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O. Stockert

Publications and source records attributed to O. Stockert.

At least 19 recordsLinked to original sources

Proximate quantum spin liquid state in the frustrated HoInCu$_4$ metal

We conducted a comprehensive and comparative muon-spin relaxation and rotation ($\mu$SR) investigation on two fcc-lattice metallic compounds, HoCdCu$_4$ ($T_\mathrm{N}\approx 8$ K) and HoInCu$_4$ ($T_\mathrm{N}\approx 0.76$ K), to elucidate the nature of their magnetic ground states and the role of frustration in stabilizing them. Our $\mu$SR results reveal that, in contrast to HoCdCu$_4$, strong magnetic frustration exists in HoInCu$_4$. Notably, in HoInCu$_{4}$, only 30% of the Ho-moments participate in the static magnetic ordering below $T_\mathrm{N}$, while the remaining 70% of the Ho-moments exhibit dynamic correlations and persistent spin dynamics down to 0.3 K, resembling a quantum spin-liquid (QSL) behavior. By contrast, in HoCdCu$_{4}$, all the Ho-moments contribute to the magnetic order below $T_\mathrm{N}$. Furthermore, in HoInCu$_{4}$, the temperature dependence of the relaxation rate indicates the presence of quantum critical fluctuations in the paramagnetic state near $T_\mathrm{N}$, suggesting the proximity to a quantum critical point (QCP). These observations suggest that the ground state of HoInCu$_{4}$ is a proximate quantum spin liquid (PQSL), a state that has not been reported before in frustrated metallic systems. Our $\mu$SR findings are further corroborated by recent inelastic neutron results on HoInCu$_4$, which show similarities to other insulating PQSL candidates, thus reinforcing our conclusions.

cond-mat.str-el

Microscopic evidence of a field-induced critical spin-liquid state in a frustrated metal

A field-induced quantum spin liquid (QSL) state is an extraordinary phenomenon, hitherto unobserved in metallic frustrated compounds. Recent bulk measurements have revealed intriguing field-induced magnetic states in metallic frustrated CePdAl. However, the nature of these field-induced states, potentially including a QSL state, remains unclear due to the lack of detailed microscopic investigation. To elucidate these field-induced states, we employed the transverse-field muon spin relaxation/rotation (TF-$\mu$SR) technique, applying various magnetic fields parallel to the c-axis in single-crystalline CePdAl over a broad temperature range (100~K-100~mK). Our $\mu$SR data indicate that field-induced low-temperature states for fields B$\leq B_{c2}(=3.4~T)$ exhibit long-range magnetic order, whereas for B>$B_{c2}$ they yield contrasting behavior. Notably, at 3.75 T, the transverse relaxation rate ($\lambda_T$) diverges following a power-law dependence below 800~mK along with an indication of finite frustration, whereas the Knight shift is temperature independent. These observations corroborate the signature of a critical spin-liquid (CSL) with antiferromagnetic spin fluctuations. Furthermore, at 4.3 T, a non-Fermi liquid state is observed where frustration is absent. This comprehensive microscopic study strongly suggests the existence of a CSL state in a metallic frustrated system.

cond-mat.str-el

Microscopic Origin of Reduced Magnetic Order in a Frustrated Metal

Although magnetic frustration in metals provides a promising avenue for novel quantum phenomena, their microscopic interpretation is often challenging. Here we use the face-centered cubic intermetallic HoInCu$_4$ as model material to show that Hamiltonians neglecting the charge degree of freedom are appropriate for frustrated metals possessing low density of states at the Fermi surface. Through neutron scattering techniques we determine matching magnetic exchange interactions in the paramagnetic and field-polarized states using an effective spin-1 Heisenberg Hamiltonian, for which we identify antiferromagnetic nearest and next-nearest neighbour interactions $J_1$ and $J_2$ that are close to the critical ratio $J_2$/$J_1$ = 1/2. The study further provides evidence that spin-wave theory fails to predict the low-energy spin dynamics in the antiferromagnetic zero-field state, which is dominated by overdamped magnetic excitations. We conclude that the low-energy fluctuations arise from quantum fluctuations, accounting for the missing moment of the strongly renormalized magnetic long-range order.

