arXiv subjects

Michael J. Graf

Publications and source records attributed to Michael J. Graf.

15 recordsLinked to original sources

arXiv2025

Magnetic dilution in the triangular lattice antiferromagnet NaYb$_{1-x}$Lu$_{x}$O$_2$

The delafossite-like compound NaYbO$_2$ hosts a triangular lattice of Yb$^{3+}$ moments and is a promising candidate for the realization of a quantum spin liquid ground state -- an exotic, quantum-disordered magnetic phase featuring long-range entanglement of spins. Tuning this system away from this quantum-disordered regime toward classical order or spin freezing is a powerful approach to shed light on the nature of the parent ground state. Here we leverage the substitution of nonmagnetic Lu$^{3+}$ onto the Yb$^{3+}$ sites to study the effects of magnetic disorder in NaYbO$_2$ using low-temperature ac susceptibility, heat capacity, and muon spin relaxation ($μ$SR) measurements. Our $μ$SR measurements reveal resilient, correlated magnetic fluctuations that persist to at least 15\% dilution, precluding conventional spin freezing and magnetic inhomogeneity. Heat capacity and magnetic susceptibility resolve a rapid suppression of the field-induced ``up-up-down'' magnetic order upon dilution and a crossover in the power-law behavior of the low-temperature magnetic excitations associated with the zero-field quantum disordered ground state. Taken together, these results support the notion of a robust network of entangled moments in NaYbO$_2$, and provides experimental validation of several models of a Heisenberg triangular lattice antiferromagnet in the presence of disorder.

cond-mat.str-el↗

arXiv2025

Pressure tuning of competing interactions on a honeycomb lattice

Magnetic exchange interactions are mediated via orbital overlaps across chemical bonds. Thus, modifying the bond angles by physical pressure or strain can tune the relative strength of competing interactions. Here we present a remarkable case of such tuning between the Heisenberg (J) and Kitaev (K) exchange, which respectively establish magnetically ordered and spin liquid phases on a honeycomb lattice. We observe a rapid suppression of the Neel temperature (TN) with pressure in Ag3LiRh2O6, a spin-1/2 honeycomb lattice with both J and K couplings. Using a combined analysis of x-ray data and first-principles calculations, we find that pressure modifies the bond angles in a way that increases the |K/J| ratio and thereby suppresses TN. Consistent with this picture, we observe a spontaneous onset of muon spin relaxation (muSR) oscillations below TN at low pressure, whereas in the high-pressure phase, oscillations appear only when T < TN/2. Unlike other candidate Kitaev materials, Ag3LiRh2O6 is tuned toward a quantum critical point by pressure while avoiding a structural dimerization in the relevant pressure range.

cond-mat.str-el↗

arXiv2024

Uncovering the Hidden Ferroaxial Density Wave as the Origin of the Axial Higgs Mode in RTe$_3$

The recent discovery of an axial amplitude (Higgs) mode in the long-studied charge density wave (CDW) systems GdTe$_3$ and LaTe$_3$ suggests a heretofore unidentified hidden order. A theoretical study proposed that the axial Higgs results from a hidden ferroaxial component of the CDW, which could arise from non-trivial orbital texture. Here, we report extensive experimental studies on ErTe$_3$ and HoTe$_3$ that possess a high-temperature CDW similar to other RTe$_3$ (R = rare earth), along with an additional low-temperature CDW with an orthogonal ordering vector. Combining Raman spectroscopy with large-angle convergent beam electron diffraction (LACBED), rotational anisotropy second-harmonic generation (RA-SHG), and muon-spin relaxation ($μ$SR), we provide unambiguous evidence that the high-temperature CDW breaks translation, rotation, and all vertical and diagonal mirror symmetries, but not time-reversal or inversion. In contrast, the low-temperature CDW only additionally breaks translation symmetry. Simultaneously, Raman scattering shows the high-temperature CDW produces an axial Higgs mode while the low-temperature mode is scalar. The weak monoclinic structural distortion and clear axial response in Raman and SHG are consistent with a ferroaxial phase in RTe$_3$ driven by coupled orbital and charge orders. Thus, our study provides a new standard for uncovering unconventional orders and confirms the power of Higgs modes to reveal them.

