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Dariusz J. Gawryluk

Publications and source records attributed to Dariusz J. Gawryluk.

16 recordsLinked to original sources

Pressure-Invariant Isotope Effect as Evidence for Electronically Driven Intertwined Order in Pr$_4$Ni$_3$O$_{10}$

We report muon-spin rotation measurements of the pressure dependence of the oxygen-isotope ($^{16}$O/$^{18}$O) effect on the spin-density wave (SDW) transition in the trilayer Ruddlesden-Popper nickelate Pr$_4$Ni$_3$O$_{10}$. At ambient pressure, the SDW transition shows a finite isotope shift, with $^{16}T_{\rm SDW}=158.04(5)$ K and $^{18}T_{\rm SDW}=159.81(6)$ K. Under hydrostatic pressure, $T_{\rm SDW}$ decreases linearly at nearly identical rates for the two isotope compositions, ${\rm d}\,^{16}T_{\rm SDW}/{\rm d}p=-4.93(5)$ K/GPa and ${\rm d}\,^{18}T_{\rm SDW}/{\rm d}p=-4.90(7)$ K/GPa, such that the isotope shift remains essentially unchanged under compression. The absence of pressure enhancement of the isotope effect points to a predominantly electronic origin of the SDW transition and is consistent with recent inelastic x-ray scattering results, suggesting a new regime of intertwined order in trilayer RP nickelates, which is stabilized by strong spin interactions.

cond-mat.supr-con↗

Multiple Magnetic Transitions in the Trilayer Nickelate Pr$_4$Ni$_3$O$_{10}$ Revealed by Muon-Spin Rotation

A muon-spin rotation/relaxation ($μ$SR) study of the trilayer Ruddlesden--Popper nickelate Pr$_4$Ni$_3$O$_{10}$ was performed at ambient pressure and under hydrostatic pressure up to 2.2 GPa. Three magnetic transitions were identified at ambient pressure: the onset of spin-density-wave (SDW) order at $T_{\rm SDW} \simeq 158$ K, an intermediate-temperature transition at $T^{\ast} \simeq 90$--100 K, and a low-temperature transition at $T_{\rm SDW}^{\rm Pr} \simeq 25$--27 K. While the intermediate transition at $T^{\ast}$ induces only minor changes in the internal-field distribution, the transition at $T_{\rm SDW}^{\rm Pr}$ is accompanied by a pronounced reconstruction of the magnetic structure, consistent with previous reports attributing enhanced interlayer coherence to the ordering of the Pr sublattice. The high-temperature transition at $T_{\rm SDW}$ is characterized by the sharp development of static internal magnetic fields with a narrow transition width of $0.65(4)$ K. Weak-transverse-field measurements reveal a finite thermal hysteresis of $0.27(6)$ K, with $T_{\rm SDW}^{\rm warming} > T_{\rm SDW}^{\rm cooling}$, indicating weakly first-order-like behavior. Hydrostatic pressure suppresses $T_{\rm SDW}$ linearly and reduces the ordered Ni magnetic moment $M$, with corresponding rates of ${\rm d}T_{\rm SDW}/{\rm d}p = -4.9(1)$ K/GPa and ${\rm d}\ln M/{\rm d}p = -2.0(5)\times10^{-2}$ GPa$^{-1}$, respectively, thereby demonstrating a gradual weakening of the spin-density-wave instability under compression.

cond-mat.supr-con↗

Oxygen-isotope effect on density wave transitions in La$_3$Ni$_2$O$_{7}$

TThe isotope effect is a powerful probe of electron-phonon interactions in solid-state systems, offering key insights into how atomic mass influences emergent quantum states. Here, the impact of oxygen isotope substitution ($^{16}{\rm O}\rightarrow \; ^{18}{\rm O}$) on charge- and spin-density wave (CDW and SDW) transitions in the double-layer Ruddlesden-Popper nickelate La$_3$Ni$_2$O$_7$ is investigated. A clear isotope effect is observed in the CDW transition: the transition temperature ($T_{\rm CDW}$) increases upon $^{18}$O substitution. In contrast, the SDW transition temperature remains unaffected within experimental uncertainty. These findings point to a strong involvement of lattice vibrations in the formation of charge order, while spin order appears to be predominantly of electronic origin. The results suggest that electron-phonon coupling, manifested through the CDW response to isotope substitution, may be relevant to the superconducting pairing mechanism in Ruddlesden-Popper nickelates.