cond-mat.str-el

Frustration-induced quantum criticality in Ni-doped CePdAl as revealed by the $\mu$SR technique

In CePdAl, the 4$f$ moments of cerium arrange to form a geometrically frustrated kagome lattice. Due to frustration, in addition to Kondo- and Ruderman-Kittel-Kasuya-Yosida interactions, this metallic system shows a long-range magnetic order (LRO) with a $T_{\rm N}$ of only 2.7\,K. Upon Ni doping at the Pd sites, $T_{\rm N}$ is further suppressed, to reach zero at a critical concentration $x_c \approx 0.15$. Here, by using muon-spin relaxation and rotation ($\mu$SR), we investigate CePd${1-x}$Ni$_x$Al at a local level for five different Ni-concentrations, both above and below $x_c$. Like the parent CePdAl compound, for $x = 0.05$, we observe an incommensurate LRO, which turns into a quasi-static magnetic order for $x = 0.1$ and 0.14. More interestingly, away from $x_c$, for $x = 0.16$ and 0.18, we still observe a non-Fermi liquid regime, evidenced by a power-law divergence of the longitudinal relaxation at low temperatures. In this case, longitudinal field measurements exhibit a time-field scaling, indicative of a cooperative spin dynamics that persists for $x > x_c$. Furthermore, like the externally applied pressure, the chemical pressure induced by Ni doping suppresses the region below $T^*$, characterized by a spin-liquid like dynamical behavior. Our results suggest that the magnetic properties of CePdAl are similarly affected by the hydrostatic- and the chemical pressure. We also confirm that the unusual non-Fermi liquid regime (compared with conventional quantum critical systems) is due to the presence of frustration that persists up to the highest Ni concentrations.

cond-mat.str-el

Coupling between magnetic and thermodynamic properties in $R$Rh$_2$Si$_2$ ($R$ = Dy, Ho)

Single crystals of DyRh$_2$Si$_2$ and HoRh$_2$Si$_2$ were investigated by thermal expansion and magnetostriction. The different types of magnetic order can clearly be seen in these measurements, particularly the canting of the moments away from the crystallographic $c$ direction below about 12~K and the spin-flip for magnetic field applied along the $c$ direction. For HoRh$_2$Si$_2$, an additional transition just below $T_{\rm N}$ is analyzed by means of the Gr\"{u}neisen ratio and is likely caused by a change of the magnetic structure. Our results nicely corroborate findings from other magnetic and thermodynamic measurements on these materials and provide further evidence suggesting the formation of magnetic domains.

cond-mat.mtrl-sci

CeCu$_{2}$Si$_{2}$ and YbRh$_{2}$Si$_{2}$: Strange Cases of Heavy-Fermion Superconductivity

The heavy-fermion superconductor CeCu$_{2}$Si$_{2}$ exhibits two-band, $d$-wave superconductivity with a finite energy gap over the whole Fermi surface around the magnetic instability where 4$f$ antiferrerromagnetic order is suppressed. In contrast, in YbRh$_{2}$Si$_{2}$ heavy-fermion superconductivity appears only when 4$f$-electronic antiferromagnetic order is replaced at ultra-low temperatures by a combined nuclear and 4$f$-spin order. Whereas both compounds exhibit different variants of antiferromagnetic instabilities, i.e., a spin-density-wave quantum critical point in CeCu$_{2}$Si$_{2}$ and one of "partial-Mott" type in YbRh$_{2}$Si$_{2}$, in both cases the Cooper pairing, as well as the pronounced "strange-metal" behavior in YbRh$_{2}$Si$_{2}$, appear to be driven by large-to-small Fermi surface fluctuations. The transport properties and scanning tunneling spectroscopy (STS) for these materials are dominated by single-ion Kondo scatterings down to very low temperatures. Further open problems of the Kondo lattice include both the interplay between superconductivity and antiferromagnetic order as well as the onset of lattice coherence. While microscopic coexistence of superconductivity and antiferromagnetism seems to require a sufficiently large staggered moment, the onset of lattice coherence in transport measurements and STS is associated solely with the crystal-field-doublet ground state, while it involves the fully degenerate Hund's rule multiplet in ARPES.