cond-mat.str-el↗

arXiv2022

Novel magnetic ordering in LiYbO2 probed by muon spin relaxation

The stretched diamond lattice material LiYbO2 has recently been reported to exhibit two magnetic transitions ($T_{N1} = 1.1 K$, $T_{N2} = 0.45 K$) via specific heat, magnetization, and neutron scattering measurements [Bordelon et al., Phys. Rev. B 103, 014420 (2021)]. Here we report complementary magnetic measurements down to T = 0.28 K via the local probe technique of muon spin relaxation. While we observe a rapid increase in the zero-field muon depolarization rate at $T_{N1}$, we do not observe any spontaneous muon precession for $T < T_{N1}$, which is typically associated with long-range magnetic ordering. The depolarization rate in the ordered state shows a surprising sensitivity to magnetic fields applied along the initial spin polarization direction. Using a simple one-dimensional model, we show that these results are consistent with the unusual random-phase bipartite incommensurate magnetic structure proposed by Bordelon et al. for the intermediate temperature range $T_{N2} < T < T_{N1}$. We also find evidence for temperature-independent magnetic fluctuations persisting to our lowest temperatures, but no obvious signature of the transition or spontaneous muon precession at and below TN2, respectively. This result is suggestive of quantum dynamics within a highly degenerate ground state.

cond-mat.str-el↗

arXiv2022

First demonstration of tuning between the Kitaev and Ising limits in a honeycomb lattice

Recent observations of novel spin-orbit coupled states have generated tremendous interest in $4d/5d$ transition metal systems. A prime example is the $J_{\text{eff}}=\frac{1}{2}$ state in iridate materials and $α$-RuCl$_{3}$ that drives Kitaev interactions. Here, by tuning the competition between spin-orbit interaction ($λ_{\text{SOC}}$) and trigonal crystal field splitting ($Δ_\text{T}$), we restructure the spin-orbital wave functions into a novel $μ=\frac{1}{2}$ state that drives Ising interactions. This is done via a topochemical reaction that converts Li$_{2}$RhO$_{3}$ to Ag$_{3}$LiRh$_{2}$O$_{6}$, leading to an enhanced trigonal distortion and a diminished spin-orbit coupling in the latter compound. Using perturbation theory, we present an explicit expression for the new $μ=\frac{1}{2}$ state in the limit $Δ_\text{T}\gg λ_{\text{SOC}}$ realized in Ag$_{3}$LiRh$_{2}$O$_{6}$, different from the conventional $J_\text{eff}=\frac{1}{2}$ state in the limit $λ_{\text{SOC}}\gg Δ_\text{T}$ realized in Li$_{2}$RhO$_{3}$. The change of ground state is followed by a dramatic change of magnetism from a 6 K spin-glass in Li$_{2}$RhO$_{3}$ to a 94 K antiferromagnet in Ag$_{3}$LiRh$_{2}$O$_{6}$. These results open a pathway for tuning materials between the two limits and creating a rich magnetic phase diagram.

cond-mat.mtrl-sci↗

arXiv2022

Radio-frequency manipulation of state populations in an entangled fluorine-muon-fluorine system

Entangled spin states are created by implanting muons into single crystal LiY0.95Ho0.05F4 to form a cluster of correlated, dipole-coupled local magnetic moments. The resulting states have well-defined energy levels allowing experimental manipulation of the state populations by electromagnetic excitation. Experimental control of the evolution of the muon spin polarization is demonstrated through application of continuous, radio-frequency magnetic excitation fields. A semiclassical model of quantum, dipole-coupled spins interacting with a classical, oscillating magnetic field accounts for the muon spin evolution. On application of the excitation field, this model shows how changes in the state populations lead to the experimentally observed effects, thus enabling a spectroscopic probe of entangled spin states with muons.

quant-ph↗

arXiv2022

Complex vortex-antivortex dynamics in the magnetic superconductor EuFe$_{2}$(As$_{0.7}$P$_{0.3}$)$_{2}$

