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Vadim Grinenko

Publications and source records attributed to Vadim Grinenko.

At least 19 recordsLinked to original sources

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 ($\mu$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

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 $\Delta\alpha$: instead of being rapidly suppressed at $T_{\rm c}$, $\Delta\alpha$ 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 $\Delta v/v$, 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

Origins of spontaneous magnetic fields in Sr$_2$RuO$_4$

The nature of the broken time reversal symmetry (BTRS) state in Sr$_2$RuO$_4$ remains elusive, and its relation to superconductivity remains controversial. There are various universal predictions for the BTRS state when it is associated with a multicomponent superconducting order parameter. In particular, in the BTRS superconducting state, spontaneous fields appear around crystalline defects, impurities, superconducting domain walls and sample surfaces. However, this phenomenon has not yet been experimentally demonstrated for any BTRS superconductor. Here, we aimed to verify these predictions for Sr$_2$RuO$_4$ by performing muon spin relaxation ($\mu$SR) measurements on Sr$_{2-y}$La$_{y}$RuO$_4$ single crystals at ambient pressure and stoichiometric Sr$_2$RuO$_4$ under hydrostatic pressure. The study allowed us to conclude that spontaneous fields in the BTRS superconducting state of Sr$_2$RuO$_4$ appear around non-magnetic inhomogeneities and, at the same time, decrease with the suppression of $T_{\rm c}$. The observed behaviour is consistent with the prediction for multicomponent BTRS superconductivity in Sr$_2$RuO$_4$. The results of the work are relevant to understanding BTRS superconductivity in general, as they demonstrate, for the first time, the relationship among the superconducting order parameter, the BTRS transition, and crystal-structure inhomogeneities.

cond-mat.supr-con

Novel coupling between charge order and time-reversal-symmetry-breaking superconductivity

The interplay between charge-density waves (CDWs), which break translational symmetry, and spatially homogeneous superconductivity, which breaks global U(1) gauge symmetry, can give rise to an intriguing phenomenon: the pair-density wave, characterized by a spatial modulation of the superconducting order parameter. Yet how CDWs couple to unconventional superconducting states-particularly those with time-reversal symmetry breaking (TRSB)-remains largely unexplored. Here, using scanning tunneling microscopy on heavily hole-doped Ba$_{1-x}$K$_x$Fe$_2$As$_2$, which hosts an s $\pm$ is superconducting state, we reveal a previously unobserved coupling between a surface CDW and TRSB superconductivity. Experimentally, the TRSB superconductivity imparts "chirality" to the CDW, which manifests as commensurate domains separated by domain walls with $\pi$-phase slips-forming what we term a bipolar CDW. The domain walls delineate TRSB domains of opposite chirality, consistent with spontaneous breaking of U(1) $\times$ Z2. Supported by theoretical modelling, we construct a framework in which a hidden interfacial pair-density modulation (PDM) mediates a linear coupling between the surface CDW and interband Josephson currents of TRSB superconductivity. Crucially, the theory shows that realizing this linear coupling requires a controlled global phase difference $\delta$ $\phi$ = $\pi$/2 between the PDM and CDW states. Our results uncover a previously overlooked connection between charge ordering and TRSB superconductivity, opening a pathway to explore intertwined quantum orders in iron-based superconductors and other strongly correlated systems.

cond-mat.supr-con

Nematic Fluctuations and Electronic Correlations in Heavily Hole-Doped Ba$_{1-x}$K$_x$Fe$_2$As$_2$ Probed by Elastoresistance

This work investigates nematic fluctuations and electronic correlations in the hole-doped iron pnictide superconductor Ba$_{1-x}$K$_x$Fe$_2$As$_2$ by means of longitudinal and transverse elastoresistance measurements over a wide doping range ($0.63 < x < 0.98$). For this purpose, the orbital character of the electronic response was revealed by decomposition of the elastoresistance into the $A_{1g}$ and $B_{2g}$ symmetry channels. It was shown that at lower doping levels nematic fluctuations in the $B_{2g}$ channel dominate, while for $x > 0.68$ the $A_{1g}$ channel becomes dominant and reaches a pronounced maximum at $x \approx 0.8$ which indicates strong orbital-selective electronic correlations. Despite the dominance of the $A_{1g}$ signal at high doping, a weak contribution in the $B_{2g}$ channel persists, which can be interpreted as a remnant of nematic fluctuations. Model calculations based on a five-orbital tight-binding Hamiltonian with interactions attribute the observed enhancement in the $A_{1g}$ channel to an orbital-selective Kondo-like resonance, predominantly involving the $d_{xy}$ orbital. We discuss our results in relation to the evolution of the Sommerfeld coefficient reported in the literature and a reported change of the superconducting order parameter. All this indicates that for $x > 0.68$ qualitatively new physics emerges. Our findings suggest that electronic correlations in the strongly hole-doped regime play an important role in superconductivity, while the detectable weak nematic fluctuations may also be of relevance.

cond-mat.str-el

Hund's coupling assisted orbital-selective superconductivity in Ba1-xKxFe2As2

While the superconducting transition temperature of hole-doped Ba_{1-x}K_{x}Fe_{2}As_{2} decreases past optimal doping, superconductivity does not completely disappear even for the fully doped KFe_{2}As_{2} compound. In fact, superconductivity is robust through a Lifshitz transition where electron bands become hole-like around the zone corner at around x=0.7, thus challenging the conventional understanding of superconductivity in iron-based systems. High-resolution angle-resolved photoemission spectroscopy is used to investigate the superconducting gap structure, as well as the normal state electronic structure, around optimal doping and across the Lifshitz transition. Our findings reveal a largely orbital-dependent superconducting gap structure, where the more strongly correlated d_{xy} band has a vanishing superconducting gap at higher doping, aligning with the Hund's metal behavior observed in the normal state. Notably, the superconducting gap on the d_{xy} band disappears before the Lifshitz transition, suggesting that the Fermi surface topology may play a secondary role. We discuss how these results point to orbital-selective superconducting pairing and how strong correlations via Hund's coupling may shape superconducting gap structures in iron-based and other multiorbital superconductors.

