arXiv subjects

Hans-Henning Klauss

Publications and source records attributed to Hans-Henning Klauss.

At least 19 recordsLinked to original sources

arXiv2026

Effective Ionic Valence and Local Magnetic Moment in Kagome Superconductors

In order to understand the unexpected similarity and the correlated behavior in kagome superconductor families AV$_3$Sb$_5$ (A = K, Rb, Cs) and ATi$_3$Bi$_5$ (A = Rb, Cs), we investigate the Hartree-scale local electronic structure of these systems. Our result indicates that V and Ti ions are both of 2+ valence such that the corresponding itinerant carrier densities are similar, and the difference in electron count is instead reflected in their quantum fluctuating ionic magnetic moments. However, due to the frustrated lattice geometry of these materials, such local moments are difficult to experimentally observe via standard probes. For verification, we systematically introduce nonmagnetic Sn impurities to locally relieve the geometric frustration and experimentally demonstrate the existence of well-defined local magnetic moments via magnetic susceptibility and muon spin rotation or relaxation ($μ$SR) measurements. All experiments discover a systematic increase of magnetic susceptibility upon increasing nonmagnetic impurity level. Our discovered ionic moments suggest a paradigm shift from the existing itinerant carrier-only picture to one incorporating strong correlation from local ionic spins. The associated interatomic and local-itinerant correlations offer a solid ground for the emergence of the observed rich correlated behavior in this new family of superconducting materials.

cond-mat.str-el↗

arXiv2026

Ultrasound Evidence for a Low-Temperature Anomaly Inside the Superconducting State of 4Hb-TaS$_2$

We report low-temperature ultrasound measurements on single crystals of the layered van der Waals superconductor 4Hb-TaS$_2$. Specific heat and ac magnetic susceptibility show a sharp bulk superconducting transition at $T_{\rm c}\approx 2.9$~K. Ultrasound measurements reveal an additional anomaly deep inside the superconducting state near $T^{*}\approx 1$~K. The most direct signature is observed in the relative ultrasonic attenuation change $Δα$: instead of being rapidly suppressed at $T_{\rm c}$, $Δα$ remains large throughout the intermediate superconducting regime and drops strongly only near $T^{*}$. This loss of acoustic dissipation is accompanied by a pronounced anomaly in the relative sound velocity change $Δv/v$, indicating strong coupling to the lattice. The low-temperature anomaly is rapidly suppressed by magnetic field and by Se substitution, suggesting a possible superconducting origin of the anomaly. We speculate that this feature may be related to induced superconductivity in the 1T layers.

cond-mat.supr-con↗

arXiv2026

Spin-liquid-like ground states in the double hydroxyperovskites CuSn(OD)6 and MnSn(OD)6 evidenced by μSR spectroscopy

Double hydroxide perovskites with magnetic transition-metal ions were recently identified as a unique class of materials that combine magnetic frustration with correlated proton disorder-a prerequisite for quantum-disordered fluctuating magnetic ground states resembling spin liquids. Here we present the results of muon spin relaxation (μSR) measurements carried out on fully deuterated samples of the double hydroxyperovskites CuSn(OH)6 (S = 1/2) and MnSn(OH)6 (S = 5/2) over the temperature range 0.053-50 K. The absence of any long-range magnetic order is confirmed down to 0.053 K. We observe no oscillations of the muon asymmetry down to the lowest temperature. The muon relaxation rates show a continuous increase with decreasing temperature, indicating persistent spin fluctuations in both compounds. Spin correlations are consistent with homogeneous spin dynamics. These observations reinforce the assertion that both compounds have a quantum-dynamic magnetic ground state that is consistent with a spin-liquid-like phase stabilized by proton disorder.

cond-mat.str-el↗

arXiv2026

Fine and Hyperfine Interactions with Multi-level Spin Relaxation of the purified Giese-Salt in Veterinary Medicine: Prussian Blue Compound Ammonium-Ferric-Hexacyano-Ferrate

Ammonium ferric hexacyanoferrate is a veterinary-medical milestone and antidote against radiocesium, well-known as Giese-salt after the Chernobyl disaster fed to domestic and wild animals, which shows even a rich interplay of properties in nanostructural chemistry and ferromagnetism. Among the broad analytical techniques, the ambivalence of macroscopic micrometer-sized agglomerates and nanoparticle sizes, a suggested enlarged Fe(II)$-$C$\equiv$N$-$Fe(III) bond length by Fe K-edge XAFS results and multi-level spin relaxation in $^{57}$Fe Mössbauer spectroscopy are highlighted. This sets this underestimated compound in a new light, e.g., for modern biomedicine and biofunctionality, extending its essential importance in addition to hypothetical future nuclear incidents

cond-mat.mtrl-sci↗

arXiv2025

Ultrasound evidence for multicomponent superconducting order parameter in Ba$_{1-x}$K$_x$Fe$_2$As$_2$ with electron quadrupling phase