We report on the investigation of the magnetic superconductor EuFe$_{2}$(As$_{0.7}$P$_{0.3}$)$_{2}$ based on muon-spin spectroscopy and ac magnetic susceptibility ($χ$) measurements. The dependence of the internal field at the muon site on temperature is indicative of a ferromagnetic ordering of Eu$^{2+}$ magnetic moments and only the conventional magnon scattering governs the longitudinal relaxation rate at low temperatures. At the same time, we observe a rich phenomenology for the imaginary component of the susceptibility $χ^{\prime\prime}$ by means of both standard ac susceptibility and a novel technique based on a microwave coplanar waveguide resonator. In particular, we detect activated trends for several features in $χ^{\prime\prime}$ over frequencies spanning ten orders of magnitude. We interpret our results in terms of the complex dynamics of vortices and antivortices influenced by the underlying structure of magnetic domains.

cond-mat.supr-con↗

arXiv2021

Evidence of a hidden flux phase in the topological kagome metal CsV$_3$Sb$_5$

Phase transitions governed by spontaneous time reversal symmetry breaking (TRSB) have long been sought in many quantum systems, including materials with anomalous Hall effect (AHE), cuprate high temperature superconductors, Iridates and so on. However, experimentally identifying such a phase transition is extremely challenging because the transition is hidden from many experimental probes. Here, using zero-field muon spin relaxation (ZF-$μ$SR) technique, we observe strong TRSB signals below 70 K in the newly discovered kagome superconductor CsV$_3$Sb$_5$. The TRSB state emerges from the 2 x 2 charge density wave (CDW) phase present below ~ 95 K. By carrying out optical second-harmonic generation (SHG) experiments, we also find that inversion symmetry is maintained in the temperature range of interest. Combining all the experimental results and symmetry constraints, we conclude that the interlayer coupled chiral flux phase (CFP) is the most promising candidate for the TRSB state among all theoretical proposals of orbital current orders. Thus, this prototypical kagome metal CsV3Sb5 can be a platform to establish a TRSB current-ordered state and explore its relationship with CDW, giant AHE, and superconductivity.

cond-mat.supr-con↗

arXiv2021

Superconductivity in the $\mathbb{Z}_2$ kagome metal KV$_3$Sb$_5$

Here we report the observation of bulk superconductivity in single crystals of the two-dimensional kagome metal KV$_3$Sb$_5$. Magnetic susceptibility, resistivity, and heat capacity measurements reveal superconductivity below $T_c = 0.93$K, and density functional theory (DFT) calculations further characterize the normal state as a $\mathbb{Z}_2$ topological metal. Our results demonstrate that the recent observation of superconductivity within the related kagome metal CsV$_3$Sb$_5$ is likely a common feature across the AV$_3$Sb$_5$ (A: K, Rb, Cs) family of compounds and establish them as a rich arena for studying the interplay between bulk superconductivity, topological surface states, and likely electronic density wave order in an exfoliable kagome lattice.

cond-mat.supr-con↗

arXiv2020

Absence of local moments in the kagome metal KV3Sb5 as determined by muon spin spectroscopy

We have carried out muon spin relaxation and rotation measurements on the newly discovered kagome metal KV3Sb5, and find a local field dominated by weak magnetic disorder which we associate with the nuclear moments present, and a modest temperature dependence which tracks the bulk magnetic susceptibility. We find no evidence for the existence of V4+ local moments, suggesting that the physics underlying the recently reported giant unconventional anomalous Hall effect in this material warrants further studies.

cond-mat.str-el↗

arXiv2020

Effect of structural disorder on the Kitaev magnet Ag$_{3}$LiIr$_{2}$O$_{6}$

Searching for an ideal Kitaev spin liquid candidate with anyonic excitations and long-range entanglement has motivated the synthesis of a new family of intercalated Kitaev magnets such as H$_{3}$LiIr$_{2}$O$_{6}$, Cu$_{2}$IrO$_{3}$, and Ag$_{3}$LiIr$_{2}$O$_{6}$. The absence of a susceptibility peak and a two-step release of the magnetic entropy in these materials has been proposed as evidence of proximity to the Kitaev spin liquid. Here we present a comparative study of the magnetic susceptibility, heat capacity, and muon spin relaxation ($μ$SR) between two samples of Ag$_{3}$LiIr$_{2}$O$_{6}$ in the clean and disordered limits. In the disordered limit, the absence of a peak in either susceptibility or heat capacity and a weakly depolarizing $μ$SR signal may suggest a proximate spin liquid ground state. In the clean limit, however, we resolve a peak in both susceptibility and heat capacity data, and observe clear oscillations in $μ$SR that confirm long-range antiferromagnetic ordering. The $μ$SR oscillations fit to a Bessel function, characteristic of an incommensurate order, as reported in the parent compound $α$-Li$_{2}$IrO$_{3}$. Our results clarify the role of structural disorder in the intercalated Kitaev magnets.

