arXiv subjects

Jeffrey W. Lynn

Publications and source records attributed to Jeffrey W. Lynn.

At least 19 recordsLinked to original sources

arXiv2025

Spin-lattice entanglement in $\mathbf{CoPS}_3$

Complex chalcogenides in the $M$PS$_3$ family of materials ($M$ = Mn, Fe, Co, and Ni) display remarkably different phase progressions depending upon the metal center orbital filling, character of the P-P linkage, and size of the van der Waals gap. There is also a stacking pattern and spin state difference between the lighter and heavier transition metal-containing systems that places CoPS$_3$ at the nexus of these activities. Despite these unique properties, this compound is under-explored. Here, we bring together Raman scattering spectroscopy and infrared absorption spectroscopy with X-ray techniques to identify a structural component to the 119 K magnetic ordering transition as well as a remarkable lower temperature set of magnon-phonon pairs that engage in avoided crossings along with a magnetic scattering continuum that correlates with phonon lifetime effects. These findings point to strong spin-phonon entanglement as well as opportunities to control these effects under external stimuli.

cond-mat.str-el↗

arXiv2025

Tuning Incommensurate Charge Order in Ba$_{1-x}$Sr$_x$Al$_4$ and Ba$_{1-y}$Eu$_y$Al$_4$

The BaAl$_4$-type structure family is home to a vast landscape of interesting and exotic properties, with descendant crystal structures hosting a variety of electronic ground states including magnetic, superconducting and strongly correlated electron phenomena. BaAl$_4$ itself hosts a non-trivial topological band structure, but is otherwise a paramagnetic metal. However, the other members of the $A$Al$_4$ family ($A$= alkali earth), including SrAl$_4$ and EuAl$_4$, exhibit symmetry-breaking ground states including charge density wave (CDW) and magnetic orders. Here we investigate the properties of the solid solution series Ba$_{1-x}$Sr$_x$Al$_4$ and Ba$_{1-y}$Eu$_y$Al$_4$ using transport, thermodynamic and scattering experiments to study the evolution of the charge-ordered state as it is suppressed with Ba substitution to zero near 50% substitution in both systems. Neutron and x-ray diffraction measurements reveal an incommensurate CDW state in SrAl$_4$ with $c$-axis-oriented ordering vector (0, 0, 0.097) that evolves with Ba substitution toward a shorter wavelength. A similar progression is observed in the Ba$_{1-y}$Eu$_y$Al$_4$ series that also scales with the ordering temperature, revealing a universal correlation between charge-order transition temperature and ordering vector that points to a critical wavevector that stabilizes CDW order in both systems. We study the evolution of the phonon band structure in the Ba$_{1-x}$Sr$_x$Al$_4$ system, revealing the suppression of the CDW phase matches the suppression of a phonon instability at precisely the same momentum as observed in experiments, confirming the electron-phonon origin of charge order in this system.

cond-mat.str-el↗

arXiv2024

Anomalous Hall effect in the antiferromagnetic Weyl semimetal SmAlSi

The intrinsic anomalous Hall effect (AHE) has been reported in numerous ferromagnetic (FM) Weyl semimetals. However, AHE in the antiferromagnetic (AFM) or paramagnetic (PM) state of Weyl semimetals has been rarely observed experimentally, and only in centrosymmetric materials. Different mechanisms have been proposed to establish the connection between the AHE and the type of magnetic order. In this paper, we report AHE in both the AFM and PM states of non-centrosymmetric compound SmAlSi. To account for the AHE in non-centrosymmetric Weyl semimetals without FM, we introduce a new mechanism based on magnetic field-induced Weyl nodes evolution. Angle-dependent quantum oscillations in SmAlSi provide evidence for the Weyl points and large AHE in both the PM and the AFM states. The proposed mechanism qualitatively explains the temperature dependence of the anomalous Hall conductivity (AHC), which displays unconventional power law behavior of the AHC in both AFM and PM states of SmAlSi.

cond-mat.mtrl-sci↗

arXiv2023

Non-collinear 2k antiferromagnetism in the Zintl semiconductor Eu$_5$In$_2$Sb$_6$

