arXiv subjects

Hubertus Luetkens

Publications and source records attributed to Hubertus Luetkens.

At least 37 records · Page 2Linked to original sources

arXiv2025

Complex spin-density-wave ordering in La$_4$Ni$_{3}$O$_{10}$

The discovery of high-temperature superconductivity in layered nickelates under pressure has recently triggered enormous interest. Studies of these compounds have revealed a density-wave-like transition at ambient pressure, though its connection with superconductivity is still not well understood. Here, we report a detailed \msr\ study on single crystals of trilayer nickelate \LNO\ at ambient pressure. We have identified a spin-density-wave (SDW) transition at the temperature of $T_\mathrm{N} \sim$130 K, as well as a broad crossover around 70 - 100 K. Based on the temperature dependence of the muon precession amplitudes and magnetic susceptibility, we attribute this additional crossover either to a spin reorientation, or to an inhomogeneous SDW ordering.

cond-mat.supr-con↗

arXiv2025

Coexistence of anomalous spin dynamics and weak magnetic order in a chiral trillium lattice K2FeSn(PO4)3

Trillium lattices, where magnetic ions form a three-dimensional chiral network of corner-sharing equilateral triangular motifs, offer a prominent platform to explore exotic quantum states. In this work, we report ground-state properties of the $S$ = 5/2 trillium lattice compound K$_{2}$FeSn(PO$_{4}$)$_{3}$ through thermodynamic, electron spin resonance (ESR), and muon spin relaxation ($μ$SR) experiments. Thermodynamic and ESR measurements reveal the two-step evolution of magnetic correlations across $T^{*}$ = 11 K, which results from an interplay between dominant antiferromagnetic Heisenberg interactions and subleading interactions. Below $T^{*}$, \textit{dc} and \textit{ac} magnetic susceptibilities indicate weak \textcolor{black}{magnetic ordering} at $T_{\rm N} \approx 2$ K under low fields, which is suppressed for $μ_{0}H \geq 2$ T, consistent with a power-law dependence of magnetic specific heat at low temperatures. $μ$SR experiments confirm the dominance of persistent spin dynamics and the absence of conventional spin freezing, supporting the subtle nature of weak magnetic ordering coexisting with spin-liquid-like fluctuations. These findings underscore the potential for realizing a classical spin-liquid ground state with exotic excitations in high-spin trillium lattice systems.

cond-mat.str-el↗

arXiv2025

Anharmonic quantum muon effects of light particles in a spin liquid material

The quantum behavior of light nuclei and other particles in materials challenges classical intuition and introduces novel phenomena. Here we demonstrate that muon spin spectroscopy ( $μ$SR) is a powerful tool for exploring the quantum effects of light particles, such as the muon, in condensed matter. The muon's quantum nature is profoundly influenced by the surrounding, offering a unique probe for understanding the role of light atoms and their role in shaping local electronic environments. In Zn-barlowite, a candidate quantum spin liquid, we show that standard density functional theory (DFT) methods, which treat the muon as a classical point-like particle, fail to capture its strong quantum anharmonic effects. Only by modeling the muon as a spatially extended quantum particle, thus accounting for the anharmonicity, can the experimental $μ$SR data be understood. This approach not only improves the interpretation of $μ$SR results but also opens the door to studying the quantum effects of other light particles, like hydrogen and lithium nuclei, which can greatly influence material properties.

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↗

arXiv2025

New Frontiers in Muon-Spin Spectroscopy Using Si-Pixel Detectors

The study of novel quantum materials relies on muon-spin rotation, relaxation, or resonance (\mSR) measurements. Yet, a fundamental limitation persists: many of these materials can only be synthesized in extremely small quantities, often at sub-millimeter scales. While \mSR ~offers unique insights into electronic and magnetic properties, existing spectrometers lack a sub-millimeter spatial resolution and the possibility of triggerless pump-probe data acquisition, which would enable more advanced measurements. The General Purpose Surface-muon instrument (GPS) at the Paul Scherrer Institute (PSI) is currently limited to a muon stopping rate of \SI{40}{\kilo\hertz} to \SI{120}{\kilo\hertz}, a constraint that will become more pressing with the upcoming High-Intensity Muon Beam (HIMB) project. To overcome these challenges, we demonstrate the feasibility of employing ultra-thin monolithic Si-pixel detectors to reconstruct the stopping position of muons within the sample, thereby significantly enhancing the capability of measuring at higher muon rate. Additionally, we explore the first steps toward a triggerless pump-probe \mSR ~measurement scheme. Unlike conventional pump-probe techniques that require external triggers, a triggerless readout system can continuously integrate stimuli pulses into the data stream, allowing real-time tracking of ultra-fast dynamics in quantum materials. This approach will enable the study of transient states, spin dynamics, and quantum coherence under external stimuli.