cond-mat.mtrl-sci↗

arXiv2020

Monopole-limited nucleation of magnetism in Eu$_{2}$Ir$_{2}$O$_{7}$

We present an in-depth analysis of muon-spin spectroscopy measurements of Eu$_{2}$Ir$_{2}$O$_{7}$ under the effect of the Eu$_{1-x}$Bi$_{x}$ isovalent and diamagnetic substitution as well as of external pressure. Our results evidence an anomalously slow increase of the magnetic volume fraction upon decreasing temperature only for stoichiometric Eu$_{2}$Ir$_{2}$O$_{7}$, pointing towards highly unconventional properties of the magnetic phase developing therein. We argue that magnetism in Eu$_{2}$Ir$_{2}$O$_{7}$ develops based on the nucleation of magnetic droplets at $T_{N}$, whose successive growth is limited by the need of a continuous generation of magnetic hedgehog monopoles.

cond-mat.str-el↗

arXiv2018

Competition between static and dynamic magnetism in the Kitaev spin liquid material Cu2IrO3

Anyonic excitations emerging from a Kitaev spin liquid can form a basis for quantum computers. Searching for such excitations motivated intense research on the honeycomb iridate materials. However, access to a spin liquid ground state has been hindered by magnetic ordering. Cu2IrO3 is a new honeycomb iridate without thermodynamic signatures of a long-range order. Here, we use muon spin relaxation to uncover the magnetic ground state of Cu2IrO3. We find a two-component depolarization with slow and fast relaxation rates corresponding to distinct regions with dynamic and static magnetism, respectively. X-ray absorption spectroscopy and first principles calculations identify a mixed copper valence as the origin of this behavior. Our results suggest that a minority of Cu2+ ions nucleate regions of static magnetism whereas the majority of Cu+/Ir4+ on the honeycomb lattice give rise to a Kitaev spin liquid.

cond-mat.str-el↗

arXiv2014

Short-range correlations in the magnetic ground state of Na4Ir3O8

The magnetic ground state of the hyper-kagome lattice in Na4Ir3O8 is explored via combined bulk magnetization, muon spin relaxation, and neutron scattering measurements. A short-range, frozen, state comprised of quasi-static moments develops below a characteristic temperature of T_F=6 K, revealing an inhomogeneous distribution of spins occupying the entirety of the sample volume. Quasi-static, short-range, spin correlations persist until at least 20 mK and differ substantially from the nominally dynamic response of a quantum spin liquid. Our data demonstrate that an inhomogeneous magnetic ground state arises in Na4Ir3O8 driven either by disorder inherent to the creation of the hyper-kagome lattice itself or stabilized via quantum fluctuations.

cond-mat.str-el↗

arXiv2011

Yb4LiGe4 - A Yb Mixed Valent Zintl Phase with Strong Electronic Correlations

Single-phase samples of Yb4LiGe4 and Yb5Ge4 were synthesized using high frequency (HF) heat treatment. Yb4LiGe4 crystallizes in orthorhombic space group Pnma with the Gd5Si4 type of crystal structure and lattice parameters a = 7.0571(1) Angs, b = 14.6239(1) Angs, and c = 7.6155(1) Angs. One Yb position in Yb5Ge4 is substituted by the lithium atom and causes a distortion of the germanium tetragons in Yb4LiGe4. Investigation of the electronic state of Yb via magnetic susceptibility and X-ray absorption near-edge spectroscopy (XANES) revealed a presence of two electronic states of ytterbium, 4f13 and 4f14 (mixed valence), in Yb5Ge4 and Yb4LiGe4. Studies of the temperature dependence of the electrical resistivity, magnetization, 7Li spin-lattice relaxation rate and the specific heat indicate that strong electronic correlations are present in Yb4LiGe4, and below approximately 50 K there is a competition between ferromagnetic and antiferromagnetic correlations. Magnetic ordering in Yb4LiGe4, if present, occurs below the reported antiferromagnetic transition temperature of 1.7 K for Yb5Ge4.

cond-mat.str-el↗