cond-mat.supr-con↗

Effect of Pressure and Oxygen-Isotope Substitution on Density-Wave Transitions in La$_4$Ni$_3$O$_{10}$

Understanding the interplay between magnetism and superconductivity in nickelate systems is a key objective in condensed matter physics. Here, we present a systematic muon-spin rotation/relaxation ($μ$SR) and resistivity study of the trilayer Ruddlesden-Popper nickelate La$_4$Ni$_3$O$_{10}$ under ambient and applied pressure, combined with oxygen-isotope substitution. At ambient pressure, two incommensurate spin-density-wave (SDW) transitions are identified at $T_{SDW}\simeq132$ K and $T^\ast\simeq80-90$ K. Comparison of the internal magnetic fields with dipole-field calculations reveals a magnetic structure consistent with antiferromagnetically coupled SDW order on the outer two Ni layers, with smaller moments on the inner layer. Above $T^\ast$, the moments lie mainly in the $ab$ plane, whereas below this temperature they develop a $c$-axis component. The internal fields at the muon stopping sites appear abruptly at $T_{SDW}$, suggesting a first-order-like SDW transition closely linked to the charge-density-wave (CDW) order occurring at the same temperature ($T_{SDW}=T_{CDW}$). Under pressure, all transition temperatures -- $T_{SDW}$, $T^\ast$, and $T_{CDW}$ -- are suppressed at a nearly uniform rate of $\simeq-13$ K/GPa. This contrasts with bilayer La$_3$Ni$_2$O$_7$, where pressure enhances the separation between the SDW and CDW transitions. Oxygen-isotope substitution ($^{16}$O $\rightarrow$ $^{18}$O) shifts $T_{CDW}$ to higher values. The isotope effect on $T_{SDW}$ and $T^\ast$ differs markedly: when CDW and SDW are intertwined, a notable isotope effect is observed on $T_{SDW}$, yielding nearly identical isotope shifts for $T_{CDW}$ and $T_{SDW}$, whereas no isotope effect is detected at $T^\ast$, where the SDW transition occurs independently of the CDW.

cond-mat.supr-con↗

Magnetism of the alternating monolayer-trilayer phase of La$_3$Ni$_2$O$_7$

Understanding the magnetic ground state of Ruddlesden-Popper nickelates is crucial, as these materials exhibit superconductivity under high pressure and host competing electronic orders that may play a key role in the pairing mechanism. In this work, we investigate the magnetic properties of the alternating monolayer-trilayer phase of La$_3$Ni$_2$O$_7$ (1313-La$_3$Ni$_2$O$_7$) using muon-spin rotation/relaxation ($μ$SR) under both ambient and hydrostatic pressure conditions. The monolayer-trilayer phase develops incommensurate magnetic order below approximately 150 K, with a mean ordering temperature of $T_{SDW} \simeq 123$ K and a transition width of $ΔT_{SDW} \simeq 15$ K. The abrupt onset of the internal magnetic field indicates a first-order-like transition. Hydrostatic pressure ($p$) suppresses the magnetic ordering temperature at a rate of $dT_{SDW}/d p \simeq -3.9$ K/GPa, demonstrating a progressive destabilization of the ordered state. By comparison with the bilayer 2222-La$_3$Ni$_2$O$_7$ and the trilayer 3333-La$_4$Ni$_3$O$_{10}$ systems, and within a unified phenomenological framework, systematic trends are identified linking the pressure dependence of $T_{SDW}$, the (in)commensurability of the magnetic order, and the character of the magnetic transition. These trends consistently indicate a gradual reduction of electronic correlation strength from the bilayer to the monolayer-trilayer and trilayer nickelates. This hierarchy suggests that the higher superconducting transition temperature observed in the 2222 phase may be closely connected to its more strongly correlated electronic nature. These results position the alternating monolayer-trilayer 1313-La$_3$Ni$_2$O$_7$ as an intermediate member linking the magnetic behavior of the bilayer 2222-La$_3$Ni$_2$O$_7$ and the trilayer 3333-La$_4$Ni$_3$O$_{10}$ Ruddlesden-Popper compounds.

cond-mat.supr-con↗

Persistence of small polarons into the superconducting phase of Ba$_{1-x}$K$_x$BiO$_3$

