selective, spin density wave ground state, a consequence of the square net structural motif in Ti$_3$Cu$_4$. A small magnetic field, $H_C$ = 4.87 T, suppresses the long-range order via a continuous second-order transition, resulting in a field-induced QCP. The magnetic Grüneisen ratio diverges as $H \rightarrow H_C$ and $T\rightarrow0$, with a sign change at $H_C$ and $T^{-1}$ scaling at $H~=~H_C$, providing evidence from thermodynamic measurements for quantum criticality for $H \parallel c$. Non-Fermi liquid (NFL) to Fermi liquid (FL) crossover is observed close to the QCP, as revealed by the power law behavior of the electrical resistivity.

cond-mat.str-el↗

arXiv2021

Frustrated Magnetism in Fluoride and Chalcogenide Pyrochlore Lattice Materials

Pyrochlore lattices, which are found in two important classes of materials -- the $A_2B_2X_7$ pyrochlore family and the $AB_2X_4$ spinel family -- are the quintessential 3-dimensional frustrated lattice architecture. While historically oxides ($X =$~O) have played the starring role in this field, the past decade has seen materials synthesis breakthroughs that have lead to the emergence of fluoride ($X =$~F) and chalcogenide ($X =$~S, Se) pyrochlore lattice materials. In this Research Update, we summarize recent progress in understanding the magnetically frustrated ground states in three families of non-oxide pyrochlore lattice materials: (i) $3d$-transition metal fluoride pyrochlores, (ii) rare earth chalcogenide spinels, and (iii) chromium chalcogenide spinels with a breathing pyrochlore lattice. We highlight how the change of anion can modify the single ion spin anisotropy due to crystal electric field effects, stabilize the incorporation of new magnetic elements, and dramatically alter the exchange pathways and thereby lead to new magnetic ground states. We also consider a range of future directions -- materials with the potential to define the next decade of research in frustrated magnetism.

cond-mat.str-el↗

arXiv2019

Intertwined magnetic, structural, and electronic transitions in V$_2$O$_3$

We present a coordinated study of the paramagnetic-to-antiferromagnetic, rhombohedral-to-monoclinic, and metal-to-insulator transitions in thin-film specimens of the classic Mott insulator V$_2$O$_3$ using low-energy muon spin relaxation, x-ray diffraction, and nanoscale-resolved near-field infrared spectroscopic techniques. The measurements provide a detailed characterization of the thermal evolution of the magnetic, structural, and electronic phase transitions occurring in a wide temperature range, including quantitative measurements of the high- and low-temperature phase fractions for each transition. The results reveal a stable coexistence of the high- and low-temperature phases over a broad temperature range throughout the transition. Careful comparison of temperature dependence of the different measurements, calibrated by the resistance of the sample, demonstrates that the electronic, magnetic, and structural degrees of freedom remain tightly coupled to each other during the transition process. We also find evidence for antiferromagnetic fluctuations in the vicinity of the phase transition, highlighting the important role of the magnetic degree of freedom in the metal-insulator transition.

cond-mat.str-el↗

arXiv2019

Kondo exhaustion and conductive surface states in antiferromagnetic YbIr$_3$Si$_7$

The interplay of Kondo screening and magnetic ordering in strongly correlated materials containing local moments is a subtle problem.[1] Usually the number of conduction electrons matches or exceeds the number of moments, and a Kondo-screened heavy Fermi liquid develops at low temperatures.[2] Changing the pressure, magnetic field, or chemical doping can displace this heavy Fermi liquid in favor of a magnetically ordered state.[3,4] Here we report the discovery of a version of such a `Kondo lattice' material, YbIr$_3$Si$_7$, in which the number of free charge carriers is much less than the number of local moments. This leads to `Kondo exhaustion':[5] the electrical conductivity tends to zero at low temperatures as all the free carriers are consumed in the formation of Kondo singlets. This effect coexists with antiferromagnetic long-range order, with a Néel temperature $T\rm_N = 4.1\,{\rm K}$. Furthermore, the material shows conductive surface states with potential topological nature, and thus presents an exciting topic for future investigations.

cond-mat.str-el↗

arXiv2019

Coexistence of metallic and nonmetallic properties in the pyrochlore Lu$_2$Rh$_2$O$_7$

Transition metal oxides of the $4d$ and $5d$ block have recently become the targets of materials discovery, largely due to their strong spin-orbit coupling that can generate exotic magnetic and electronic states. Here we report the high pressure synthesis of Lu$_2$Rh$_2$O$_7$, a new cubic pyrochlore oxide based on $4d^5$ Rh$^{4+}$ and characterizations via thermodynamic, electrical transport, and muon spin relaxation measurements. Magnetic susceptibility measurements reveal a large temperature-independent Pauli paramagnetic contribution, while heat capacity shows an enhanced Sommerfeld coefficient, $γ$ = 21.8(1) mJ/mol-Rh K$^2$. Muon spin relaxation measurements confirm that Lu$_2$Rh$_2$O$_7$ remains paramagnetic down to 2 K. Taken in combination, these three measurements suggest that Lu$_2$Rh$_2$O$_7$ is a correlated paramagnetic metal with a Wilson ratio of $R_W = 2.5$. However, electric transport measurements present a striking contradiction as the resistivity of Lu$_2$Rh$_2$O$_7$ is observed to monotonically increase with decreasing temperature, indicative of a nonmetallic state. Furthermore, although the magnitude of the resistivity is that of a semiconductor, the temperature dependence does not obey any conventional form. Thus, we propose that Lu$_2$Rh$_2$O$_7$ may belong to the same novel class of non-Fermi liquids as the nonmetallic metal FeCrAs.