Eu$_5$In$_2$Sb$_6$ is an orthorhombic non-symmorphic small band gap semiconductor with three distinct Eu$^{2+}$ sites and two low-temperature magnetic phase transitions. The material displays one of the greatest (negative) magnetoresistances of known stoichiometric antiferromagnets and belongs to a family of Zintl materials that may host an axion insulator. Using single crystal neutron diffraction, we show that the $T_{\mathrm{N1}}=14\mathrm{~K}$ second-order phase transition is associated with long-range antiferromagnetic order within the chemical unit cell $\left( k_1 = (000) \right)$. Upon cooling below $T_{\mathrm{N1}}$, the relative sublattice magnetizations of this structure vary until a second-order phase transition at $T_{\mathrm{N2}}=7\mathrm{~K}$ that doubles the unit cell along the $\hat{c}$ axis $\left( k_2 = \left(00\frac{1}{2}\right) \right)$. We show the anisotropic susceptibility and our magnetic neutron diffraction data are consistent with magnetic structures described by the $Γ_3$ irreducible representation with the staggered magnetization of the $k_1$ and $k_2$ components polarized along the $\hat{b}$ and $\hat{a}$ axis, respectively. As the $k_2$ component develops, the amplitude of the $k_1$ component is reduced, which indicates a 2k non-collinear magnetic structure. Density functional theory is used to calculate the energies of these magnetic structures and to show the $k_1$ phase is a metal so $T_{\mathrm{N1}}$ is a rare example of a unit-cell-preserving second-order phase transition from a paramagnetic semiconductor to an antiferromagnetic metal. DFT indicates the transition at $T_{\mathrm{N2}}$ to a doubled unit cell reduces the carrier density of the metal, which is consistent with resistivity data.

cond-mat.str-el↗

arXiv2023

Post deposition interfacial Néel temperature tuning in magnetoelectric B:Cr2O3

Boron (B) alloying transforms the magnetoelectric antiferromagnet Cr2O3 into a multifunctional single-phase material which enables electric field driven π/2 rotation of the Néel vector. Nonvolatile, voltage-controlled Néel vector rotation is a much-desired material property in the context of antiferromagnetic spintronics enabling ultra-low power, ultra-fast, nonvolatile memory, and logic device applications. Néel vector rotation is detected with the help of heavy metal (Pt) Hall-bars in proximity of pulsed laser deposited B:Cr2O3 films. To facilitate operation of B:Cr2O3-based devices in CMOS environments, the Néel temperature, TN, of the functional film must be tunable to values significantly above room temperature. Cold neutron depth profiling and x-ray photoemission spectroscopy depth profiling reveal thermally activated B-accumulation at the B:Cr2O3/ vacuum interface in thin films deposited on Al2O3 substrates. We attribute the B-enrichment to surface segregation. Magnetotransport data confirm B-accumulation at the interface within a layer of about 50 nm thick where the device properties reside. Here TN enhances from 334 K prior to annealing, to 477 K after annealing for several hours. Scaling analysis determines TN as a function of the annealing temperature. Stability of post-annealing device properties is evident from reproducible Néel vector rotation at 370 K performed over the course of weeks.

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↗

arXiv2022

Frustrated magnetic interactions and quenched spin fluctuations in CrAs

The discovery of pressure-induced superconductivity in helimagnets (CrAs, MnP) has attracted considerable interest in understanding the relationship between complex magnetism and unconventional superconductivity. However, the nature of the magnetism and magnetic interactions that drive the unusual double-helical magnetic order in these materials remains unclear. Here, we report neutron scattering measurements of magnetic excitations in CrAs single crystals at ambient pressure. Our experiments reveal well defined spin wave excitations up to about 150 meV with a pseudogap below 7 meV, which can be effectively described by the Heisenberg model with nearest neighbor exchange interactions. Most surprisingly, the spin excitations are largely quenched above the Neel temperature, in contrast to cuprates and iron pnictides where the spectral weight is mostly preserved in the paramagnetic state. Our results suggest that the helimagnetic order is driven by strongly frustrated exchange interactions, and that CrAs is at the verge of itinerant and correlation-induced localized states, which is therefore highly pressure-tunable and favorable for superconductivity.