Bipolaronic superconductivity is an exotic pairing mechanism proposed for materials like Ba$_{1-x}$K$_x$BiO$_3$ (BKBO); however, conclusive experimental evidence for a (bi)polaron metallic state in this material remains elusive. Here, we combine resonant inelastic x-ray and neutron total scattering techniques with advanced modelling to study the local lattice distortions, electronic structure, and electron-phonon coupling ($e$-ph) in BKBO as a function of doping. Data for the parent compound ($x = 0$) indicates that the electronic gap opens in predominantly oxygen-derived states strongly coupled to a long-range ordered breathing distortion of the oxygen sublattice. Upon doping, short-range breathing distortions and sizable ($e$-ph) coupling persist into the superconducting regime ($x = 0.4$). Comparisons with exact diagonalization and determinant quantum Monte Carlo calculations further support this conclusion. Our results provide compelling evidence that BKBO's metallic phase hosts a liquid of small (bi)polarons derived from local breathing distortions of the lattice, with implications for understanding the low-temperature superconducting instability

cond-mat.supr-con↗

Discovery of nodal-line superconductivity in chiral crystals

Chiral crystals, whose key feature is the structural handedness, host exotic quantum phenomena driven by the interplay of band topology, spin-orbit coupling (SOC), and electronic correlations. Due to the limited availability of suitable chiral-crystal materials, their unconventional superconductivity (SC) remains largely unexplored. Here, we report the discovery of unconventional SC in the La(Rh,Ir)Si family of materials by combining muon-spin spectroscopy, band-structure calculations, and perturbation theory. This family, characterized by a double-helix chiral structure, hosts exotic multifold fermions that are absent in other topological chiral crystals. While LaRhSi behaves as a fully-gapped superconductor, the substitution of 4$d$-Rh by 5$d$-Ir significantly enhances the SOC and leads to the emergence of topological nodal-line SC in LaIrSi. The developed model shows that the nodal-line SC arises from an isotropic SOC with a specific strength. Such an exotic mechanism expands our conventional understanding of material candidates for unconventional SC, which typically rely on a significantly anisotropic SOC to promote the triplet pairing. Our work establishes a new type of phase diagram, which provides a comprehensive roadmap for identifying and engineering unconventional SC in chiral crystals. Furthermore, it calls for renewed investigations of unconventional SC in other widely studied superconductors with a chiral structure.

cond-mat.supr-con↗

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↗

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↗

Magnetic Phase Diagram of ErB$_4$ as Explored by Neutron Scattering

The tetragonal $4f$-electron intermetallic ErB$_4$ is characterized by strong Ising anisotropy along the tetragonal $c$ axis. The magnetic moments on the erbium sites can be mapped onto a Shastry-Sutherland (SSL) lattice resulting in geometrical frustration. At zero magnetic field ErB$_4$ exhibits collinear columnar antiferromagnetic (CAFM) order below $T_\text{N} = 15.4$ K. In the presence of a magnetic field parallel to the $c$ axis, ErB$_4$ exhibits a plateau at $1/2$ of the saturation magnetization $M_\text{S}$, which arises at a spin flip transition at $H_1$ $=$ 1.9 T. Fractional magnetization plateaus and other exotic spin phases are a well-established characteristic feature of frustrated spin systems. Monte Carlo simulations propose that ErB$_4$ is an ideal candidate to feature a spin supersolid phase in close vicinity of $H_1$ between the CAFM and $M/M_\text{S}=1/2$ plateau (HP) phase. Here we combine single-crystal neutron diffraction and inelastic neutron scattering to study the magnetic phase diagram and the crystal electric field (CEF) ground state of ErB$_4$. Our measurements as a function of magnetic field find no signature of the spin supersolid phase but allow us to determine the magnetic structure of the HP phase to be of the uuud type consistent with an Ising material. The magnetic moment $μ_{\mathrm{CEF}}$ $=$ 8.96 $μ_B$ expected from the CEF configuration determined by our inelastic neutron scattering measurements is also consistent with the ordered moment observed in neutron diffraction showing that the moments are fully ordered and close to the Er$^{3+}$ free ion moment (9.6 $μ_B$).

