arXiv subjects

T. Siegrist

Publications and source records attributed to T. Siegrist.

At least 19 recordsLinked to original sources

arXiv2024

Tomographic Imaging of Orbital Vortex Lines in Three-Dimensional Momentum Space

We report the experimental discovery of orbital vortex lines in the three-dimensional (3D) band structure of a topological semimetal. Combining linear and circular dichroism in soft x-ray angle-resolved photoemission (SX-ARPES) with first-principles theory, we image the winding of atomic orbital angular momentum, thereby revealing - and determining the location of - lines of vorticity in full 3D momentum space. Our observation of momentum-space vortex lines with quantized winding number establishes an analogue to real-space quantum vortices, for instance, in type-II superconductors and certain non-collinear magnets. These results establish multimodal dichroism in SX-ARPES as an approach to trace 3D orbital textures. Our present findings particularly constitute the first imaging of non-trivial quantum-phase winding at line nodes and may pave the way to new orbitronic phenomena in quantum materials

cond-mat.str-el↗

arXiv2023

Momentum-space signatures of Berry flux monopoles in a Weyl semimetal

Since the early days of Dirac flux quantization, magnetic monopoles have been sought after as a potential corollary of quantized electric charge. As opposed to magnetic monopoles embedded into the theory of electromagnetism, Weyl crystals exhibit Berry flux monopoles in reciprocal parameter space. As a function of crystal momentum, such monopoles locate at the degeneracy point of the Weyl cone. Here, we report momentum-resolved spectroscopic signatures of Berry flux monopoles in TaAs as a paradigmatic Weyl semimetal. We have probed the orbital and spin angular momentum (OAM and SAM) of the Weyl-fermion states by angle-resolved photoemission spectroscopy at bulk-sensitive soft X-ray energies (SX-ARPES) combined with photoelectron spin detection and circular dichroism. Supported by first-principles calculations, our measurements image characteristics of a topologically non-trivial winding of the OAM at the Weyl nodes and unveil a chirality-dependent SAM of the Weyl bands. Our results experimentally visualize the non-trivial momentum-space topology in a Weyl semimetal, promising to have profound implications for the study of quantum-geometric effects in solids.

cond-mat.mtrl-sci↗

arXiv2022

The Geometrically Frustrated Spin Glass (Fe1-pGap)2TiO5

The unusual anisotropy of the spin glass transition in the pseudobrookite system Fe$_2$TiO$_5$ has been interpreted as arising from an induced, van der Waals-like, interaction among magnetic clusters. Here we present susceptibility ($χ$) and specific heat data (C) for Fe2TiO5 diluted with non-magnetic Ga, (Fe$_{1-p}$Ga$_p$)$_2$TiO$_5$, for disorder parameter p = 0, 0.11, and 0.42, and elastic neutron scattering data for p = 0.20. A uniform suppression of T{_g} is observed upon increasing p, along with a value of $χ(T_g)$ that increases as T$_g$ decreases, i.e. $dχ(T_g)/dT_g< 0$. We also observe C(T) $\propto$ T$^2$ in the low temperature limit. The observed behavior places (Fe$_{1-p}$Ga$_p$)$_2$TiO$_5$ in the category of a strongly geometrically frustrated spin glass.

cond-mat.dis-nn↗

arXiv2021

A phase diagram for light-induced superconductivity in $κ$-(ET)$_2$-X

Resonant optical excitation of certain molecular vibrations in $κ$-(BEDT-TTF)$_2$Cu[N(CN)$_2$]Br has been shown to induce transient superconducting-like optical properties at temperatures far above equilibrium $T_c$. Here, we report experiments across the bandwidth-tuned phase diagram of this class of materials, and study the Mott insulator $κ$-(BEDT-TTF)$_2$Cu[N(CN)$_2$]Cl and the metallic compound $κ$-(BEDT-TTF)$_2$Cu(NCS)$_2$. We find non-equilibrium photoinduced superconductivity only in $κ$-(BEDT-TTF)$_2$Cu[N(CN)$_2$]Br, indicating that the proximity to the Mott insulating phase and possibly the presence of preexisting superconducting fluctuations are pre-requisites for this effect.