cond-mat.supr-con↗

arXiv2022

Magnetic ground state of the Kitaev Na$_2$Co$_2$TeO$_6$ spin liquid candidate

As a candidate Kitaev material, Na$_2$Co$_2$TeO$_6$ exhibits intriguing magnetism on a honeycomb lattice that is believed to be $C_3$-symmetric. Here we report a neutron diffraction study of high quality single crystals under $a$-axis magnetic fields. Our data support the less common notion of a magnetic ground state that corresponds to a triple-$\mathbf{q}$ magnetic structure with $C_3$ symmetry, rather than the multi-domain zigzag structure typically assumed in prototype Kitaev spin liquid candidates. In particular, we find that the field is unable to repopulate the supposed zigzag domains, where the only alternative explanation is that the domains are strongly pinned by hitherto unidentified structural reasons. If the triple-$\mathbf{q}$ structure is correct then this requires reevaluation of many candidate Kitaev materials. We also find that fields beyond about 10 Tesla suppress the long range antiferromagnetic order, allowing new magnetic behavior to emerge different from that expected for a spin liquid.

cond-mat.str-el↗

arXiv2022

Incommensurate magnetic orders and topological Hall effect in the square-net centrosymmetric EuGa$_2$Al$_2$ system

Neutron diffraction on the centrosymmetric square-net magnet EuGa$_2$Al$_2$ reveals multiple incommensurate magnetic states (AFM1,2,3) in zero field. In applied field, a new magnetic phase (A) is identified from magnetization and transport measurements, bounded by two of the $μ_0H$~=~0 incommensurate magnetic phases (AFM1,helical and AFM3, cycloidal) with different moment orientations. Moreover, magneto-transport measurements indicate the presence of a topological Hall effect, with maximum values centered in the A phase. Together, these results render EuGa$_2$Al$_2$ a material with non-coplanar or topological spin texture in applied field. X-ray diffraction reveals an out-of-plane (OOP) charge density wave (CDW) below $T_{CDW} \sim$ 50 K while the magnetic propagation vector lies in plane below $T_N$ = 19.5 K. Together these data point to a new route to realizing in-plane non-collinear spin textures through an OOP CDW. In turn, these non-collinear spin textures may be unstable against the formation of topological spin textures in an applied field.

cond-mat.str-el↗

arXiv2022

Absence of precursor incommensurate charge order in electronic nematic Ba0.35Sr0.65Ni2As2

Recent discoveries of charge order and electronic nematic order in the iron-based superconductors and cuprates have pointed towards the possibility of nematic and charge fluctuations playing a role in the enhancement of superconductivity. The Ba1-xSrxNi2As2 system, closely related in structure to the BaFe2As2 system, has recently been shown to exhibit both types of ordering without the presence of any magnetic order. We report single crystal X-ray diffraction, resistance transport measurements, and magnetization of \BaSrLate, providing evidence that the previously reported incommensurate charge order with wavevector $(0,0.28,0)_{tet}$ in the tetragonal state of \BaNi~vanishes by this concentration of Sr substitution together with nematic order. Our measurements suggest that the nematic and incommensurate charge orders are closely tied in the tetragonal state, and show that the $(0,0.33,0)_{tri}$ charge ordering in the triclinic phase of BaNi2As2 evolves to become $(0,0.5,0)_{tri}$ charge ordering at $x$=0.65 before vanishing at $x$=0.71.

cond-mat.str-el↗

arXiv2022

Effect of iron vacancies on the magnetic order and spin dynamics of the spin ladder BaFe$_{2-δ}$S$_{1.5}$Se$_{1.5}$

Quasi-one-dimensional iron chalcogenides possess various magnetic states depending on the lattice distortion, electronic correlations, and presence of defects. We present neutron diffraction and inelastic neutron scattering experiments on the spin ladder compound BaFe$_{2-δ}$S$_{1.5}$Se$_{1.5}$ with $\sim$6% iron vacancies. The data reveal that long-range magnetic order is absent, while the characteristic magnetic excitations that correspond to both the stripe- and block-type antiferromagnetic correlations are observed. First-principles calculations support the existence of both stripe and block-type antiferromagnetic short-range order in the experimental sample. The disappearance of long-range magnetic order may be due to the competition between these two magnetic orders, which is greatly enhanced for a certain concentration of iron vacancies, which we calculate to be about 6%, consistent with the measured iron vacancy concentration. Our results highlight how iron vacancies in the iron-based spin ladder system strongly influence the magnetic ground state.

