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HoNiSi$_{3}$ is an intermetallic compound characterized by two successive antiferromagnetic transitions at $T_{N1} = 6.3$ K and $T_{N2} = 10.4$ K. Here, its zero-field microscopic magnetic structure is inferred from resonant x-ray magnetic diffraction experiments on a single crystalline sample that complement previous bulk magnetic susceptibility data. For $T < T_{N2}$, the primitive magnetic unit cell matches the chemical cell. The magnetic structure features ferromagnetic {\it ac} planes stacked in an antiferromagnetic $\uparrow \downarrow \uparrow \downarrow$ pattern. For $T_{N1} < T < T_{N2}$, the ordered magnetic moment points along $\vec{a}$, and for $T < T_{N1}$ a component along $\vec{c}$ also orders. A symmetry analysis indicates that the magnetic structure for $T

We report the observation of an unexpected quadratic temperature dependence of the heat capacity in the vanadium sulphide metal V5S8 at low temperatures which is independent of applied magnetic field. We find that the behaviour of the heat capacity is consistent with an unconventional phonon spectrum which is linear in wavevector in the c direction but quadratic in the a-b plane, indicating a form of geometrical elastic criticality. In the case of V5S8 we also observe an unusual intermediate transition at high magnetic fields between the expected spin-flop and spin-flip transitions. We demonstrate that the intermediate field-induced transition is in agreement with a model of two sublattices with frustrated inter- and intra-sublattice spin couplings.

The authors reply to the Comment arXiv:2104.03770 by P. Canfield et. al.

The partial (up to 7 %) substitution of Cd for Zn in the Yb-based heavy-fermion material YbFe$_2$Zn$_{20}$ is known to induce a slight ($\sim 20$ %) reduction of the Sommerfeld specific heat coefficient $\gamma$ and a huge (up to two orders of magnitude) reduction of the $T^2$ resistivity coefficient $A$, corresponding to a drastic and unexpected reduction of the Kadowaki-Woods ratio $A/\gamma ^2$. Here, Yb $L_{3}$-edge X-ray absorption spectroscopy shows that the Yb valence state is close to $3+$ for all $x$, whereas X-ray diffraction reveals that Cd replace the Zn ions only at the $16c$ site of the $Fd\bar{3}m$ cubic structure, leaving the $48f$ and $96g$ sites with full Zn occupation. Ab-initio electronic structure calculations in pure and Cd-doped materials, carried out without considering correlations, show multiple conduction bands with only minor modifications of the band dispersions near the Fermi level and therefore do not explain the resistivity drop introduced by Cd substitution. We propose that the site-selective Cd substitution introduces light conduction bands with substantial contribution of Cd($16c$) $5p$ levels that have weak coupling to the Yb$^{3+}$ $4f$ moments. These light fermions coexist with heavy fermions originated from other conduction bands with larger participation of Zn($48f$ and $96g$) $4p$ levels that remain strongly coupled with the Yb$^{3+}$ local moments., Comment: 9 pages, 4 figures, to appear in Phys. Rev. B

The crystal growth and the structural, transport and magnetic properties of the magnetically frustrated YbMn$_2$Sb$_2$ single crystals are reported. The crystals show a trigonal symmetry (space group $P\bar{3}m1$), where corrugated honeycomb layers of MnSb are separated by Yb atoms. No structural phase transition was observed down to 22~K. The resistivity measurements show a predominantly insulating behavior. The combined resistivity, dc susceptibility and heat capacity measurements confirm successive transitions at 230~K, 116~K and 27~K, being the transition at $T_N$=116~K due to the Mn$^{+2}$ lattice antiferromagnetic ordering. Muon spin rotation experiments ($\mu$SR) reveal a more complicated scenario, with temperature dependence of the magnetic volume fraction reflecting short range and long range magnetic order, and a strongly disordered magnetic ground state. The role of spin-lattice coupling and its relationship with exchange interactions between Mn moments are discussed as possible cause of the complex magnetic behavior observed.

The series of intermetallic compounds $R$NiSi$_3$ ($R$ = rare earth) shows interesting magnetic properties evolving with $R$ and metamagnetic transitions under applied magnetic field for some of the compounds. The microscopic magnetic structures must be determined to rationalize such rich behavior. Here, resonant x-ray magnetic diffraction experiments are performed on single crystals of GdNiSi$_{3}$ and TbNiSi$_{3}$ at zero field. The primitive magnetic unit cell matches the chemical cell below the N\'eel temperatures $T_{N}$ = 22.2 and 33.2 K, respectively. The magnetic structure is determined to be the same for both compounds (magnetic space group $Cmmm'$). It features ferromagnetic {\it ac} planes that are stacked in an antiferromagnetic $+-+-$ pattern, with the rare-earth magnetic moments pointing along the $\vec{a}$ direction, which contrasts with the $+--+$ stacking and moment direction along the $\vec{b}$ axis previously reported for YbNiSi$_3$. This indicates a sign reversal of the coupling constant between second-neighbor $R$ planes as $R$ is varied from Gd and Tb to Yb. The long {\it b} lattice parameter of GdNiSi$_{3}$ and TbNiSi$_{3}$ shows a magnetoelastic expansion upon cooling below $T_N$, pointing to the conclusion that the $+-+-$ stacking is stabilized under lattice expansion. A competition between distinct magnetic stacking patterns with similar exchange energies tuned by the size of $R$ sets the stage for the magnetic ground state instability observed along this series.