cond-mat.supr-con↗

arXiv2020

Fluctuation-Induced Interactions and the Spin Glass Transition in $Fe_2TiO_5$

We investigate the spin-glass transition in the strongly frustrated well-known compound $Fe_2TiO_5$. A remarkable feature of this transition, widely discussed in the literature, is its anisotropic properties: the transition manifests itself in the magnetic susceptibly only along one axis, despite $Fe^{3+}$ $d^5$ spins having no orbital component. We demonstrate, using neutron scattering, that below the transition temperature $T_g = 55 K$, $Fe_2TiO_5$ develops nanoscale surfboard shaped antiferromagnetic regions in which the $Fe^{3+}$ spins are aligned perpendicular to the axis which exhibits freezing. We show that the glass transition may result from the freezing of transverse fluctuations of the magnetization of these regions and we develop a mean-field replica theory of such a transition, revealing a type of magnetic van der Waals effect.

cond-mat.dis-nn↗

arXiv2020

Layer- and Gate-tunable Spin-Orbit Coupling in a High Mobility Few-Layer Semiconductor

Spin-orbit coupling (SOC) is a relativistic effect, where an electron moving in an electric field experiences an effective magnetic field in its rest frame. In crystals without inversion symmetry, it lifts the spin degeneracy and leads to many magnetic, spintronic and topological phenomena and applications. In bulk materials, SOC strength is a constant that cannot be modified. Here we demonstrate SOC and intrinsic spin-splitting in atomically thin InSe, which can be modified over an unprecedentedly large range. From quantum oscillations, we establish that the SOC parameter αis thickness-dependent; it can be continuously modulated over a wide range by an out-of-plane electric field, achieving intrinsic spin splitting tunable between 0 and 20 meV. Surprisingly, αcould be enhanced by an order of magnitude in some devices, suggesting that SOC can be further manipulated. Our work highlights the extraordinary tunability of SOC in 2D materials, which can be harnessed for in operando spintronic and topological devices and applications.

cond-mat.mes-hall↗

arXiv2020

Magnetostriction of AlFe2B2 in High Magnetic Fields

Using the experimental capability of the novel X-ray diffraction instrument available at the 25 Tesla Florida Split Coil Magnet at the NHMFL, Tallahassee we present an extensive investigation on the magnetostriction of polycrystalline AlFe2B2. The magnetostriction was measured near the ferromagnetic transition temperature (Curie temperature TC = 280 K, determined via DC magnetization measurements), namely, at 250, 290, and 300 K. AlFe2B2 exhibits an anisotropic change in lattice parameters as a function of magnetic field near the Curie temperature, and a monotonic variation as a function of applied field has been observed, i.e., the c-axis increases significantly while the a- and b-axes decrease with the increasing field in the vicinity of TC, irrespective of the measurement temperature. The volume magnetostriction decreases with decreasing temperature and changes its sign across TC. Density functional theory calculations for the non-polarized and spin-polarized (ferromagnetic) models confirm that the observed changes in lattice parameters due to spin polarization are consistent with the experiment. The relationships for magnetostriction are estimated based on a simplified Landau model that agrees well with the experimental results.

cond-mat.mtrl-sci↗

arXiv2020

Tuning the structural and antiferromagnetic phase transitions in UCr$_{2}$Si$_2$: hydrostatic pressure and chemical substitution