Experiments have pointed to the formation of the electron quadrupling condensate in Ba$_{1-x}$K$_x$Fe$_2$As$_2$ at $x \sim 0.8$. The state spontaneously breaks time-reversal symmetry and is sandwiched between two critical points, separating it from the broken time-reversal symmetry (BTRS) superconducting state at $T_{\rm c}^{U(1)}$ and normal-metal state at $T_{\rm c}^{\rm Z2}$. We report a theory of the acoustic effects spectroscopy of systems with an electron quadrupling phase based on ultrasound-velocity measurements. We show that the experimental results are consistent with BTRS superconductivity at $x \sim 0.8$, fulfilling the necessary condition for the formation of electron quadrupling in Ba$_{1-x}$K$_x$Fe$_2$As$_2$. We provide the theoretical basis and the experimental strategy to study the order parameter symmetry of emerging quadrupling condensates in superconductors.

cond-mat.supr-con↗

arXiv2025

Evidence of pseudogap and absence of spin magnetism in the time-reversal-symmetry-breaking state of Ba$_{1-x}$K$_x$Fe$_2$As$_2$

Muon-spin-rotation ($μ$SR) experiments and the observation of a spontaneous Nernst effect indicate time-reversal symmetry breaking (BTRS) at $T_{\rm c}^{\rm Z2}$ above the superconducting transition temperature $T_{\rm c}$ in Ba$_{1-x}$K$_x$Fe$_2$As$_2$, with $x\approx0.8$. Further studies have pointed out that BTRS is caused by the formation of a new state of matter associated with the condensation of pairs of electron pairs. Despite exhibiting multiple unconventional effects that warrant further investigation, the electronic spectral properties of this electron quadrupling state remain largely unexplored. Here, we present detailed $^{75}$As nuclear magnetic resonance (NMR) measurements of Ba$_{1-x}$K$_x$Fe$_2$As$_2$, with $x = 0.77$, which has $T_{\rm c}^{\rm Z2}$ > $T_{\rm c}$ according to measurements of the spontaneous Nernst effect. The NMR data obtained in this work provide the first direct electronic spectral characteristics of the electron quadrupling state by indicating that it evolves from a pseudogap that sets in at $T^*$ well above $T_{\rm c}^{\rm Z2}$. This pseudogap behavior is consistent with $μ$SR Knight-shift, specific-heat, and transport data indicating the formation of a bound state of electrons. According to a theory of electron quadrupling condensates, such bound-state formations should precede the onset of BTRS correlations between pairs of electron pairs. The second important insight from NMR data is the absence of spin-related magnetism. The temperature dependence of the spin-lattice relaxation rate $1/T_1T$ and the evolution of the NMR linewidth prove the absence of a magnetic transition at $T_{\rm c}^{\rm Z2}$ and rule out even a proximity to some magnetic instability. This indicates that the spontaneous magnetic fields detected in this compound are not caused by spin magnetism but are associated with persistent real-space currents.

cond-mat.supr-con↗

arXiv2023

$μ$SR measurements on Sr$_2$RuO$_4$ under $\langle 110 \rangle$ uniaxial stress

Muon spin rotation/relaxation ($μ$SR) and polar Kerr effect measurements provide evidence for a time-reversal symmetry breaking (TRSB) superconducting state in Sr$_2$RuO$_4$. However, the absence of a cusp in the superconducting transition temperature ($T_{\rm c}$) vs. stress and the absence of a resolvable specific heat anomaly at TRSB transition temperature ($T_{\rm TRSB}$) under uniaxial stress challenge a hypothesis of TRSB superconductivity. Recent $μ$SR studies under pressure and with disorder indicate that the splitting between $T_{\rm c}$ and $T_{\rm TRSB}$ occurs only when the structural tetragonal symmetry is broken. To further test such behavior, we measured $T_\text{c}$ through susceptibility measurements, and $T_\text{TRSB}$ through $μ$SR, under uniaxial stress applied along a $\langle 110 \rangle$ lattice direction. We have obtained preliminary evidence for suppression of $T_\text{TRSB}$ below $T_\text{c}$, at a rate much higher than the suppression rate of $T_\text{c}$.

