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For the last few decades, researchers have been intrigued by multipolar ordering phenomena while looking for the related quantum criticality in the heavy-fermion Kondo system Ce$_{1-x}$La$_{x}$B$_6$. However, critical phenomena induced by substitution level ($x$), temperature ($T$), and magnetic field ($B$) are poorly understood despite a large collection of experimental results is available. In this work, we present $T$-$B$, $x$-$T$, and $x$-$B$ phase diagrams of Ce$_{1-x}$La$_x$B$_6$ ($\mathbf{B}\parallel[110]$). These are completed by analyzing heat capacity, magnetocaloric effect (MCE), and elastic neutron scattering. A drastic increase of the Sommerfeld coefficient $\gamma_0$, which is estimated from the heat capacity down to 0.05 K, is observed with increasing $x$. The precise $T$-$B$ phase diagram which includes an unforeseen high-entropy region is drawn by analyzing the MCE for the first time in Ce$_{1-x}$La$_x$B$_6$. The $x$-$B$ phase diagram, which supports the existence of a QCP at $x>0.75$, is obtained by the same analysis. A detailed interpretation of phase diagrams strongly indicates positive correlation between the fluctuating multipoles and the effective electron mass., Comment: 11 pages, 8 figures

In zero magnetic field, the famous neutron spin resonance in the f-electron superconductor CeCoIn5 is similar to the recently discovered exciton peak in the non-superconducting CeB6. Magnetic field splits the resonance in CeCoIn5 into two components, indicating that it is a doublet. Here we employ inelastic neutron scattering (INS) to scrutinize the field dependence of spin fluctuations in CeB6. The exciton shows a markedly different behavior without any field splitting. Instead, we observe a second field-induced magnon whose energy increases with field. At the ferromagnetic zone center, however, we find only a single mode with a non-monotonic field dependence. At low fields, it is initially suppressed to zero together with the antiferromagnetic order parameter, but then reappears at higher fields inside the hidden-order phase, following the energy of an electron spin resonance (ESR). This is a unique example of a ferromagnetic resonance in a heavy-fermion metal seen by both ESR and INS consistently over a broad range of magnetic fields., Comment: 7 pages, 6 figures including one animation, accepted to Phys. Rev. B

Cerium hexaboride is a cubic f-electron heavy-fermion compound that displays a rich array of low-temperature magnetic ordering phenomena which have been the subject of investigation for more than 50 years. Its complex behaviour is the result of competing interactions, with both itinerant and local electrons playing important roles. Investigating this material has proven to be a substantial challenge, in particular because of the appearance of a "magnetically hidden order" phase, which remained elusive to neutron-scattering investigations for many years. It was not until the development of modern x-ray scattering techniques that the long suspected multipolar origin of this phase was confirmed. Doping with non-magnetic lanthanum dilutes the magnetic cerium sublattice and reduces the f-electron count, bringing about substantial changes to the ground state with the emergence of new phases and quantum critical phenomena. To this day, Ce(1-x)La(x)B6 and its related compounds remain a subject of intense interest. Despite the substantial progress in understanding their behaviour, they continue to reveal new and unexplained physical phenomena. Here we present a review of the accumulated body of knowledge on this family of materials in order to provide a firm standpoint for future investigations., Comment: Review article: 43 pages, 17 figures, 178 references

CeB(6) is a model compound exhibiting antiferroquadrupolar (AFQ) order, its magnetic properties being typically interpreted within localized models. More recently, the observation of strong and sharp magnetic exciton modes forming in its antiferromagnetic (AFM) state at both ferromagnetic and AFQ wave vectors suggested a significant contribution of itinerant electrons to the spin dynamics. Here we investigate the evolution of the AFQ excitation upon the application of an external magnetic field and the substitution of Ce with non-magnetic La, both parameters known to suppress the AFM phase. We find that the exciton energy decreases proportionally to T_N upon doping. In field, its intensity is suppressed, while its energy remains constant. Its disappearance above the critical field of the AFM phase is preceded by the formation of two modes, whose energies grow linearly with magnetic field upon entering the AFQ phase. These findings suggest a crossover from itinerant to localized spin dynamics between the two phases, the coupling to heavy-fermion quasiparticles being crucial for a comprehensive description of the magnon spectrum., Comment: Extended version with a longer introduction and an additional figure. 6 pages and 5 figures