cond-mat.str-el↗

Magnetostructural Coupling at the Néel point in YNiO3 Single Crystals

The recent discovery of superconductivity in infinite layer thin films and bulk Ruddlesden-Popper nickelates has stimulated the investigation of other predicted properties of these materials. Among them, the existence of magnetism-driven ferroelectricity in the parent compounds RNiO3 (R = 4f lanthanide and Y) at the onset of the Néel order, TN, has remained particularly elusive. Using diffraction techniques, we reveal here the existence of magnetostriction at TN in bulk YNiO3 single crystals. Interestingly, the associated lattice anomalies are much more pronounced along the b crystal axis, which coincides with the electric polarization direction expected from symmetry arguments. This axis undergoes an abrupt contraction below TN that reaches deltab/b ~ - 0.01 %, a value comparable to those found in some magnetoresistive manganites and much larger than those reported for magnetism-driven multiferroics. This observation suggests a strong spin-lattice coupling in these materials, consistent with theoretical predictions. Using the symmetry-adapted distortion mode formalism we identify the main ionic displacements contributing to the lattice anomalies and discuss the most likely polar displacements below TN. Furthermore, our data support symmetric superexchange as the most likely mechanism responsible for the magnetoelastic coupling. These results, that may be common to the full RNiO3 family, provide new experimental evidence supporting the predicted existence of magnetism-driven ferroelectricity in RNiO3 perovskites

cond-mat.str-el↗

Spin order and dynamics in the topological rare-earth germanide semimetals

The $RE$Al(Si,Ge) ($RE$ = rare earth) family, known to break both the inversion- and time-reversal symmetries, represents one of the most suitable platforms for investigating the interplay between correlated-electron phenomena and topologically nontrivial bands. Here, we report on systematic magnetic, transport, and muon-spin rotation and relaxation ($μ$SR) measurements on (Nd,Sm)AlGe single crystals, which exhibit antiferromagnetic (AFM) transitions at $T_\mathrm{N} = 6.1$ and 5.9 K, respectively. In addition, NdAlGe undergoes also an incommensurate-to-commensurate ferrimagnetic transition at 4.5 K. Weak transverse-field $μ$SR measurements confirm the AFM transitions, featuring a $\sim$90 % magnetic volume fraction. In both cases, zero-field (ZF) $μ$SR measurements reveal a more disordered internal field distribution in NdAlGe than in SmAlGe, reflected in a larger transverse muon-spin relaxation rate $λ^\mathrm{T}$ at $T \ll T_\mathrm{N}$. This may be due to the complex magnetic structure of NdAlGe, which undergoes a series of metamagnetic transitions in an external magnetic field, while SmAlGe shows only a robust AFM order. In NdAlGe, the topological Hall effect (THE) appears between the first and the second metamagnetic transitions for $H \parallel c$, while it is absent in SmAlGe. Such THE in NdAlGe is most likely attributed to the field-induced topological spin textures. The longitudinal muon-spin relaxation rate $λ^\mathrm{L}(T)$, diverges near the AFM order, followed by a clear drop at $T < T_\mathrm{N}$. In the magnetically ordered state, spin fluctuations are significantly stronger in NdAlGe than in SmAlGe. In general, our longitudinal-field $μ$SR data indicate vigorous spin fluctuations in NdAlGe, thus providing valuable insights into the origin of THE and of the possible topological spin textures in $RE$Al(Si,Ge) Weyl semimetals.

cond-mat.str-el↗

YBa$_{1-x}$Sr$_{x}$CuFeO$_{5}$ layered perovskites: exploring the magnetic order beyond the paramagnetic-collinear-spiral triple point

Layered perovskites of general formula AA'CuFeO$_5$ are one of the few examples of cycloidal spiral magnets where the ordering temperatures $T_{spiral}$ can be tuned far beyond room temperature by introducing modest amounts of Cu/Fe chemical disorder in the crystal structure. This rare property makes these materials prominent candidates to host multiferroicity and magnetoelectric coupling at room temperature. Moreover, it has been proposed that the highest $T_{spiral}$ value that can be reached in this structural family ($\sim$ 400 K) corresponds to a paramagnetic-collinear-spiral triple point with potential to show exotic physics. Since generating high amounts of Cu/Fe disorder is experimentally difficult, the phase diagram region beyond the triple point has been barely explored. To fill this gap we investigate here the YBa$_{1-x}$Sr$_{x}$CuFeO$_{5}$ solid solutions ($0 \leq x \leq 1$), where we replace Ba with Sr with the aim of enhancing the impact of the experimentally available Cu/Fe disorder. Using a combination of bulk magnetization, synchrotron X-ray and neutron powder diffraction we show that the spiral state is destabilized beyond a critical degree of Cu/Fe disorder, being replaced by a non-frustrated, fully antiferromagnetic state with propagation vector k$_{c2}$ = $(\frac{1}{2}, \frac{1}{2}, 0)$ and ordering temperature $T_{coll2}$ $\geq$ $T_{spiral}$, which is progressively stabilized beyond the triple point. Interestingly, $T_{spiral}$ and $T_{coll2}$ increase with $x$ at the same rate. This suggests a common, disorder-driven origin, consistent with theoretical predictions.