physics.ins-det↗

arXiv2025

Robust Magnetic Polaron Percolation in the Antiferromagnetic CMR System EuCd$_2$P$_2$

Antiferromagnetic EuCd$_2$P$_2$ has attracted considerable attention due to its unconventional (magneto)transport properties. At a temperature $T_{\rm peak}$ significantly above the magnetic ordering temperature $T_\textrm{N} = 11\,$K a large peak in resistivity is observed which gets strongly suppressed in magnetic field, resulting in a colossal magnetoresistance (CMR), for which magnetic fluctuations and the formation of ferromagnetic clusters have been proposed as underlying mechanisms. Employing a selection of sensitive probes including fluctuation spectroscopy and third-harmonic resistance, Hall effect, AC susceptibility and $μ$SR measurements, allows for a direct comparison of electronic and magnetic properties on multiple time scales. We find compelling evidence for the formation and percolation of magnetic polarons, which explains the CMR of the system. Large peaks in the weakly-nonlinear transport and the resistance noise power spectral density at zero magnetic field signify an inhomogeneous, percolating electronic system below $T^\ast \approx 2\,T_\textrm{N}$ with a percolation threshold at $T_{\rm peak}$. In magnetic fields, the onset of large negative MR in the paramagnetic regime occurs at a universal critical magnetization similar to ferromagnetic CMR materials. The size of the magnetic polarons at the percolation threshold is estimated to $\sim 1 - 2\,$nm. The mechanism of magntic cluster formation and percolation in EuCd$_2$P$_2$ appears to be rather robust despite large variations in carrier concentration and likely is relevant for other Eu-based antiferromagnetic CMR systems.

cond-mat.str-el↗

arXiv2025

Pressure-enhanced splitting of density wave transitions in La$_3$Ni$_2$O$_{7-δ}$

The observation of superconductivity in La$_3$Ni$_2$O$_{7-δ}$ under pressure, following the suppression of a high-temperature density wave state, has attracted considerable attention. The nature of this density wave order was not clearly identified. Here, we probe the magnetic response of the zero-pressure phase of La$_3$Ni$_2$O$_{7-δ}$ as hydrostatic pressure is applied and find that the apparent single density wave transition at zero applied pressure splits into two. The comparison of our muon-spin rotation and relaxation experiments with dipole-field numerical analysis reveals the magnetic structure's compatibility with a stripe-type arrangement of Ni moments, characterized by alternating lines of magnetic moments and nonmagnetic stripes at ambient pressure. When pressure is applied, the magnetic ordering temperature increases, while the unidentified density wave transition temperature falls. Our findings reveal that the ground state of the La$_3$Ni$_2$O$_{7-δ}$ system is characterized by the coexistence of two distinct orders -- a magnetically ordered spin density wave and a lower-temperature ordering that is most likely a charge density wave -- with a notable pressure-enhanced separation between them.

cond-mat.supr-con↗

arXiv2025

Advanced muon-spin spectroscopy with high lateral resolution using Si-pixel detectors

Muon-spin spectroscopy at continuous sources has stagnated at a stopped muons rate of ~40 kHz for the last few decades. The major limiting factor is the requirement of a single muon in the sample during the typical 10 μs data gate window. To overcome this limit and to be able to perform muon-spin relaxation (μSR) measurements on millimeter-sized samples, one can use vertex reconstruction methods to construct μSR spectra. This is now possible thanks to the availability of very thin monolithic Si-pixel chips, which offer minimal particle scattering and high count rate. Here we present results from a Si-pixel based spectrometer that utilizes vertex reconstruction schemes for the incoming muons and emitted positrons. With this spectrometer we were able to obtain a first vertex reconstructed μSR (VR-μSR) spectrum. The unique capabilities and benefits of such a spectrometer are discussed.