Using inelastic neutron scattering, we have observed a quasi-one-dimensional dispersive magnetic excitation in the frustrated triangular-lattice spin-2 chain oxide Ca3Co2O6. At the lowest temperature (T = 1.5 K), this magnon is characterized by a large zone-center spin gap of ~27 meV, which we attribute to the large single-ion anisotropy, and disperses along the chain direction with a bandwidth of ~3.5 meV. In the directions orthogonal to the chains, no measurable dispersion was found. With increasing temperature, the magnon dispersion shifts towards lower energies, yet persists up to at least 150 K, indicating that the ferromagnetic intrachain correlations survive up to 6 times higher temperatures than the long-range interchain antiferromagnetic order. The magnon dispersion can be well described within the predictions of linear spin-wave theory for a system of weakly coupled ferromagnetic chains with large single-ion anisotropy, enabling the direct quantitative determination of the magnetic exchange and anisotropy parameters., Comment: 7 pages, 6 figures including one animation

Heavy-fermion metals exhibit a plethora of low-temperature ordering phenomena, among them the so-called hidden-order phases that in contrast to conventional magnetic order are invisible to standard neutron diffraction. One of the oldest and structurally simplest hidden-order compounds, CeB6, became famous for an elusive phase that was attributed to the antiferroquadrupolar ordering of cerium-4f moments. In its ground state, CeB6 also develops a more usual antiferromagnetic (AFM) order. Hence, its essential low-temperature physics was always considered to be solely governed by AFM interactions between the dipolar and multipolar Ce moments. Here we overturn this established perspective by uncovering an intense ferromagnetic (FM) low-energy collective mode that dominates the magnetic excitation spectrum of CeB6. Our inelastic neutron-scattering data reveal that the intensity of this FM excitation by far exceeds that of conventional spin-wave magnons emanating from the AFM wave vectors, thus placing CeB6 much closer to a FM instability than could be anticipated. This propensity of CeB6 to ferromagnetism may account for much of its unexplained behavior, such as the existence of a pronounced electron spin resonance, and should lead to a substantial revision of existing theories that have so far largely neglected the role of FM interactions., Comment: 7 pages including supplemental material

We investigate magnetic ordering in metallic Ba[Fe(1-x)Mn(x)](2)As(2) and discuss the unusual magnetic phase, which was recently discovered for Mn concentrations x > 10%. We argue that it can be understood as a Griffiths-type phase that forms above the quantum critical point associated with the suppression of the stripe-antiferromagnetic spin-density-wave (SDW) order in BaFe2As2 by the randomly introduced localized Mn moments acting as strong magnetic impurities. While the SDW transition at x = 0, 2.5% and 5% remains equally sharp, in the x = 12% sample we observe an abrupt smearing of the antiferromagnetic transition in temperature and a considerable suppression of the spin gap in the magnetic excitation spectrum. According to our muon-spin-relaxation, nuclear magnetic resonance and neutron-scattering data, antiferromagnetically ordered rare regions start forming in the x = 12% sample significantly above the N\'eel temperature of the parent compound. Upon cooling, their volume grows continuously, leading to an increase in the magnetic Bragg intensity and to the gradual opening of a partial spin gap in the magnetic excitation spectrum. Using neutron Larmor diffraction, we also demonstrate that the magnetically ordered volume is characterized by a finite orthorhombic distortion, which could not be resolved in previous diffraction studies most probably due to its coexistence with the tetragonal phase and a microstrain-induced broadening of the Bragg reflections. We argue that Ba[Fe(1-x)Mn(x)](2)As(2) could represent an interesting model spin-glass system, in which localized magnetic moments are randomly embedded into a SDW metal with Fermi surface nesting., Comment: 15 pages, 13 figures