Structural phase transitions in $f$-electron materials have attracted sustained attention both for practical and basic science reasons, including that they offer an environment to directly investigate relationships between structure and the $f$-state. Here we present results for UCr$_2$Si$_2$, where structural (tetragonal $\rightarrow$ monoclinic) and antiferromagnetic phase transitions are seen at $T_{\rm{S}}$ $=$ 205 K and $T_{\rm{N}}$ $=$ 25 K, respectively. We also provide evidence for an additional second order phase transition at $T_{\rm{X}}$ = 280 K. We show that $T_{\rm{X}}$, $T_{\rm{S}}$, and $T_{\rm{N}}$ respond in distinct ways to the application of hydrostatic pressure and Cr $\rightarrow$ Ru chemical substitution. In particular, hydrostatic compression increases the structural ordering temperature, eventually causes it to merge with $T_{\rm{X}}$ and destroys the antiferromagnetism. In contrast, chemical substitution in the series UCr$_{2-x}$Ru$_x$Si$_2$ suppresses both $T_{\rm{S}}$ and $T_{\rm{N}}$, causing them to approach zero temperature near $x$ $\approx$ 0.16 and 0.08, respectively. The distinct $T-P$ and $T-x$ phase diagrams are related to the evolution of the rigid Cr-Si and Si-Si substructures, where applied pressure semi-uniformly compresses the unit cell and Cr $\rightarrow$ Ru substitution results in uniaxial lattice compression along the tetragonal $c$-axis and an expansion in the $ab$-plane. These results provide insights into an interesting class of strongly correlated quantum materials where degrees of freedom associated with $f$-electron magnetism, strong electronic correlations, and structural instabilities are readily controlled.

cond-mat.str-el↗

arXiv2020

Quantum critical point in the itinerant ferromagnet Ni$_{1-x}$Rh$_x$

We report a chemical substitution-induced ferromagnetic quantum critical point in polycrystalline Ni$_{1-x}$Rh$_x$ alloys. Through magnetization and muon spin relaxation measurements, we show that the ferromagnetic ordering temperature is suppressed continuously to zero at $x_{crit} = 0.375$ while the magnetic volume fraction remains 100% up to $x_{crit}$, pointing to a second order transition. Non-Fermi liquid behavior is observed close to $x_{crit}$, where the electronic specific heat $C_{el}/T$ diverges logarithmically, while immediately above $x_{crit}$ the volume thermal expansion coefficient $α_{V}/T$ and the Grüneisen ratio $Γ= α_{V}/C_{el}$ both diverge logarithmically in the low temperature limit, further indication of a ferromagnetic quantum critical point in Ni$_{1-x}$Rh$_x$.

cond-mat.str-el↗

arXiv2020

Photo-molecular high temperature superconductivity

Superconductivity in organic conductors is often tuned by the application of chemical or external pressure. With this type of tuning, orbital overlaps and electronic bandwidths are manipulated, whilst the properties of the molecular building blocks remain virtually unperturbed.Here, we show that the excitation of local molecular vibrations in the charge-transfer salt $κ-(BEDT-TTF)_2Cu[N(CN)_2]Br$ induces a colossal increase in carrier mobility and the opening of a superconducting-like optical gap. Both features track the density of quasi-particles of the equilibrium metal, and can be achieved up to a characteristic coherence temperature $T^* \approxeq 50 K$, far higher than the equilibrium transition temperature $T_C = 12.5 K$. Notably, the large optical gap achieved by photo-excitation is not observed in the equilibrium superconductor, pointing to a light induced state that is different from that obtained by cooling. First-principle calculations and model Hamiltonian dynamics predict a transient state with long-range pairing correlations, providing a possible physical scenario for photo-molecular superconductivity.

cond-mat.supr-con↗

arXiv2019

Evidence for Undoped Weyl Semimetal Charge Transport in $Y_{2}Ir_{2}O_{7}$

Weyl fermions scattering from a random Coulomb potential are predicted to exhibit resistivity versus temperature $ρ\space α\space T^{-4}$ in a single particle model. Here we show that, in closed environment-grown polycrystalline samples of $Y_{2}Ir_{2}O_{7}$, $ρ= ρ_{0} T^{-4}$ over four orders of magnitude in $ρ$. While the measured prefactor, $ρ_{0}$, is obtained from the model using reasonable materials parameters, the $T^{-4}$ behavior extends far beyond the model's range of applicability. In particular, the behavior extends into the low-temperature, high-resistivity region where the Ioffe-Regel parameter, $k_{T} \ell \ll 2π$. Strong on-site Coulomb correlations, instrumental for predicting a Weyl semimetal state in $Y_{2}Ir_{2}O_{7}$, are the possible origin of such "bad" Weyl semimetal behavior.