cond-mat.supr-con

Spin-liquid signatures in the quantum critical regime of pressurized CePdAl

CePdAl is a prototypical frustrated Kondo lattice with partial long-range order (LRO) at $T_\mathrm{N}=2.7$ K. Previous bulk experiments under hydrostatic pressure found signatures for a quantum critical regime that extends from $p_\mathrm{c} \approx 0.9$ GPa, where LRO disappears, up to $\sim 1.7$ GPa. We employed extensive muon spin relaxation and rotation ($\mu$SR) experiments under pressure. The continuous and complete suppression of LRO at $p_\mathrm{c}$ is confirmed. Above $T_\mathrm{N}(p)$ and beyond $p_\mathrm{c}$, an additional crossover scale $T^\ast(p)$ characterizes the change from pure to stretched exponential relaxation in zero field. Remarkably $T^\ast(p)$ agrees with previously determined signatures of entropy accumulation above LRO. This coincidence microscopically evidences fluctuating frustrated spins at $T\leq T^\ast$ with spin-liquid behavior. Power-law divergences of the temperature and longitudinal field dependences of the relaxation rate, with time-field scaling, at pressures between $p_c$ and 1.7 GPa characterize this regime as quantum critical.

cond-mat.str-el

Gradual pressure-induced enhancement of magnon excitations in CeCoSi

CeCoSi is an intermetallic antiferromagnet with a very unusual temperature-pressure phase diagram: at ambient pressure it orders below $T_{\mathrm{N}} = 8.8$ K, while application of hydrostatic pressure induces a new magnetically ordered phase with exceptionally high transition temperature of $\sim40$ K at 1.5 GPa. We studied the magnetic properties and the pressure-induced magnetic phase of CeCoSi by means of elastic and inelastic neutron scattering (INS) and heat capacity measurements. At ambient pressure CeCoSi orders into a simple commensurate AFM structure with a reduced ordered moment of only $m_{\mathrm{Ce}} = 0.37(6)$ $\mu_{\mathrm{B}}$. Specific heat and low-energy INS indicate a significant gap in the low-energy magnon excitation spectrum in the antiferromagnetic phase, with the CEF excitations located above 10 meV. Hydrostatic pressure gradually shifts the energy of the magnon band towards higher energies, and the temperature dependence of the magnons measured at 1.5 GPa is consistent with the phase diagram. Moreover, the CEF excitations are also drastically modified under pressure.

cond-mat.str-el

Multidimensional entropy landscape of quantum criticality

The Third Law of Thermodynamics states that the entropy of any system in equilibrium has to vanish at absolute zero temperature. At nonzero temperatures, on the other hand, matter is expected to accumulate entropy near a quantum critical point (QCP), where it undergoes a continuous transition from one ground state to another. Here, we determine, based on general thermodynamic principles, the spatial-dimensional profile of the entropy S near a QCP and its steepest descent in the corresponding multidimensional stress space. We demonstrate this approach for the canonical quantum critical compound CeCu6-xAux near its onset of antiferromagnetic order. We are able to link the directional stress dependence of S to the previously determined geometry of quantum critical fluctuations. Our demonstration of the multidimensional entropy landscape provides the foundation to understand how quantum criticality nucleates novel phases such as high-temperature superconductivity.

cond-mat.str-el

Interplay between unconventional superconductivity and heavy-fermion quantum criticality: CeCu$_2$Si$_2$ versus YbRh$_2$Si$_2$