Spin excitations stemming from the metallic phase of the ferrochalcogenide superconductor K(0.77)Fe(1.85)Se(2) (T_c=32 K) were mapped out in the ab plane by means of the time-of-flight neutron spectroscopy. We observed a magnetic resonant mode at Q_res=(1/2 1/4), whose energy and in-plane shape are almost identical to those in the related compound Rb(0.8)Fe(1.6)Se(2). This lets us infer that there is a unique underlying electronic structure of the bulk superconducting phase K(x)Fe(2)Se(2), which is universal for all alkali-metal iron selenide superconductors and stands in contrast to the doping-tunable phase diagrams of the related iron pnictides. Furthermore, the spectral weight of the resonance on the absolute scale, normalized to the volume fraction of the superconducting phase, is several times larger than in optimally doped BaFe(2-x)Co(x)As(2). We also found no evidence for any additional low-energy branches of spin excitations away from Q_res. Our results provide new input for theoretical models of the spin dynamics in iron based superconductors.

75As nuclear magnetic resonance (NMR) experiments were performed on Ba(Fe1-xMnx)2As2 (xMn = 2.5%, 5% and 12%) single crystals. The Fe layer magnetic susceptibility far from Mn atoms is probed by the75As NMR line shift and is found similar to that of BaFe2As2, implying that Mn does not induce charge doping. A satellite line associated with the Mn nearest neighbours (n.n.) of 75As displays a Curie-Weiss shift which demonstrates that Mn carries a local magnetic moment. This is confirmed by the main line broadening typical of a RKKY-like Mn-induced staggered spin polarization. The Mn moment is due to the localization of the additional Mn hole. These findings explain why Mn does not induce superconductivity in the pnictides contrary to other dopants such as Co, Ni, Ru or K., Comment: 6 pages, 7 figures

We report results of inelastic-neutron-scattering measurements of low-energy spin-wave excitations in two structurally distinct families of iron-pnictide parent compounds: Na(1-{\delta})FeAs and BaFe2As2. Despite their very different values of the ordered magnetic moment and N\'eel temperatures, T_N, in the antiferromagnetic state both compounds exhibit similar spin gaps of the order of 10 meV at the magnetic Brillouin-zone center. The gap opens sharply below T_N, with no signatures of a precursor gap at temperatures between the orthorhombic and magnetic phase transitions in Na(1-{\delta})FeAs. We also find a relatively weak dispersion of the spin-wave gap in BaFe2As2 along the out-of-plane momentum component, q_z. At the magnetic zone boundary (q_z = 0), spin excitations in the ordered state persist down to 20 meV, which implies a much smaller value of the effective out-of-plane exchange interaction, J_c, as compared to previous estimates based on fitting the high-energy spin-wave dispersion to a Heisenberg-type model., Comment: 5 pages, 4 figures, 1 table

77Se and 87Rb nuclear magnetic resonance (NMR) experiments on Rb0.74Fe1.6Se2 reveal clearly distinct spectra originating from a majority antiferromagnetic (AF) and a minority metallic-superconducting (SC) phase. The very narrow NMR line of the SC phase evidences the absence of Fe vacancies and any trace of AF order. The Rb content of the SC phase is deduced from intensity measurements identifying Rb0.3(1)Fe2Se2 as the actual composition of the SC fraction. The resulting estimate of 0:15 electrons/Fe brings this class of superconductors 245 family closer to the other Fe-based superconductor families., Comment: To be published in Phys.Rev.Lett. (editor's suggestion). 5 pages, 4 figures

Single crystals of superconducting KxFe2-ySe2 have been grown with the optical floating-zone technique under application of 8 bar of argon pressure. We found that large and high quality single crystals with dimensions of ~\varnothing6 \times 10 mm could be obtained at the termination of the grown ingot through quenching, while the remaining part of the ingot decomposed. As-grown single crystals commonly represent an intergrowth of two sets of the c-axis characterized by slightly different lattice constants. Single crystal of K0.80Fe1.81Se2 shows a superconducting transition at Tc = 31.6 K, leading to a near 100% expulsion of the external magnetic field in magnetization measurements. On the other hand, neutron-diffraction data indicate that superconductivity in the sample coexists with a iron-vacancy superstructure and static antiferromagnetic order. The anisotropic ratio of the upper critical field Hc2 for both H//c and H//ab configurations is \sim3.46.

