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Since their theoretical discovery more than a half-century ago, vortices observed in bulk superconductors have carried a quantized value of magnetic flux determined only by fundamental constants. A recent experiment reported 'unquantized' quantum vortices carrying the same fraction of flux quantum in Ba$_{0.23}$K$_{0.77}$Fe$_2$As$_2$ in a small temperature range below its superconducting critical temperature ($T_C$). Here, we use scanning superconducting quantum interference device (sSQUID) microscopy with improved sensitivity to investigate the genesis of fractional vortices in Ba$_{0.23}$K$_{0.77}$Fe$_2$As$_2$. We report the direct observation of a single-flux quantum vortex splitting into two different fractions with increasing temperature. The flux of the two fractions has opposite dependence on temperature, while the total flux sums up to one flux quantum despite their spatial separation. Overall, our study shows the existence of different fractional vortices and their stability in temperature ranging from 0.1 to 0.99 $T_C$. Besides the implications of this observation for the fundamental question of quantum vorticity, the discovery of these objects paves the way for the new platform for anyon quasiparticles and applications for fractional fluxonics.

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., Comment: 16 pages, 4 figures

Recent experiments have pointed to the formation of a new state of matter, the electron quadrupling condensate in Ba$_{1-x}$K$_x$Fe$_2$As$_2$. The state spontaneously breaks time-reversal symmetry and is sandwiched between two critical points, separating it from the superconducting and normal-metal states. We report a theory of the acoustic effects of systems with an electron quadrupling phase based on ultrasound-velocity measurements of Ba$_{1-x}$K$_x$Fe$_2$As$_2$ single crystals. The theoretical analysis suggests that the ultrasound data can be understood by considering a plain $s$+i$d_{xy}$ order parameter or an $s$+i$s$ order parameter with symmetry-breaking deformations in this material with enhanced nematic susceptibility for the [110] direction, or when the transition to the quartic state is a weakly first-order. Our work provides the theoretical basis and proposes the experimental strategy to study the order parameter symmetry of emerging quadrupling condensates in superconductors., Comment: v2: The crystal orientation is corrected and the ultrasound data re-analyzed. Data for a reference sample at a different doping without the BTRS state is added. 11 pages, 6 figures

The present studies show that long-range magnetic order takes place in RuBr$_3$ at $\approx$ 34 K. The observations of clear oscillations in the muon time spectra demonstrate the presence of well-defined internal fields at the muon sites. The magnetic ordering appears to be very robust and static suggesting a more conventional nature of magnetic ordering in the RuBr$_3$ system at zero field. Present investigations prove that in RuBr$_3$ the Kitaev interactions are likely to be weakened at zero field in comparison to the $\alpha$-RuCl$_3$ system. This proves that it is possible to tune the Kitaev interactions by replacing Cl with heavier halogen elements such as Br., Comment: 5 pages, 5 figures

We report on a novel material obtained by modifying pristine YBCO superconductor in solid phase synthesis via simultaneous partial substitution of Ba by Sr and O by Se. Simultaneous application of EDX and EBSD confirmed that Se atoms indeed enter the crystalline lattice cell. The detailed XRD analysis further confirmed this conclusion and revealed that the obtained polycrystalline material contains 5 phases, with the major phase ($>$30\%) being a cuprate YBa$_{1.4}$Sr$_{0.6}$Cu$_{3}$O$_{6}$Se$% _{0.51}$. The obtained superconductor demonstrates unique properties, including i) two superconducting transitions with $T_{c1}\approx$ 35 K (granular surface phase) and $T_{c2}\approx$ 13 K (bulk granular phase) - this granular phase arrangement naturally yields the Wohlleben effect; ii) reentrant diamagnetism and resistive state; iii) strong paramagnetism with Curie-Weiss behavior (% $\theta_{CW} \approx$ 4 K) and the ferromagnetic phase overruled by superconductivity; iv) Schottky anomaly visible in the heat capacity data and most likely delivered by small clusters of magnetic moments. Thorough analysis of the heat capacity data reveals a strong-coupling $d-$wave pairing in its bulk phase (with $2\Delta /T_{c}\approx 5$), and, most importantly, a very unusual anomaly in this cuprate. There are reasons to associate this anomaly with the quantum criticality observed in traditional cuprate superconductors at much higher fields (achievable only in certain laboratories). In our case, the fields leading to quantum criticality are much weaker ($\sim $7-9 T) thus opening avenues for exploration of the interplay between superconductivity and pair density waves by the wider research community.