cond-mat.supr-con↗

arXiv2021

Phase Diagram of YbZnGaO4 in Applied Magnetic Field

Recently, Yb-based triangular lattice antiferromagnets have garnered significant interest as possible quantum spin liquid candidates. One example is YbMgGaO4, which showed many promising spin liquid features, but also possesses a high degree of disorder owing to site-mixing between the non-magnetic cations. To further elucidate the role of chemical disorder and to explore the phase diagram of these materials in applied field, we present neutron scattering and sensitive magnetometry measurements of the closely related compound, YbZnGaO4. Our results suggest a difference in magnetic anisotropy between the two compounds, and we use key observations of the magnetic phase crossover to motivate an exploration of the field- and exchange parameter-dependent phase diagram, providing an expanded view of the available magnetic states in applied field. This enriched map of the phase space serves as a basis to restrict the values of parameters describing the magnetic Hamiltonian with broad application to recently discovered related materials.

cond-mat.str-el↗

arXiv2021

Universal dynamics of magnetic monopoles in two-dimensional kagomé ice

A magnetic monopole in spin ice is a novel quasiparticle excitation in condensed matter physics, and we found that the ac frequency dependent magnetic susceptibility $χ(ω)$ in the two-dimensional (2D) spin ice (so-called kagomé ice) of Dy$_2$Ti$_2$O$_7$ shows a single scaling form. This behavior can be understood in terms of the dynamical scaling law for 2D Coulomb gas (CG) systems [Phys. Rev. B 90, 144428 (2014)], characterized by the charge correlation length $ξ(\propto1/\sqrt{ω_1})$, where $ω_{1}$ is a characteristic frequency proportional to the peak position of the imaginary part of $χ(ω)$. It is a generic behavior among a wide variety of models such as the vortex dynamics of 2D superconductors, 2D superfluids, classical XY magnets, and dynamics of melting of Wigner crystals.

cond-mat.other↗

arXiv2020

Chiral properties of the zero-field spiral state and field-induced magnetic phases of the itinerant kagome metal YMn$_6$Sn$_6$

Applying a magnetic field in the hexagonal plane of YMn$_6$Sn$_6$ leads to a complex magnetic phase diagram of commensurate and incommensurate phases, one of which coexists with the topological Hall effect (THE) generated by a unique fluctuation-driven mechanism. Using unpolarized neutron diffraction, we report on the solved magnetic structure for two previously identified, but unknown, commensurate phases. These include a low-temperature, high-field fan-like phase and a room-temperature, low-field canted antiferromagnetic phase. An intermediate incommensurate phase between the fan-like and forced ferromagnetic phases is also identified as the last known phase of the in-plane field-temperature diagram. Additional characterization using synchrotron powder diffraction reveals extremely high-quality, single-phase crystals, which suggests that the presence of two incommensurate magnetic structures throughout much of the phase diagram is an intrinsic property of the system. Interestingly, polarized neutron diffraction shows that the centrosymmetric system hosts preferential chirality in the zero-field double-flat-spiral phase, which, along with the THE, is a topologically non-trivial characteristic.

cond-mat.str-el↗

arXiv2020

Magnetic Order and Competition With Superconductivity in (Er-Ho)Ni$_{2}$B$_{2}$C

The rare earth magnetic order in pure and doped Er$_{(1-x)}$Ho$_{x}$Ni$_2$B$_2$C (x~=~0,~0.25,~0.50,~0.75,~1) single crystal samples was investigated using magnetization and neutron diffraction measurements. Superconducting quaternary borocarbides, $R$Ni$_2$B$_2$C where R~=~Er, Ho , are both magnetic intermetallic superconductors with the transition temperatures $\sim$ 10 K. These compounds also develop magnetic order in the vicinity of this temperature. Depending on the rare earth composition the coupling between superconductivity and magnetism creates several phases, ranging from a reentrant superconductor with a mixture of commensurate and incommensurate antiferromagnetism to a total incommensurate antiferromagnetic spin modulation with a weak ferromagnetic state. All of these phases coexist with superconductivity. RKKY magnetic interactions are used to describe the magnetic orders in the pure compounds. However, the doping of Ho on Er (or Er on Ho) sites which have two strong magnetic moments with two different easy directions creates new and complicated magnetic modulations with possible local disorder effects. One fascinating effect is the development of an induced magnetic state resembling the pure and doped $R_2$CuO$_4$, R~=~Nd and Pr.