physics.ins-det↗

arXiv2025

Pressure Effect on the Spin Density Wave Transition in La$_2$PrNi$_2$O$_{6.96}$

High-pressure studies reveal a stark contrast between the superconducting properties of double-layer Ruddlesden-Popper (RP) nickelates La$_2$PrNi$_2$O$_7$ and La$_3$Ni$_2$O$_7$. While La$_2$PrNi$_2$O$_7$ exhibits bulk superconductivity, La$_3$Ni$_2$O$_7$ displays filamentary behavior, suggesting that superconductivity is confined to phase interfaces rather than the bulk. Since magnetism emerges near the superconducting phase, understanding its differences in La$_3$Ni$_2$O$_7$ and La$_2$PrNi$_2$O$_7$ is essential for clarifying their underlying electronic and magnetic properties. In this work we study the magnetic responce of La$_2$PrNi$_2$O$_{6.96}$ under pressures up to 2.3 GPa using the muon-spin rotation/relaxation ($μ$SR) technique. The application of external pressure increases the Néel temperature $T_{\rm N}$ from approximately 161 K at ambient pressure ($p=0$) to about 170 K at $p=2.3$ GPa. The temperature dependence of the internal magnetic field $B_{\rm int}(T)$ (i.e., the magnetic order parameter) follows the power-law relation $B_{\rm int} = B_{\rm int}(0) \left(1 - \left[T/T_{\rm N}\right]^α\right)^β$, with consistent exponent values of $α\simeq 1.95$ and $β\simeq 0.35$ across different pressures. The value of the ordered moments at the Ni sites, which is proportional to $B_{\rm int}$, remain unaffected by pressure. Our findings suggest that the magnetic properties of double-layer RP nickelate La$_3$Ni$_2$O$_7$ are broadly unaffected by Pr to La substitution.

cond-mat.supr-con↗

arXiv2025

Unraveling Spin Density Wave Order in Layered Nickelates $\mathrm{La_3Ni_2O_7}$ and $\mathrm{La_2PrNi_2O_7}$ via Neutron Diffraction

The discovery of pressure-induced superconductivity in two- and three-layer Ruddlesden-Popper nickelates has generated significant interest in these materials as a platform for unconventional superconductivity. While their ground state exhibits magnetism, a direct determination of their magnetic structure remains elusive. Understanding this aspect is crucial, as magnetism may play a role in the pairing mechanism of superconductivity in these compounds. We resolve the magnetic structures of the bilayer (2222) polymorphs of La3Ni2O7 and La2PrNi2O7 using neutron powder diffraction (NPD) and muon-spin rotation/relaxation (muSR). Magnetic neutron scattering appears below approximately 150 K in both compounds and is observed at the (qx, 1/2, 0) position, with qx = 0 and 1/2 for La3Ni2O7 and qx = 0 for La2PrNi2O7. Within a single layer, alternating low (0.05 - 0.075 muB) and high (0.66 muB) magnetic moment stripes form. These layers stack antiferromagnetically along the c-direction to form bilayers. The presence of two propagation vectors (qx = 0 and 1/2) in undoped La3Ni2O7 suggests the coexistence of two magnetic stacking polymorphs within a single crystallographic phase. The muSR spectra further confirm these magnetic structures. Our findings provide a detailed understanding of the magnetic ground state in bilayer nickelates, offering insights into possible precursor states that may influence the emergence of superconductivity in these materials.

cond-mat.supr-con↗

arXiv2025

Quantum spin liquid ground state in a rare-earth triangular antiferromagnet SmTa$_7$O$_{19}$

The rare-earth-based geometrically frustrated triangular magnets have attracted considerable attention due to the intricate interplay between strong spin-orbit coupling and the crystal electric field (CEF), which often leads to effective spin-1/2 degrees of freedom and therefore promotes strong quantum fluctuations at low temperatures, thus offering an excellent route to stabilize a quantum spin liquid (QSL) ground state. We have investigated the ground state magnetic properties of a polycrystalline sample of $\text{SmTa}_7\text{O}_{19}$ which we propose to have a gapless QSL ground state by employing powder X-ray diffraction (XRD), X-ray absorption spectroscopy (XAS), DC and AC-magnetic susceptibility, $M$ vs. $H$ isotherm, specific heat, and muon spin rotation/relaxation measurements ($μ$SR) down to 30 mK. The combined structural and electronic studies reveal the formation of an edge-sharing equilateral triangular lattice of Sm$^{3+}$ ions in $ab$ plane. The DC, AC magnetic susceptibility, and heat capacity measurements reveal that $\text{SmTa}_7\text{O}_{19}$ does not exhibit any long-range magnetic ordering transition down to 50 mK. The zero-field (ZF)-$μ$SR study strongly refutes the long-range magnetically ordered ground state and/or any partial spin-freezing down to at least 30 mK. The ZF-muon-spin relaxation rate is weakly temperature dependent between 50 and 20 K, rapidly increases below $\sim$20 K and saturates at low temperatures between 2 K and 30 mK, which has been attributed to a characteristic signature of QSL systems. Further, our longitudinal-field (LF)-$μ$SR measurements at 0.1 K reveal a dynamic nature of the magnetic ground state. In addition, our high-field specific heat data suggest a gapless nature of spin excitations in this compound.