cond-mat.str-el↗

arXiv2018

Weak ferromagnetism and glassy state in kappa-(BEDT-TTF)2Hg(SCN)2Br

Since the first observation of weak ferromagnetism in the charge-transfer salt kappa-(BEDT-TTF)2-Cu[N(CN)2]Cl [U. Welp et al., Phys. Rev. Lett. 69, 840 (1992)], no further evidence of ferromagnetism in this class of organic materials has been reported. Here we present static and dynamic spin susceptibility measurements on kappa-(BEDT-TTF)2Hg(SCN)2Br revealing weak ferromagnetism below about TWF = 20 K. We suggest that frustrated spins in the molecular dimers suppress long-range order, forming a spin-glass ground state in the insulating phase.

cond-mat.str-el↗

arXiv2018

Effects of chemical disorder in the itinerant antiferromagnet Ti$_{1-x}$V$_x$Au

The fragile nature of itinerant magnetism can be exploited using non-thermal parameters to study quantum criticality. The recently discovered quantum critical point (QCP) in the Sc-doped (hole-like doping) itinerant antiferromagnet TiAu (Ti$_{1-x}$Sc$_{x}$Au) raised questions about the effects of the crystal and electronic structures on the overall magnetic behavior. In this study, doping with V (electron-like doping) in Ti$_{1-x}$V$_{x}$Au introduces chemical disorder which suppresses antiferromagnetic order from $T_{\rm N} =$ 36~K for $x = 0$ down to 10 K for $x =$ 0.15, whereupon a solubility limit is reached. Signatures of non-Fermi-liquid behavior are observed in transport and specific heat measurements similar to Ti$_{1-x}$Sc$_{x}$Au, even though Ti$_{1-x}$V$_{x}$Au is far from a QCP for the accessible compositions $x \leq 0.15$.

cond-mat.str-el↗

arXiv2017

Possible devil's staircase in the Kondo lattice CeSbSe

The temperature ($T$) - magnetic field ($H$) phase diagram for the tetragonal layered compound CeSbSe, is determined from magnetization, specific heat, and electrical resistivity measurements. This system exhibits complex magnetic ordering at $T_{\rm{M}}$ $=$ 3 K and the application of a magnetic field results in a cascade of magnetically ordered states for $H$ $\lesssim$ 1.8 T which are characterized by fractional integer size steps: i.e., a possible Devil's staircase is observed. Electrical transport measurements show a weak temperature dependence and large residual resistivity which suggest a small charge carrier density and strong scattering from the $f$-moments. These features reveal Kondo lattice behavior where the $f$-moments are incompletely screened, resulting in a fine balanced magnetic interaction between different Ce neighbors that is mediated by the RKKY interaction. This produces the nearly degenerate magnetically ordered states that are accessed under an applied magnetic field.

cond-mat.str-el↗

arXiv2017

Electronic Landscape of Ce-based Intermetallics: CeCu$_2$Si$_2$ at an Extreme

CeCu$_2$Si$_2$ is an exemplary correlated electron metal that features two domes of unconventional superconductivity in its temperature-pressure phase diagram. The first dome surrounds an antiferromagnetic quantum critical point, whereas the more exotic second dome may span the termination point of a line of $f$-electron valence transitions. This behavior has received intense interest, but what has been missing are ways to access the high pressure behavior under milder conditions. Here we study Si $\rightarrow$ P chemical substitution, which compresses the unit cell volume but simultaneously weakens the hybridization between the $f$- and conduction electron states and encourages complex magnetism. At concentrations that show magnetism, applied pressure suppresses the magnetic ordering temperature and superconductivity is recovered for samples with low disorder. These results reveal that the electronic behavior in this system is controlled by a nontrivial combination of effects from unit cell volume and electronic shell filling. Guided by this topography we discuss prospects for uncovering a valence fluctuation quantum phase transition in the broader family of Ce-based ThCr$_2$Si$_2$-type materials through chemical substitution.