cond-mat.supr-con↗

arXiv2020

Novel magnetic states and nematic spin chirality in the kagome lattice metal YMn$_{6}$Sn$_{6}$

Identification, understanding, and manipulation of novel magnetic textures is essential for the discovery of new quantum materials for future spin-based electronic devices. In particular, materials that manifest a large response to external stimuli such as a magnetic field are subject to intense investigation. Here, we study the kagome-net magnet YMn$_{6}$Sn$_{6}$ by magnetometry, transport, and neutron diffraction measurements combined with first principles calculations. We identify a number of nontrivial magnetic phases, explain their microscopic nature, and demonstrate that one of them hosts a large topological Hall effect (THE). We propose a new nematic chirality mechanism, reminiscent of the nematicity in Fe-based superconductors, which leads to the THE at elevated temperatures. This interesting physics comes from parametrically frustrated interplanar exchange interactions that trigger strong magnetic fluctuations. Our results pave a path to new chiral spin textures, promising for novel spintronics.

cond-mat.str-el↗

arXiv2020

Magnetic phase transitions and spin density distribution in the molecular multiferroic GaV$_4$S$_8$ system

We have carried out neutron diffraction and small angle neutron scattering measurements on a high quality single crystal of the cubic lacunar spinel multiferroic, GaV$_4$S$_8$, as a function of magnetic field and temperature to determine the magnetic properties for the single electron that is located on the tetrahedrally coordinated V$_4$ molecular unit. Our results are in good agreement with the structural transition at 44 K from cubic to rhombohedral symmetry where the system becomes a robust ferroelectric, while long range magnetic order develops below 13 K in the form of an incommensurate cycloidal magnetic structure, which can transform into a Néel-type skyrmion phase in a modest applied magnetic field. Below 5.9(3) K, the crystal enters a ferromagnetic phase, and we find the magnetic order parameter indicates a long range ordered ground state with an ordered moment of 0.23(1) $μ_\mathrm{B}$ per V ion. Both polarized and unpolarized neutron data in the ferroelectric-paramagnetic phase have been measured to determine the magnetic form factor. The data are consistent with a model of the single spin being uniformly distributed across the V$_4$ molecular unit, rather than residing on the single apical V ion, in substantial agreement with the results of first-principles theory. In the magnetically ordered state, polarized neutron measurements are important since both the cycloidal and ferromagnetic order parameters are clearly coupled to the ferroelectricity, causing the structural peaks to be temperature and field dependent. For the ferromagnetic ground state, the spins are locked along the $[1,1,1]$ direction by a surprisingly large anisotropy.

cond-mat.str-el↗

arXiv2020

Correlating magnetic structure and magnetotransport in semimetal thin films of Eu$_{1-x}$Sm$_x$TiO$_3$

We report on the evolution of the average and depth-dependent magnetic order in thin film samples of biaxially stressed and electron-doped EuTiO$_3$ for samples across a doping range $<$0.1 to 7.8 $\times 10^{20}$ cm$^{-3}$. Under an applied in-plane magnetic field, the G-type antiferromagnetic ground state undergoes a continuous spin-flop phase transition into in-plane, field-polarized ferromagnetism. The critical field for ferromagnetism slightly decreases with an increasing number of free carriers, yet the field evolution of the spin-flop transition is qualitatively similar across the doping range. Unexpectedly, we observe interfacial ferromagnetism with saturated Eu$^{2+}$ moments at the substrate interface at low fields preceding ferromagnetic saturation throughout the bulk of the degenerate semiconductor film. We discuss the implications of these findings for the unusual magnetotransport properties of this compound.

cond-mat.str-el↗