cond-mat.str-el↗

arXiv2018

Disentangling superconducting and magnetic orders in NaFe_1-xNi_xAs using muon spin rotation

Muon spin rotation and relaxation studies have been performed on a "111" family of iron-based superconductors NaFe_1-xNi_xAs. Static magnetic order was characterized by obtaining the temperature and doping dependences of the local ordered magnetic moment size and the volume fraction of the magnetically ordered regions. For x = 0 and 0.4 %, a transition to a nearly-homogeneous long range magnetically ordered state is observed, while for higher x than 0.4 % magnetic order becomes more disordered and is completely suppressed for x = 1.5 %. The magnetic volume fraction continuously decreases with increasing x. The combination of magnetic and superconducting volumes implies that a spatially-overlapping coexistence of magnetism and superconductivity spans a large region of the T-x phase diagram for NaFe_1-xNi_xAs . A strong reduction of both the ordered moment size and the volume fraction is observed below the superconducting T_C for x = 0.6, 1.0, and 1.3 %, in contrast to other iron pnictides in which one of these two parameters exhibits a reduction below TC, but not both. The suppression of magnetic order is further enhanced with increased Ni doping, leading to a reentrant non-magnetic state below T_C for x = 1.3 %. The reentrant behavior indicates an interplay between antiferromagnetism and superconductivity involving competition for the same electrons. These observations are consistent with the sign-changing s-wave superconducting state, which is expected to appear on the verge of microscopic coexistence and phase separation with magnetism. We also present a universal linear relationship between the local ordered moment size and the antiferromagnetic ordering temperature TN across a variety of iron-based superconductors. We argue that this linear relationship is consistent with an itinerant-electron approach, in which Fermi surface nesting drives antiferromagnetic ordering.

cond-mat.supr-con↗

arXiv2017

Experimental Insights into Ground State Selection of Quantum XY Pyrochlores

Extensive experimental investigations of the magnetic structures and excitations in the XY pyrochlores have been carried out over the last decade. Three families of XY pyrochlores have emerged: Yb$_2B_2$O$_7$, Er$_2B_2$O$_7$, and, most recently, $AA'$Co$_2$F$_7$. In each case, the magnetic cation (either Yb, Er, or Co) exhibits XY anisotropy within the local pyrochlore coordinates, a consequence of crystal field effects. Materials in these families display rich phase behavior and are candidates for exotic ground states, such as quantum spin ice, and exotic ground state selection via order-by-disorder mechanisms. In this review, we present an experimental summary of the ground state properties of the XY pyrochlores, including evidence that they are strongly influenced by phase competition. We empirically demonstrate the signatures for phase competition in a frustrated magnet: multiple heat capacity anomalies, suppressed $T_N$ or $T_C$, sample and pressure dependent ground states, and unconventional spin dynamics.

cond-mat.str-el↗

arXiv2016

Volume-wise destruction of the antiferromagnetic Mott insulating state through quantum tuning

Metal-to-insulator transitions (MITs) are a dramatic manifestation of strong electron correlations in solids1. The insulating phase can often be suppressed by quantum tuning, i.e. varying a nonthermal parameter such as chemical composi- tion or pressure, resulting in a zero-temperature quantum phase transition (QPT) to a metallic state driven by quantum fluctuations, in contrast to conventional phase transitions driven by thermal fluctuations. Theories of exotic phenomena known to occur near the Mott QPT such as quantum criticality and high-temperature superconductivity often assume a second-order QPT, but direct experimental evidence for either first- or second-order behavior at the magnetic QPT associated with the Mott transition has been scarce and further masked by the superconducting phase in unconventional superconductors. Most measurements of QPTs have been performed by volume-integrated probes, such as neutron scattering, magnetization, and transport, in which discontinuous behavior, phase separation, and spatially inhomogeneous responses are averaged and smeared out, leading at times to misidentification as continuous second-order transitions. Here, we demonstrate through muon spin relaxation/rotation (MuSR) experiments on two archetypal Mott insulating systems, composition-tuned RENiO3 (RE=rare earth element) and pressured-tuned V2O3, that the QPT from antiferromagnetic insulator to paramagnetic metal is first-order: the magnetically ordered volume fraction decreases to zero at the QPT, resulting in a broad region of intrinsic phase separation, while the ordered magnetic moment retains its full value across the phase diagram until it is suddenly destroyed at the QPT. These findings call for further investigation into the role of inelastic soft modes and the nature of dynamic spin and charge fluctuations underlying the transition.

cond-mat.str-el↗

arXiv2016

Coexistence of superconductivity and antiferromagnetism in Ca$_{0.74(1)}$La$_{0.26(1)}$(Fe$_{1-x}$Co$_{x}$)As$_{2}$ single crystals

We report the transport, thermodynamic, $μ$SR and neutron study of the Ca$_{0.74(1)}$La$_{0.26(1)}$(Fe$_{1-x}$Co$_{x}$)As$_{2}$ single crystals, mapping out the temperature-doping level phase diagram. Upon Co substitution on the Fe site, the structural/magnetic phase transitions in this 112 compound are suppressed and superconductivity up to 20 K occurs. Our measurements of the superconducting and magnetic volume fractions show that these two phases coexist microscopically in the underdoped region, in contrast to the related 10-3-8 Ca$_{10}$(Pt$_{3}$As$_{8}$)((Fe$_{1-x}$Pt$_x$)$_{2}$As$_{2}$)$_{5}$ compound, where coexistence is absent. Supported by model calculations, we discuss the differences in the phase diagrams of the 112 and 10-3-8 compounds in terms of the FeAs interlayer coupling, whose strength is affected by the character of the spacer layer, which is metallic in the 112 and insulating in the 10-3-8.

cond-mat.supr-con↗