cond-mat.supr-con↗

arXiv2022

Calorimetric evidence for two phase transitions in Ba$_{\rm 1-x}$K$_{\rm x}$Fe$_{2}$As$_{2}$ with fermion pairing and quadrupling states

Theoretically, materials that break multiple symmetries allow, under certain conditions, the formation of four-fermion condensates above the superconducting critical temperature. Such states can be stabilized by phase fluctuations. Recently a fermionic quadrupling condensate that breaks the $Z_2$ time-reversal symmetry was reported in Ba$_{\rm 1-x}$K$_{\rm x}$Fe$_{2}$As$_{2}$ [V. Grinenko et al., Nat. Phys. 17, 1254 (2021)]. Evidence for the new state of matter comes from muon-spin rotation, transport, thermoelectric, and ultrasound experiments. Observing a specific heat anomaly is a very important signature of a transition to a new state of matter. However, a fluctuation-induced specific heat singularity is usually very challenging to resolve from a background of other contributions. Here, we report on detecting two anomalies in the specific heat of Ba$_{\rm 1-x}$K$_{\rm x}$Fe$_{2}$As$_{2}$ at zero magnetic field. The anomaly at the higher temperature is accompanied by the appearance of a spontaneous Nernst effect, indicating broken time-reversal ($Z_2$) symmetry. The second anomaly at the lower temperature coincides with the transition to a zero resistance state, indicating superconductivity breaking the $U(1)$ gauge symmetry. Our data provide calorimetric evidence for the $Z_2$ phase formation above the superconducting phase transition.

cond-mat.supr-con↗

arXiv2021

Quartic metal: Spontaneous breaking of time-reversal symmetry due to four-fermion correlations in Ba$_{1-x}$K$_x$Fe$_2$As$_2$

Discoveries of ordered quantum states of matter are of great fundamental interest, and often lead to unique applications. The most well known example -- superconductivity -- is caused by the formation and condensation of pairs of electrons. A key property of superconductors is diamagnetism: magnetic fields are screened by dissipationless currents. Fundamentally, what distinguishes superconducting states from normal states is a spontaneously broken symmetry corresponding to long-range coherence of fermion pairs. Here we report a set of experimental observations in hole doped Ba$_{1-x}$K$_x$Fe$_2$As$_2$ which are not consistent with conventional superconducting behavior. Our specific-heat measurements indicate the formation of fermionic bound states when the temperature is lowered from the normal state. However, for $x \sim 0.8$, instead of the standard for superconductors, zero resistance and diamagnetic screening, for a range of temperatures, we observe the opposite effect: the generation of self-induced magnetic fields measured by spontaneous Nernst effect and muon spin rotation experiments. The finite resistance and the lack of any detectable diamagnetic screening in this state exclude the spontaneously broken symmetry associated with superconducting two-fermion correlations. Instead, combined evidence from transport and thermodynamic measurements indicates that the formation of fermionic bound states leads to spontaneous breaking of time-reversal symmetry above the superconducting transition temperature. These results demonstrate the existence of a broken-time-reversal-symmetry bosonic metal state. In the framework of a multiband theory, such a state is characterized by quartic correlations: the long-range order exists only for {\it pairs} of fermion pairs.

cond-mat.supr-con↗

arXiv2021

Unsplit superconducting and time reversal symmetry breaking transitions in Sr$_2$RuO$_4$ under hydrostatic pressure and disorder

There is considerable evidence that the superconducting state of Sr$_2$RuO$_4$ breaks time reversal symmetry. In the experiments showing time reversal symmetry breaking its onset temperature, $T_\text{TRSB}$, is generally found to match the critical temperature, $T_\text{c}$, within resolution. In combination with evidence for even parity, this result has led to consideration of a $d_{xz} \pm id_{yz}$ order parameter. The degeneracy of the two components of this order parameter is protected by symmetry, yielding $T_\text{TRSB} = T_\text{c}$, but it has a hard-to-explain horizontal line node at $k_z=0$. Therefore, $s \pm id$ and $d \pm ig$ order parameters are also under consideration. These avoid the horizontal line node, but require tuning to obtain $T_\text{TRSB} \approx T_\text{c}$. To obtain evidence distinguishing these two possible scenarios (of symmetry-protected versus accidental degeneracy), we employ zero-field muon spin rotation/relaxation to study pure Sr$_2$RuO$_4$ under hydrostatic pressure, and Sr$_{1.98}$La$_{0.02}$RuO$_4$ at zero pressure. Both hydrostatic pressure and La substitution alter $T_\text{c}$ without lifting the tetragonal lattice symmetry, so if the degeneracy is symmetry-protected $T_\text{TRSB}$ should track changes in $T_\text{c}$, while if it is accidental, these transition temperatures should generally separate. We observe $T_\text{TRSB}$ to track $T_\text{c}$, supporting the hypothesis of $d_{xz} \pm id_{yz}$ order.