cond-mat.str-el↗

arXiv2017

Electronic Structure and Magnetism in the Layered Triangular Lattice Compound CeAuAl$_4$Ge$_2$

Results are reported for the $f$-electron intermetallic CeAuAl$_4$Ge$_2$, where the atomic arrangement of the cerium ions creates the conditions for geometric frustration. Despite this, magnetic susceptibility measurements reveal that the low temperature magnetic exchange interaction is weak, resulting in marginally frustrated behavior and ordering near $T_{\rm{M}}$ $\approx$ 1.4 K. This occurs within a metallic Kondo lattice, where electrical resistivity and heat capacity measurements show that the Kondo-driven electronic correlations are negligible. Quantum oscillations are detected in ac-magnetic susceptibility measurements and uncover small charge carrier effective masses. Electronic structure calculations reveal that when the experimentally observed antiferromagnetic exchange interaction and the on-$f$-site Coulomb repulsion (Hubbard) U are considered, the $f$-electron bands move away from the Fermi level, resulting in electronic behavior that is dominated by the $s$-, $p$-, and $d$- bands, which are all characterized by light electron masses. Thus, CeAuAl$_4$Ge$_2$ provides a starting point for investigating geometric magnetic frustration in a cerium lattice without strong Kondo hybridization, where calculations provide useful guidance.

cond-mat.mtrl-sci↗

arXiv2016

Uncovering the behavior of Hf2Te2P and the candidate Dirac metal Zr2Te2P

Results are reported for single crystal specimens of Hf$_2$Te$_2$P and compared to its structural analogue Zr$_2$Te$_2$P, which was recently proposed to be a potential reservoir for Dirac physics.[1] Both materials are produced using the iodine vapor transport method and the resulting crystals are exfoliable. The bulk electrical transport and thermodynamic properties indicate Fermi liquid behavior at low temperature for both compounds. Quantum oscillations are observed in magnetization measurements for fields applied parallel but not perpendicular to the $c$-axis, suggesting that the Fermi surfaces are quasi-two dimensional. Frequencies are determined from quantum oscillations for several parts of the Fermi surfaces. Lifshitz-Kosevich fits to the temperature dependent amplitudes of the oscillations reveal small effective masses, with a particularly small value $m^*$ $=$ 0.046$m_0$ for the α branch of Zr$_2$Te$_2$P. Electronic structure calculations are in good agreement with quantum oscillation results and illustrate the effect of a stronger spin-orbit interaction going from Zr to Hf. These results suggest that by using appropriate tuning parameters this class of materials may deepen the pool of novel Dirac phenomena.

cond-mat.mtrl-sci↗

arXiv2015

Temperature - Pressure phase diagram of the cubic Laves phase Au$_2$Pb

The temperature ($T$) as a function of pressure ($P$) phase diagram is reported for the cubic Laves phase compound Au$_2$Pb, which was recently proposed to support linearly dispersing "topological" bands, together with conventional quadratic bands. At ambient pressure, Au$_2$Pb exhibits several structural phase transitions at $T_1$ $=$ 97 K, $T_2$ $=$ 51 K, and $T_3$ $=$ 40 K with superconductivity below $T_{\rm{c}}$ $=$ 1.2 K. Applied pressure results in a rich phase diagram where $T_1$, $T_2$, and $T_3$ evolve strongly with $P$ and a new phase is stabilized for $P$ $>$ 0.64 GPa that also supports superconductivity below 1.1 K. These observations suggest that Au$_2$Pb is an ideal system in which to investigate the relationship between structural degrees of freedom, band topology, and resulting anomalous behaviors.

cond-mat.mtrl-sci↗