cond-mat.str-el↗

arXiv2025

Exerting chemical pressure on the kagome lattice as frustration control in the kapellasite family $A$Cu$_3$(OH)$_{6+x}$(Cl,Br)$_{3-x}$

The kapellasite family $A$Cu$_3$(OH)$_{6+x}$(Cl,Br)$_{3-x}$ forms a series of compounds, wherein the chemical pressure realized by the $A-$site cation tunes the spin exchange in the frustrated distorted kagome lattice. Via hydrothermal synthesis we have grown single crystals of the whole series for $A=$ rare-earths and found a clear structural transition to a superstructure variant at a specific chemical pressure level exerted by $A$~=~Dy. Phases with crystal structures in the vicinity of this superstructure transition realize a distorted kagome lattice of the Cu$^{2+}$ cations with characteristic features of a spin liquid. Here, subtle structural disorder as well as controlled chemical pressure can stabilize the spin liquid phase. We study the crystal structure and the magnetic ground state of these phases via single crystal x-ray diffraction, magnetic susceptibility, specific heat and muon spin spectroscopy measurements.

cond-mat.str-el↗

arXiv2025

(H,Li)$_{6}$Ru$_{2}$O$_{6}$ : a possible zero-field Ru$^{3+}$-based Kitaev Quantum Spin Liquid

We report the synthesis and properties of (H,Li)$_{6}$Ru$_{2}$O$_{6}$, which is shown to be a $J_{\text{eff}}=\frac{1}{2}$ system made out of Ru$^{3+}$ moments in a honeycomb geometry. Bulk magnetization, heat capacity, nuclear magnetic resonance (NMR), and muon spin relaxation ($μ$SR) rule out the presence of static moments or any spin glass phase down to 84 mK. All techniques suggest a crossover to a liquid-like state below about 40 K. The $^{7}$Li nuclear magnetic resonance (NMR) shift data suggest a non-zero $T$-independent spin susceptibility at low $T$. In zero field, $C_m/T$ shows $T^{-0.9}$ divergence which is consistent with vacancy-induced effects on low-energy excitations of the pristine Kitaev spin liquid. With field, power-law variations in the $^{7}$Li NMR spin-lattice relaxation rate 1/T$_{1}$ and magnetic heat capacity $C_{m}$ show quantitatively new scaling behaviors. A two-step entropy release in heat capacity is also observed putatively from $Z_{2}$ flux (low-$T$ step) and itinerant Majorana fermions (high-$T$ step). Based on these findings, we propose that (H,Li)$_{6}$Ru$_{2}$O$_{6}$ realizes a Kitaev spin liquid with no evidence of inherent magnetic ordering in zero field unlike $α$-RuCl$_{3}$ where approximately $8$ Tesla field is required to suppress magnetic order.

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↗

arXiv2024

Vacancy-induced suppression of CDW order and its impact on magnetic order in kagome antiferromagnet FeGe