Inelastic neutron scattering is employed to study the reciprocal-space structure and dispersion of magnetic excitations in the normal and superconducting states of single-crystalline Rb0.8Fe1.6Se2. We show that the recently discovered magnetic resonant mode in this compound has a quasi-two-dimensional character, similar to overdoped iron-pnictide superconductors. Moreover, it has a rich in-plane structure that is dominated by four elliptical peaks, symmetrically surrounding the Brillouin zone corner, without sqrt(5) x sqrt(5) reconstruction. We also present evidence for the dispersion of the resonance peak, as its position in momentum space depends on energy. Comparison of our findings with the results of band structure calculations provides strong support for the itinerant origin of the observed signal. It can be traced back to the nesting of electron-like Fermi pockets in the doped metallic phase of the sample in the absence of iron-vacancy ordering.

Resonant magnetic excitations are widely recognized as hallmarks of unconventional superconductivity in copper oxides, iron pnictides, and heavy-fermion compounds. Numerous model calculations have related these modes to the microscopic properties of the pair wave function, but the mechanisms underlying their formation are still debated. Here we report the discovery of a similar resonant mode in the non-superconducting, antiferromagnetically ordered heavy-fermion metal CeB6. Unlike conventional magnons, the mode is non-dispersive, and its intensity is sharply concentrated around a wave vector separate from those characterizing the antiferromagnetic order. The magnetic intensity distribution rather suggests that the mode is associated with a coexisting order parameter of the unusual antiferro-quadrupolar phase of CeB6, which has long remained "hidden" to the neutron-scattering probes. The mode energy increases continuously below the onset temperature for antiferromagnetism, in parallel to the opening of a nearly isotropic spin gap throughout the Brillouin zone. These attributes bear strong similarity to those of the resonant modes observed in unconventional superconductors below their critical temperatures. This unexpected commonality between the two disparate ground states indicates the dominance of itinerant spin dynamics in the ordered low-temperature phases of CeB6 and throws new light on the interplay between antiferromagnetism, superconductivity, and "hidden" order parameters in correlated-electron materials.

We have studied the low-energy spin-excitation spectrum of the single-crystalline Rb2Fe4Se5 superconductor (Tc = 32 K) by means of inelastic neutron scattering. In the superconducting state, we observe a magnetic resonant mode centered at an energy of 14 meV and at the (0.5 0.25 0.5) wave vector (unfolded Fe-sublattice notation), which differs from the ones characterizing magnetic resonant modes in other iron-based superconductors. Our finding suggests that the 245-iron-selenides are unconventional superconductors with a sign-changing order parameter, in which bulk superconductivity coexists with the sqrt(5) x sqrt(5) magnetic superstructure. The estimated ratios of the resonance energy to Tc and the superconducting gap indicate moderate pairing strength in this compound, similar to that in optimally doped 1111- and 122-pnictides., Comment: To be published in Phys. Rev. Lett. Figures and references have been updated in v2

Platelet-like single crystals of the Ca(Fe1-xCox)2As2 series having lateral dimensions up to 15 mm and thickness up to 0.5 mm were obtained from the high temperature solution growth technique using Sn flux. Upon Co doping, the c-axis of the tetragonal unit cell decreases, while the a-axis shows a less significant variation. Pristine CaFe2As2 shows a combined spin-density-wave and structural transition near T = 166 K which gradually shifts to lower temperatures and splits with increasing Co-doping. Both transitions terminate abruptly at a critical Co-concentration of xc = 0.075. For x \geq 0.05, superconductivity appears at low temperatures with a maximum transition temperature TC of around 20 K. The superconducting volume fraction increases with Co concentration up to x = 0.09 followed by a gradual decrease with further increase of the doping level. The electronic phase diagram of Ca(Fe1-xCox)2As2 (0 \leq x \leq 0.2) series is constructed from the magnetization and electric resistivity data. We show that the low-temperature superconducting properties of Co-doped CaFe2As2 differ considerably from those of BaFe2As2 reported previously. These differences seem to be related to the extreme pressure sensitivity of CaFe2As2 relative to its Ba counterpart., Comment: 27 pages, 13 figures, article