In this paper the low-temperature properties of two isostructural canonical heavy-fermion compounds are contrasted with regards to the interplay between antiferromagnetic (AF) quantum criticality and superconductivity. For CeCu$_2$Si$_2$, fully-gapped d-wave superconductivity forms in the vicinity of an itinerant three-dimensional heavy-fermion spin-density-wave (SDW) quantum critical point (QCP). Inelastic neutron scattering results highlight that both quantum critical SDW fluctuations as well as Mott-type fluctuations of local magnetic moments contribute to the formation of Cooper pairs in CeCu$_2$Si$_2$. In YbRh$_2$Si$_2$, superconductivity appears to be suppressed at $T\gtrsim~10$ mK by AF order ($T_N$ = 70 mK). Ultra-low temperature measurements reveal a hybrid order between nuclear and 4f-electronic spins, which is dominated by the Yb-derived nuclear spins, to develop at $T_A$ slightly above 2 mK. The hybrid order turns out to strongly compete with the primary 4f-electronic order and to push the material towards its QCP. Apparently, this paves the way for heavy-fermion superconductivity to form at $T_c$ = 2 mK. Like the pressure - induced QCP in CeRhIn$_5$, the magnetic field - induced one in YbRh$_2$Si$_2$ is of the local Kondo-destroying variety which corresponds to a Mott-type transition at zero temperature. Therefore, these materials form the link between the large family of about fifty low-$T$ unconventional heavy - fermion superconductors and other families of unconventional superconductors with higher $T_c$s, notably the doped Mott insulators of the cuprates, organic charge-transfer salts and some of the Fe-based superconductors. Our study suggests that heavy-fermion superconductivity near an AF QCP is a robust phenomenon.

cond-mat.supr-con

Magnetic and structural quantum phase transitions in CeCu6-xAux are independent

The heavy-fermion compound CeCu$_{6-x}$Au$_x$ has become a model system for unconventional magnetic quantum criticality. For small Au concentrations $0 \leq x < 0.16$, the compound undergoes a structural transition from orthorhombic to monoclinic crystal symmetry at a temperature $T_{s}$ with $T_{s} \rightarrow 0$ for $x \approx 0.15$. Antiferromagnetic order sets in close to $x \approx 0.1$. To shed light on the interplay between quantum critical magnetic and structural fluctuations we performed neutron-scattering and thermodynamic measurements on samples with $0 \leq x\leq 0.3$. The resulting phase diagram shows that the antiferromagnetic and monoclinic phase coexist in a tiny Au concentration range between $x\approx 0.1$ and $0.15$. The application of hydrostatic and chemical pressure allows to clearly separate the transitions from each other and to explore a possible effect of the structural transition on the magnetic quantum critical behavior. Our measurements demonstrate that at low temperatures the unconventional quantum criticality exclusively arises from magnetic fluctuations and is not affected by the monoclinic distortion.

cond-mat.str-el

Time-resolved collapse and revival of the Kondo state near a quantum phase transition

One of the most successful paradigms of many-body physics is the concept of quasiparticles: excitations in strongly interacting matter behaving like weakly interacting particles in free space. Quasiparticles in metals are very robust objects. Yet, when a system's ground state undergoes a qualitative change at a quantum critical point (QCP), the quasiparticles may disintegrate and give way to an exotic quantum-fluid state of matter. The nature of this breakdown is intensely debated, because the emergent quantum fluid dominates the material properties up to high temperature and might even be related to the occurence of superconductivity in some compounds. Here we trace the dynamics of heavy-fermion quasiparticles in CeCu$_{6-x}$Au$_{x}$ and monitor their evolution towards the QCP in time-resolved experiments, supported by many-body calculations. A terahertz pulse disrupts the many-body heavy-fermion state. Under emission of a delayed, phase-coherent terahertz reflex the heavy-fermion state recovers, with a coherence time 100 times longer than typically associated with correlated metals. The quasiparticle weight collapses towards the QCP, yet its formation temperature remains constant -- phenomena believed to be mutually exclusive. Coexistence in the same experiment calls for revisions in our view on quantum criticality.

cond-mat.str-el

Unique magnetic structure of YbCo$_2$Si$_2$

We report on the results of powder and single crystal neutron diffraction to investigate the magnetic order in YbCo$_2$Si$_2$ below the Néel temperature $T_{\rm N} = 1.7~$K in detail. Two different magnetically ordered phases can clearly be distinguished. At lowest temperatures a commensurate magnetic structure with a propagation vector ${\bf k}_1 = (0.25~ 0.25~ 1)$ is found, while the intermediate phase ($T > 0.9~$K) is characterized by an incommensurate magnetic structure with ${\bf k}_2 = (0.25~ 0.086~ 1)$. The magnetic structure in YbCo$_2$Si$_2$ is in marked contrast to all other known RCo$_2$Si$_2$ compounds (R = rare earth element) likely due to some itineracy of the Yb 4f states being responsible for the magnetism.