We report on measurements of the in-plane magnetic penetration depth ($\lambda_{\rm ab}$) 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 $\lambda^{-2}_{\rm ab}$ 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 $\lambda_{ab}^{-2}$ as a function of the applied magnetic field. The experimental zero-field and zero-temperature value of $\lambda_{\rm ab}=124(3)$ nm agrees with $\lambda_{\rm ab}\simeq 130$ 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 $\lambda_{\rm ab}^{-2}$ on $T$, so the higher angular harmonics of the energy gap function need to be introduced., Comment: 7 pages, 3 figures

The ability to efficiently control charge and spin in the cuprate high-temperature superconductors is crucial for fundamental research and underpins technological development. Here, we explore the tunability of magnetism, superconductivity and crystal structure in the stripe phase of the cuprate La_2-xBa_xCuO_4, with x = 0.115 and 0.135, by employing temperature-dependent (down to 400 mK) muon-spin rotation and AC susceptibility, as well as X-ray scattering experiments under compressive uniaxial stress in the CuO_2 plane. A sixfold increase of the 3-dimensional (3D) superconducting critical temperature T_c and a full recovery of the 3D phase coherence is observed in both samples with the application of extremely low uniaxial stress of 0.1 GPa. This finding demonstrates the removal of the well-known 1/8-anomaly of cuprates by uniaxial stress. On the other hand, the spin-stripe order temperature as well as the magnetic fraction at 400 mK show only a modest decrease under stress. Moreover, the onset temperatures of 3D superconductivity and spin-stripe order are very similar in the large stress regime. However, a substantial decrease of the magnetic volume fraction and a full suppression of the low-temperature tetragonal structure is found at elevated temperatures, which is a necessary condition for the development of the 3D superconducting phase with optimal T_c. Our results evidence a remarkable cooperation between the long-range static spin-stripe order and the underlying crystalline order with the three-dimensional fully coherent superconductivity. Overall, these results suggest that the stripe- and the SC order may have a common physical mechanism., Comment: 11 pages, 5 figures. This work builds on our earlier findings on LBCO, arXiv:2008.01159, and substantially expands it

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., Comment: 19 pages, 9 figures

Muon spin rotation/relaxation ($\mu$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 $\mu$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 $\mu$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 $T_\text{c}$., Comment: 9 pages, 4 figures and Appendix, accepted for publication in PRB

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., Comment: 12 pages, 3 figures and Supplementary information

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.

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., Comment: 31 pages, 11 figures, supplemental information

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., Comment: 14 pages, 8 Figures

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., Comment: Review of Scientific Instruments accepted for publication Oct 2020, 9 pages, 8 figures

We report muon spin rotation and magnetic susceptibility experiments on in-plane stress effects on the static spin-stripe order and superconductivity in the cuprate system La2-xBaxCuO4 with x = 0.115. An extremely low uniaxial stress of 0.1 GPa induces a substantial decrease in the magnetic volume fraction and a dramatic rise in the onset of 3D superconductivity, from 10 to 32 K; however, the onset of at-least-2D superconductivity is much less sensitive to stress. These results show not only that large-volume-fraction spin-stripe order is anti-correlated with 3D superconducting (SC) coherence, but also that these states are energetically very finely balanced. Moreover, the onset temperatures of 3D superconductivity and spin-stripe order are very similar in the large stress regime. These results strongly suggest a similar pairing mechanism for spin-stripe order, the spatially-modulated 2D and uniform 3D SC orders, imposing an important constraint on theoretical models., Comment: To appear in Physical Review Letters (2020)

Recently, several putative quantum spin liquid (QSL) states were discovered in ${\tilde S} = 1/2$ rare-earth based triangular-lattice antiferromagnets (TLAF) with the delafossite structure. A way to clarify the origin of the QSL state in these systems is to identify ways to tune them from the putative QSL state towards long-range magnetic order. Here, we introduce the Ce-based TLAF KCeS$_2$ and show via low-temperature specific heat and $\mu$SR investigations that it yields magnetic order below $T_{\mathrm N} = 0.38$ K despite the same delafossite structure. We identify a well separated ${\tilde S} = 1/2$ ground state for KCeS$_2$ from inelastic neutron scattering and embedded-cluster quantum chemical calculations. Magnetization and electron spin resonance measurements on single crystals indicate a strong easy-plane $g$~factor anisotropy, in agreement with the ab initio calculations. Finally, our specific-heat studies reveal an in-plane anisotropy of the magnetic field-temperature phase diagram which may indicate anisotropic magnetic interactions in KCeS$_2$., Comment: submission to Scipost Physics