Two-dimensional (2D) kagome lattice metals are interesting because they display flat electronic bands, Dirac points, Van Hove singularities, and can have interplay between charge density wave (CDW), magnetic order, and superconductivity. In kagome lattice antiferromagnet FeGe, a short-range CDW order was found deep within an antiferromagnetically ordered state, interacting with the magnetic order. Surprisingly, post-growth annealing of FeGe at 560$^{\circ}$C can suppress the CDW order while annealing at 320$^{\circ}$C induces a long-range CDW order, with the ability to cycle between the states repeatedly by annealing. Here we perform transport, neutron scattering, scanning transmission electron microscopy (STEM), and muon spin rotation ($μ$SR) experiments to unveil the microscopic mechanism of the annealing process and its impact on magneto-transport, CDW, and magnetic properties of FeGe. We find that 560$^{\circ}$C annealing creates germanium vacancies uniformly distributed throughout the FeGe kagome lattice, which prevent the formation of Ge-Ge dimers necessary for the CDW order. Upon annealing at 320$^{\circ}$C, the system segregates into stoichiometric FeGe regions with long-range CDW order and regions with stacking faults that act as nucleation sites for the CDW. The presence or absence of CDW order greatly affects the anomalous Hall effect, incommensurate magnetic order, and spin-lattice coupling in FeGe, thus placing FeGe as the only known kagome lattice material with a tunable CDW and magnetic order, potentially useful for sensing and information transmission.

cond-mat.str-el↗

arXiv2024

Coexistence of local magnetism and superconductivity in the heavy-fermion CeRh$_2$As$_2$ revealed by $μ$SR studies

The superconducting (SC) state ($T_\mathrm{c}$ = 0.3 K) of the heavy-fermion compound CeRh$_2$As$_2$, which undergoes an unusual field-induced transition to another high-field SC state, emerges from an unknown ordered state below $T_\mathrm{o}$ = 0.55 K. While an electronic multipolar order of itinerant Ce-4$f$ states was proposed to account for the $T_\mathrm{o}$ phase, the exact order parameter has not been known to date. Here, we report on muon spin relaxation ($μ$SR) studies of the magnetic and SC properties in CeRh$_2$As$_2$ single crystals at low temperatures. We reveal a magnetic origin of the $T_\mathrm{o}$ order by identifying a spontaneous internal field below $T_\mathrm{o}$ = 0.55 K. Furthermore, we find evidence of a microscopic coexistence of local magnetism with bulk superconductivity. Our findings open the possibility that the $T_\mathrm{o}$ phase involves both dipole and higher order Ce-4$f$ moment degrees of freedom and accounts for the unusual non-Fermi liquid behavior.

cond-mat.str-el↗

arXiv2024

Tuning of Charge Order by Uniaxial Stress in a Cuprate Superconductor

Strongly correlated electron materials are often characterized by competition and interplay of multiple quantum states. For example, in high-temperature cuprate superconductors unconventional superconductivity, spin- and charge-density wave orders coexist. A key question is whether competing states coexist on the atomic scale or if they segregate into distinct 'islands'. Using X-ray diffraction, we investigate the competition between charge order and superconductivity in the archetypal cuprate La(2-x)BaxCuO4, around the x = 1/8-doping, where uniaxial stress restores optimal 3D superconductivity at approximately 0.06 GPa. We find that the charge order peaks and the correlation length along the stripe are strongly reduced up to the critical stress, above which they stay constant. Simultaneously, the charge order onset temperature only shows a modest decrease. Our findings suggest that optimal 3D superconductivity is not linked to the absence of charge stripes but instead requires their arrangement into smaller 'islands'. Our results provide insight into the length scales over which the interplay between superconductivity and charge order takes place.

cond-mat.supr-con↗

arXiv2023

Emergence of flat bands and their impact on superconductivity of Mo$_5$Si$_{3-x}$P$_x$

The first-principles calculations and measurements of the magnetic penetration depths, the upper critical field, and the specific heat were performed for a family of Mo$_5$Si$_{3-x}$P$_x$ superconducotrs. First-principles calculations suggest the presence of a flat band dispersion, which gradually shifts to the Fermi level as a function of phosphorus doping $x$. The flat band approaches the Fermi level at $x\simeq 1.3$, thus separating Mo$_5$Si$_{3-x}$P$_x$ between the purely steep band and the steep band/flat band superconducting regimes. The emergence of flat bands lead to an abrupt change of nearly all the superconducting quantities. In particular, a strong reduction of the coherence length $ξ$ and enhancement of the penetration depth $λ$ result in nearly factor of three increase of the Ginzburg-Landau parameter $κ=λ/ξ$ (from $κ\simeq 25$ for $x\lesssim 1.2$ to $κ\simeq 70$ for $x\gtrsim 1.4$) thus initiating the transition of Mo$_5$Si$_{3-x}$P$_x$ from a moderate to an extreme type-II superconductivity.

cond-mat.supr-con↗