cond-mat.str-el↗

Crystal-field states and defect levels in candidate quantum spin ice Ce$_{2}$Hf$_{2}$O$_{7}$

We report the synthesis of powder and single-crystal samples of the cerium pyrohafnate and their characterization using neutron diffraction, thermogravimetry and X-ray absorption spectroscopy. We evaluate the amount of non-magnetic Ce$^{4+}$ defects and use this result to interpret the spectrum of crystal-electric field transitions observed using inelastic neutron scattering. The analysis of these single-ion transitions indicates the dipole-octupole nature of the ground state doublet and a significant degree of spin-lattice coupling. The single-ion properties calculated from the crystal-electric field parameters obtained spectroscopically are in good agreement with bulk magnetic susceptibility data down to about 1 K. Below this temperature, the behavior of the magnetic susceptibility indicates a correlated regime without showing any sign of magnetic long-range order or freezing down to 0.08 K. We conclude that Ce$_2$Hf$_2$O$_{7}$ is another candidate to investigate exotic correlated states of quantum matter such as the octupolar quantum spin ice recently argued to exist in the isostructural compounds Ce$_2$Sn$_2$O$_7$ and Ce$_2$Zr$_2$O$_7$.

cond-mat.str-el↗

Cu-doping effects on the ferromagnetic semimetal CeAuGe

We present a study of Cu-substitution effects in 4f-Ce intermetallic compound CeAu1-xCuxGe, with potentially unusual electronic states, in the whole concentration range (x = 0.0 - 1.0). The parent CeAuGe compound, crystallizing in a non-centrosymmetric hexagonal structure, is a ferromagnetic semimetal with Curie temperature 10 K. Cu-doping on Au-site of CeAuGe, CeAu1-xCuxGe, changes the crystal structure from the non-centrosymmetric (P63mc) to centrosymmetric (P63/mmc) space group at the concentration x ~ 0.5, where the c-lattice constant has a maximum value. Magnetic susceptibility and electrical resistivity measurements reveal that all Cu-doped compounds undergo magnetic phase transition near 10 K, with the maximum transition temperature of 12 K for x = 0.5. The neutron powder diffraction experiments show the ferromagnetic ordering of Ce3+ magnetic moments with a value of ~ 1.2 Bohr magneton at 1.8 K, oriented perpendicular to the hexagonal c-axis. By using symmetry analysis, we have found the solutions for the magnetic structure in the ferromagnetic Shubnikov space groups Cmc'21' and P21'/m' for x < 0.5 and x >= 0.5, respectively. Electrical resistivity exhibits a metallic temperature behaviour in all compounds. The resistivity has a local minimum in the paramagnetic state due to Kondo effects at high doping x = 0.8 and 1.0. At the small Cu-doping level, x = 0.2, the resistivity shows a broad feature at the ferromagnetic transition temperature and an additional transition-like peculiarity at 2.5 K in the ferromagnetic state.

cond-mat.str-el↗

RENiO3 single crystals (RE = Nd, Sm, Gd, Dy, Y, Ho, Er, Lu) grown from molten salts under 2000 bar oxygen-gas pressure

The electronic properties of transition-metal oxides with highly correlated electrons are of central importance in modern condensed matter physics and chemistry, both for their fundamental scientific interest, and for their potential for advanced electronic applications. The design of materials with tailored properties has been, however, restricted by the limited understanding of their structure-property relationships, which are particularly complex in the proximity of the regime where localized electrons become gradually mobile. RENiO3 perovskites, characterized by the presence of spontaneous metal to insulator transitions, are one of the most widely used model materials for the investigation of this region in theoretical studies. However, crucial experimental information needed to validate theoretical predictions is still lacking due to their challenging high-pressure synthesis, which has prevented to date the growth of sizable bulk single crystals with RE different than La, Pr and Nd. Here we report the first successful growth of single crystals with RE = Nd, Sm, Gd, Dy, Y, Ho, Er and Lu and sizes up to ~75 μm, grown from molten salts in temperature gradient under 2000 bar oxygen gas pressure. The crystals display regular prismatic shapes with flat facets, and their crystal structures, metal-insulator and antiferromagnetic order transition temperatures are in excellent agreement with previously reported values obtained from polycrystalline samples. The availability of such crystals opens access to measurements that have hitherto been impossible to conduct. This should contribute to a better understanding of the fascinating properties of materials with highly correlated electrons, and guide future efforts to engineer transition metal oxides with tailored functional properties.

cond-mat.mtrl-sci↗