We present an extensive study of the structural, magnetic and thermodynamic properties of high-quality monocrystals of the two heterometallic oxyborates from the ludwigite family: Cu$_2$GaBO$_5$ and Cu$_2$AlBO$_5$ in the temperature range above 2 K. The distinctive feature of the investigated structures is the selective distribution of Cu and Ga/Al cations. The unit cell of Cu$_2$GaBO$_5$ and Cu$_2$AlBO$_5$ contains four nonequivalent crystallographic sites of metal ions. Two sites in the structure from four nonequivalent crystallographic sites of metal ions of Cu$_2$GaBO$_5$ are fully occupied by Cu atoms which form the quasi one-dimensional chains along the a-axis. For Cu$_2$AlBO$_5$ all sites are partially occupied by Al and Cu atoms. The joint analysis of low-temperature data on magnetic susceptibility and magnetic contribution to the specific heat showed that Cu$_2$AlBO$_5$ and Cu$_2$GaBO$_5$ exhibit an antiferromagnetic transition at $T_{\rm N} \approx 3$ and 4 K, respectively. The magnetic contributions to the specific heat for both compounds were obtained after subtracting the phonon contribution. It is shown that the external magnetic field above 2.5 T leads to a broadening of the magnetic phase transition indicating suppression of the long-range antiferromagnetic order.

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-$\mu$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$_4$., Comment: 28 pages, 12 figures

Rare-earth delafossites were recently proposed as promising candidates for the realization of an effective $S$=1/2 quantum spin liquid (QSL) on the triangular lattice. In contrast to the most actively studied triangular-lattice antiferromagnet YbMgGaO$_4$, which is known for considerable structural disorder due to site intermixing, NaYbS$_2$ delafossite realizes structurally ideal triangular layers. We present detailed $\mu$SR studies on this regular (undistorted) triangular Yb sublattice based system with effective spin $J_{\mathrm{eff}}=1/2$ in the temperature range 0.05 - 40 K. Zero-field (ZF) and longitudinal field (LF) $\mu$SR studies confirm the absence of any long range magnetic order state down to 0.05K ($\sim J$/80). Current $\mu$SR results together with the so far available bulk characterization data suggest that NaYbS$_2$ is an ideal candidate to identify QSL ground state., Comment: Submitted to PRB as Rapid communication on 18th Oct19

We report muon spin rotation ($\mu$SR) and magnetization measurements under pressure on Fe$_{1+\delta}$Se$_\mathrm{1\text{-}x}$S$_\mathrm{x}$ with x $\approx 0.11$.Above $p\approx0.6$ GPa we find microscopic coexistence of superconductivity with an extended dome of long range magnetic order that spans a pressure range between previously reported separated magnetic phases. The magnetism initially competes on an atomic scale with the coexisting superconductivity leading to a local maximum and minimum of the superconducting $T_\mathrm{c}(p)$. The maximum of $T_\mathrm{c}$ corresponds to the onset of magnetism while the minimum coincides with the pressure of strongest competition. A shift of the maximum of $T_\mathrm{c}(p)$ for a series of single crystals with x up to 0.14 roughly extrapolates to a putative magnetic and superconducting state at ambient pressure for x $\geq0.2$., Comment: 10 pages, 6 figures, including supplemental material

The interplay between the nematic order and magnetism in FeSe is not yet well understood. There is a controversy concerning the relationship between orbital and spin degrees of freedom in FeSe and their relevance for superconductivity. Here we investigate the effect of S substitution on the nematic transition temperature ($T_{\rm n}$) and the low-energy spin fluctuations (SF) in FeSe single crystals. We show that the low-energy SF emerge below the nematic transition. The difference between the onset temperature for the critical SF ($T_{\rm SF}$) and $T_{\rm n}$ is small for FeSe but significantly increases with S substitution. Below $T_{\rm SF}$ the Korringa relation is violated and the effective muon hyperfine coupling constant changes a sign. Our results exclude a direct coupling of the low-energy SF to the electronic nematic order indicating a presence of multiple spin degrees of freedom in FeSe$_{\rm 1-x}$S$_{\rm x}$., Comment: 8 pages, 5 figures