cond-mat.supr-con↗

arXiv2020

Piezoelectric-driven uniaxial pressure cell for muon spin relaxation and neutron scattering experiments

We present a piezoelectric-driven uniaxial pressure cell that is optimized for muon spin relaxation and neutron scattering experiments, and that is operable over a wide temperature range including cryogenic temperatures. To accommodate the large samples required for these measurement techniques, the cell is designed to generate forces up to 1000 N, and to minimize the background signal the space around the sample is kept as open as possible. We demonstrate here that by mounting plate-like samples with epoxy, a uniaxial stress exceeding 1 GPa can be achieved in an active volume of 5 mm3. We show that for practical operation it is important to monitor both the force and displacement applied to the sample. Also, because time is critical during facility experiments, samples are mounted in detachable holders that can be rapidly exchanged. The piezoelectric actuators are likewise contained in an exchangeable cartridge.

physics.app-ph↗

arXiv2020

Split superconducting and time-reversal symmetry-breaking transitions, and magnetic order in Sr$_2$RuO$_4$ under uniaxial stress

Among unconventional superconductors, Sr$_2$RuO$_4$ has become a benchmark for experimentation and theoretical analysis because its normal-state electronic structure is known with exceptional precision, and because of experimental evidence that its superconductivity has, very unusually, a spontaneous angular momentum, i.e. a chiral state. This hypothesis of chirality is however difficult to reconcile with recent evidence on the spin part of the order parameter. Measurements under uniaxial stress offer an ideal way to test for chirality, because under uniaxial stress the superconducting and chiral transitions are predicted to split, allowing the empirical signatures of each to be identified separately. Here, we report zerofield muon spin relaxation (ZF-$μ$SR) measurements on crystals placed under uniaxial stresses of up to 1.05 GPa. We report a clear stress-induced splitting between the onset temperatures of superconductivity and time-reversal symmetry breaking, consistent with qualitative expectations for chiral superconductivity. We also report the appearance of unexpected bulk magnetic order under a uniaxial stress of ~ 1.0 GPa in clean Sr$_2$RuO$_4$.

cond-mat.supr-con↗

arXiv2018

Suppression of the magnetic order in CeFeAsO: non-equivalence of hydrostatic and chemical pressure

We present a detailed investigation of the electronic properties of CeFeAsO under chemical (As by P substitution) and hydrostatic pressure by means of in-house and synchrotron Mössbauer spectroscopy. The Fe magnetism is suppressed due to both pressures and no magnetic order was observed above a P-substitution level of 40% or 5.2 GPa hydrostatic pressure. We compared both pressures and found that the isovalent As by P substitution change the crystallographic and electronic properties differently than hydrostatic pressure.

cond-mat.supr-con↗

arXiv2015

Microscopic coexistence of superconductivity and magnetism in Ca1-xNaxFe2As2

We present a detailed investigation of the magnetic and superconducting properties of Ca1-xNaxFe2As2 single crystals with x = 0.00, 0.35, 0.50, and 0.67 by means of the local probe techniques Moessbauer spectroscopy and muon spin relaxation experiments. With increasing Na substitution level, the magnetic order parameter as well as the magneto-structural phase transition are suppressed. For x = 0.50 we find a microscopic coexistence of magnetic and superconducting phases accompanied by a reduction of the magnetic order parameter below the superconducting transition temperature Tc. A systematic comparison with other 122 pnictides reveals a square-root correlation between the reduction of the magnetic order parameter and the ratio of the transition temperatures, Tc/TN, which can be understood in the framework of a Landau theory. In the optimally doped sample with Tc = 34 K, diluted magnetism is found and the temperature dependence of the penetration depth and superfluid density are obtained, proving the presence of two superconducting s-wave gaps

cond-mat.supr-con↗

arXiv2014

Interplay of magnetism and superconductivity in EuFe$_{2}$(As$_{1-x}$P$_{x}$)$_{2}$ single crystals probed by muon spin rotation and ${}^{57}$Fe Mössbauer spectroscopy