cond-mat.str-el

Magnetic-field enhanced aniferromagnetism in non-centrosymmetric heavy-fermion superconductor CePt$_3$Si

The effect of magnetic field on the static and dynamic spin correlations in the non-centrosymmetric heavy-fermion superconductor CePt$_3$Si was investigated by neutron scattering. The application of a magnetic field B increases the antiferromagnetic (AFM) peak intensity. This increase depends strongly on the field direction: for B${\parallel}$[0 0 1] the intensity increases by a factor of 4.6 at a field of 6.6 T, which corresponds to more than a doubling of the AFM moment, while the moment increases by only 10 % for B${\parallel}$[1 0 0] at 5 T. This is in strong contrast to the inelastic response near the antiferromagnetic ordering vector, where no marked field variations are observed for B${\parallel}$[0 0 1] up to 3.8 T. The results reveal that the AFM state in CePt$_3$Si, which coexists with superconductivity, is distinctly different from other unconventional superconductors.

cond-mat.str-el

Routes to heavy-fermion superconductivity

Superconductivity in lanthanide- and actinide-based heavy-fermion metals can have different microscopic origins. Among others, Cooper pair formation based on fluctuations of the valence, of the quadrupole moment or of the spin of the localized 4f/5f shell have been proposed. Spin-fluctuation mediated superconductivity in CeCu2Si2 was demonstrated by inelastic neutron scattering to exist in the vicinity of a spin-density-wave quantum critical point. The isostructural HF compound YbRh2Si2 which is prototypical for a Kondo-breakdown quantum critical point has so far not shown any sign of superconductivity down to approximately 10mK. In contrast, results of de-Haas-van-Alphen experiments by Shishido et al. (J. Phys. Soc. Jpn. 74, 1103 (2005)) suggest superconductivity in CeRhIn5 close to an antiferromagnetic quantum critical point beyond the spin-density-wave type, at which the Kondo effect breaks down. For the related compound CeCoIn5 however, a field-induced quantum critical point of spin-density-wave type is extrapolated to exist inside the superconducting phase.

cond-mat.supr-con

Magnetically driven superconductivity in CeCu2Si2

The origin of unconventional superconductivity, including high-temperature and heavy-fermion superconductivity, is still a matter of controversy. Spin excitations instead of phonons are thought to be responsible for the formation of Cooper pairs. Using inelastic neutron scattering, we present the first in-depth study of the magnetic excitation spectrum in momentum and energy space in the superconducting and the normal states of CeCu2Si2. A clear spin excitation gap is observed in the superconducting state. We determine a lowering of the magnetic exchange energy in the superconducting state, in an amount considerably larger than the superconducting condensation energy. Our findings identify the antiferromagnetic excitations as the major driving force for superconducting pairing in this prototypical heavy-fermion compound located near an antiferromagnetic quantum critical point.

cond-mat.supr-con

Temperature dependence of low-energy phonons in magnetic nonsuperconducting TbNi2B2C

We report temperature dependence of low-energy phonons in magnetic nonsuperconducting TbNi2B2C single crystals measured by inelastic neutron scattering. We observed a low-temperature softening and broadening of two phonon branches, qualitatively similar to that previously reported for superconducting RNi2B2C (R= rare earth, Y) compounds. This result suggests that the superconductivity in TbNi2B2C compounds is absent not because of a weak electron-phonon coupling but as a result of pairbreaking due to magnetism.

cond-mat.supr-con

Magnetism and superconductivity driven by identical 4$f$ states in a heavy-fermion metal

The apparently inimical relationship between magnetism and superconductivity has come under increasing scrutiny in a wide range of material classes, where the free energy landscape conspires to bring them in close proximity to each other. This is particularly the case when these phases microscopically interpenetrate, though the manner in which this can be accomplished remains to be fully comprehended. Here, we present combined measurements of elastic neutron scattering, magnetotransport, and heat capacity on a prototypical heavy fermion system, in which antiferromagnetism and superconductivity are observed. Monitoring the response of these states to the presence of the other, as well as to external thermal and magnetic perturbations, points to the possibility that they emerge from different parts of the Fermi surface. This enables a single 4$f$ state to be both localized and itinerant, thus accounting for the coexistence of magnetism and superconductivity.

cond-mat.str-el