cond-mat.supr-con

Inhomogeneity-driven multiform Spontaneous Hall Effect in conventional and unconventional superconductors

The spontaneous Hall effect (SHE), a finite voltage occurring transversal to the electrical current in zero-magnetic field, has been observed in both conventional and unconventional superconductors, appearing as a peak near the superconducting transition temperature. The origin of SHE is strongly debated, with proposed explanations ranging from intrinsic and extrinsic mechanisms such as spontaneous symmetry breaking and time-reversal symmetry breaking (BTRS), Abrikosov vortex motion, or extrinsic factors like material inhomogeneities, such as non-uniform critical temperature (Tc) distributions or structural asymmetries. This work is an experimental study of the SHE in various superconducting materials. We focused on conventional, low-Tc, sharp transition Nb and unconventional, intermediate-Tc, smeared transition Fe(Se,Te). Our findings show distinct SHE peaks around the superconducting transition, with variations in height, sign and shape, indicating a possible common mechanism independent of the specific material. We propose that spatial inhomogeneities in the critical temperature, caused by local chemical composition variations, disorder, or other forms of electronic spatial inhomogeneities could explain the appearing of the SHE. This hypothesis is supported by comprehensive finite elements simulations of randomly distributed Tc by varying Tc-distribution, spatial scale of disorder and amplitude of the superconducting transition. The comparison between experimental results and simulations suggest a unified origin for the SHE in different superconductors, whereas different phenomenology can be explained in terms of amplitude of the transition temperature in respect to Tc-distribution.

cond-mat.supr-con

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 ($\mu$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 $\mu$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

Direct observation of quantum vortex fractionalization in multiband superconductors

Magnetic field is expelled from a superconductor, unless it forms quantum vortices, consisting of a core singularity with current circulating around it. The London quantization condition implies that there is one core singularity per quantum of magnetic flux in single-component superconductors, while in multiband materials fractional vortices are possible. Here, we report the first observation of quantum vortex core fractionalization on the potassium terminated surface of multiband superconductor KFe2As2 by scanning tunneling microscopy. We observe splitting of an integer-flux vortex into several fractional vortices, leading to disparity between numbers of flux quanta and vortex cores. Our findings demonstrate that fractionalized core singularities are possible in a multiband superconductor, opening avenue for new experimental platforms with quasiparticles with fractional statistics.

cond-mat.supr-con

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

In-plane magnetic penetration depth in Sr$_2$RuO$_4$: muon-spin rotation/relaxation study

We report on measurements of the in-plane magnetic penetration depth ($λ_{\rm ab}$) in single crystals of Sr$_2$RuO$_4$ down to $\simeq 0.015$ K by means of muon-spin rotation/relaxation. The linear temperature dependence of $λ^{-2}_{\rm ab}$ for $T\lesssim 0.7$ K suggests the presence of nodes in the superconducting gap. This statement is further substantiated by observation of the Volovik effect, $i.e.$ the reduction of $λ_{ab}^{-2}$ as a function of the applied magnetic field. The experimental zero-field and zero-temperature value of $λ_{\rm ab}=124(3)$ nm agrees with $λ_{\rm ab}\simeq 130$ nm, calculated based on results of electronic structure measurements reported in [Phys. Rev X 9, 021048 (2019)]. Our analysis reveals that a simple nodal superconducting energy gap, described by the lowest possible harmonic of a gap function, does not capture the dependence of $λ_{\rm ab}^{-2}$ on $T$, so the higher angular harmonics of the energy gap function need to be introduced.

cond-mat.supr-con

Observation of superconducting vortices carrying a temperature-dependent fraction of the flux quantum

The magnetic response is a state-defining property of superconductors. The magnetic flux penetrates type-II bulk superconductors by forming quantum vortices when the enclosed magnetic flux is equal to the magnetic flux quantum. The flux quantum is the universal quantity that depends only on the ratio of fundamental constants: the electron charge and the Planck constant. This work investigates the vortex state in the hole-overdoped Ba$_{1-x}$K$_x$Fe$_2$As$_2$ by using scanning superconducting quantum interference device (SQUID) magnetometry. We observed quantum vortices that carry only a fraction of the flux quantum, which vary continuously with temperature. This finding establishes the phenomenon that superconductors support quantum vortices with non-universally quantized magnetic flux. Furthermore, the demonstrations of the mobility of the fractional vortices and the manipulability of their positions open up a route for future fluxonics applications.

cond-mat.supr-con

$μ$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

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

Elastoresistivity of heavily hole doped 122 iron pnictides superconductors

Nematicity in the heavily hole-doped iron pnictide superconductors remains controversial. Sizeable nematic fluctuations and even nematic orders far from a magnetic instability were declared in RbFe$_2$As$_2$ and its sister compounds. Here we report a systematic elastoresistance study of series of isovalent- and electron-doped KFe$_2$As$_2$ crystals. We found divergent elastoresistance upon cooling for all the crystals along their [110] direction. The amplitude of elastoresistivity diverges if K is substituted with larger ions or if the system is driven towards a Lifshitz transition. However, we conclude none of them necessarily indicates an independent nematic critical point. Instead, the increased nematicity can be associated with another electronic criticality. In particular, we propose a mechanism how elastoresistivity is enhanced at a Lifshitz transition.

cond-mat.supr-con

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

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

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