We present our results of a local probe study on EuFe$_{2}$(As$_{1-x}$P$_{x}$)$_{2}$ single crystals with $x$=0.13, 0.19 and 0.28 by means of muon spin rotation and ${}^{57}$Fe Mössbauer spectroscopy. We focus our discussion on the sample with $x$=0.19 viz. at the optimal substitution level, where bulk superconductivity ($T_{\text{SC}}=28$ K) sets in above static europium order ($T^{\text{Eu}}=20$K) but well below the onset of the iron antiferromagnetic (AFM) transition ($\sim$100 K). We find enhanced spin dynamics in the Fe sublattice closely above $T_{\text{SC}}$ and propose that these are related to enhanced Eu fluctuations due to the evident coupling of both sublattices observed in our experiments.

cond-mat.supr-con↗

arXiv2014

Microscopic Coexistence of Magnetism and Superconductivity in charge compensated Ba1-xKx(Fe1-yCoy)2As2

We present a detailed investigation of the electronic phase diagram of effectively charge compensated Ba1-xKx(Fe1-yCoy)2As2 with x/2 = y. Our experimental study by means of x-ray diffraction, Mössbauer spectroscopy, muon spin relaxation and ac susceptibility measurements on polycrystalline samples is complemented by density functional electronic structure calculations. For low substitution levels of x/2 = y \< 0.13, the system displays an orthorhombically distorted and antiferromagnetically ordered ground state. The low temperature structural and magnetic order parameters are successively reduced with increasing substitution level. We observe a linear relationship between the structural and the magnetic order parameter as a function of temperature and substitution level for x/2 = y \< 0.13. At intermediate substitution levels in the range between 0.13 and 0.19, we find superconductivity with a maximum Tc of 15 K coexisting with static magnetic order on a microscopic length scale. For higher substitution levels x/2 = y \> 0.25 a tetragonal non-magnetic ground state is observed. Our DFT calculations yield a signifcant reduction of the Fe 3d density of states at the Fermi energy and a strong suppression of the ordered magnetic moment in excellent agreement with experimental results. The appearance of superconductivity within the antiferromagnetic state can by explained by the introduction of disorder due to non-magnetic impurities to a system with a constant charge carrier density. Our experimental study by means of x-ray diffraction, Mössbauer spectroscopy, muon spin relaxation and ac susceptibility measurements on polycrystalline samples is complemented by density functional electronic structure calculations.

cond-mat.supr-con↗

arXiv2013

Short range magnetic order and effective suppression of superconductivity by manganese-doping in LaFe1-xMnxAsO1-yFy

We present a study of the structural and physical properties of directly hole doped LaFe1-xMnxAsO (x = 0.0-0.2) and the influence of charge compensation / electron-doping by additional F doping in LaFe0.9Mn0.1AsO1-yFy (y = 0.1-0.5). High quality polycrystalline samples were prepared using a solid state metathesis reaction. The unit cell increases upon Mn doping, but decreases again when additional F is inserted. The semiconducting character of LaFe1-xMnxAsO decreases with additional F doping. Muon spin relaxation (muSR) measurements reveal short range magnetic order in LaFe1-xMnxAsO and a suppression of magnetism by additional electron-doping with fluoride in LaFe0.9Mn0.1AsO1-yFy. Superconductivity remains absent even though the electronic preconditions are fulfilled in electron-doped LaFe0.9Mn0.1AsO1-yFy at x > 0.1, which is suggestive of effective pair breaking by Mn in this system.

cond-mat.supr-con↗

arXiv2012

Strong Competition of Superconducting and Magnetic Order Parameters in Ba1-xNaxFe2As2

We study the interplay of magnetic and superconducting order in single crystalline hole doped Ba1-xNaxFe2As2 using muon spin relaxation. We find microscopic coexistence of magnetic order and superconductivity. In a strongly underdoped specimen the two forms of order coexist without any measurable reduction of the ordered magnetic moment by superconductivity, while in a nearly optimally doped sample the ordered magnetic moment is strongly suppressed below the superconducting transition temperature. This coupling can be well described within the framework of an effective two-band model incorporating inter- and intra-band interactions. In optimally doped Ba1-xNaxFe2As2 we observe no traces of static or dynamic magnetism and the temperature dependence of the superfluid density is consistent with two s-wave gaps without nodes.

cond-mat.supr-con↗