Temperature dependent magnetization, muon spin rotation and $^{57}$Fe M\"ossbauer spectroscopy experiments performed on crystals of intermetallic FeGa$_{3-y}$Ge$_{y}$ ($y=0.11,0.14,0.17,0.22,0.27$, $0.29,0.32$) are reported. Whereas at $y=0.11$ even a sensitive magnetic microprobe such as $\mu$SR does not detect magnetism, all other samples display weak ferromagnetism with a magnetic moment of up to 0.22 $\mu_B$ per Fe atom. As a function of doping and of temperature a crossover from short range to long range magnetic order is observed, characterized by a broadly distributed spontaneous internal field. However, the $y=0.14$ and $y=0.17$ remain in the short range ordered state down to the lowest investigated temperature. The transition from short range to long range order appears to be accompanied by a change of the character of the spin fluctuations, which exhibit spin wave excitations signature in the LRO part of the phase diagram. M\"ossbauer spectroscopy for $y=0.27$ and 0.32 indicates that the internal field lies in the plane perpendicular to the crystallographic $c$ axis. The field distribution and its evolution with doping suggest that the details of the Fe magnetic moment formation and the consequent magnetic state are determined not only by the dopant concentration but also by the way the replacement of the Ga atoms surrounding the Fe is accomplished.

Experiments on the $Gd^{3+}$ Electron Spin Resonance (ESR) in the filled skutterudite $Ce_{1-x}Gd_{x}Fe_{4}P_{12}$ ($x \approx 0.001$), at temperatures where the host resistivity manifests a smooth insulator-metal crossover, provides evidence of the underlying Kondo physics associated with this system. At low temperatures (below $T \approx K$), $Ce_{1-x}Gd_{x}Fe_{4}P_{12}$ behaves as a Kondo-insulator with a relatively large hybridization gap, and the $Gd^{3+}$ ESR spectra displays a fine structure with lorentzian line shape, typical of insulating media. The electronic gap is attributed to the large hybridization present in the coherent regime of a Kondo lattice, when Ce 4f-electrons cooperate with band properties at half-filling. Mean-field calculations suggest that the electron-phonon interaction is fundamental at explaining the strong 4f-electron hybridization in this filled skutterudite. The resulting electronic structure is strongly temperature dependent, and at about $T^{*} \approx 160 K$ the system undergoes an insulator-to-metal transition induced by the withdrawal of 4f-electrons from the Fermi volume, the system becoming metallic and non-magnetic. The $Gd^{3+}$ ESR fine structure coalesces into a single dysonian resonance, as in metals. Still, our simulations suggest that exchange-narrowing via the usual Korringa mechanism, alone, is not capable of describing the thermal behavior of the ESR spectra in the entire temperature region ($4.2$ - $300$ K). We propose that temperature activated fluctuating-valence of the Ce ions is the missing ingredient that, added to the usual exchange-narrowing mechanism, fully describes this unique temperature dependence of the $Gd^{3+}$ ESR fine structure observed in $Ce_{1-x}Gd_{x}Fe_{4}P_{12}$., Comment: 19 pages, 6 figures

A detailed microscopic and quantitative description of the electronic and magnetic properties of Gd$^{3+}$-doped YCo$_{2}$Zn$_{20}$ single crystals (Y$_{1-x}$Gd$_{x}$Co$_{2}$Zn$_{20}$: (0.002 $\lesssim x \leq $ 1.00) is reported through a combination of temperature-dependent electron spin resonance (ESR), heat capacity and $dc$ magnetic susceptibility experiments, plus first-principles density functional theory (DFT) calculations. The ESR results indicate that this system features an \emph{exchange bottleneck} scenario wherein various channels for the spin-lattice relaxation mechanism of the Gd$^{3+}$ ions can be identified via exchange interactions with different types of conduction electrons at the Fermi level. Quantitative support from the other techniques allow to extract the exchange interaction parameters between the localized magnetic moments of the Gd$^{3+}$ ions and the different types of conduction electrons present at the Fermi level ($J_{fs}$, $J_{fp}$ and $J_{fd}$). Despite the complexity of the crystal structure, our combination of experimental and electronic structure data establish GdCo$_{2}$Zn$_{20}$ as a model RKKY system by predicting a Curie-Weiss temperature $\theta_{C} = -1.2(2)$~K directly from microscopic parameters, in very good agreement with the bulk value from magnetization data. The successful microscopic understanding of the electronic structure and behavior for the two end compounds YCo$_{2}$Zn$_{20}$ and GdCo$_{2}$Zn$_{20}$ means they can be used as references to help describe the more complex electronic properties of related materials., Comment: Phys. Rev. B (accepted)

FeGa$_3$ is an unusual intermetallic semiconductor that presents intriguing magnetic responses to the tuning of its electronic properties. When doped with Ge, the system evolves from diamagnetic to paramagnetic to ferromagnetic ground states that are not well understood. In this work, we have performed a joint theoretical and experimental study of FeGa$_{3-x}$Ge$_x$ using Density Functional Theory and magnetic susceptibility measurements. For low Ge concentrations we observe the formation of localized moments on some Fe atoms and, as the dopant concentration increases, a more delocalized magnetic behavior emerges. The magnetic configuration strongly depends on the dopant distribution, leading even to the appearance of antiferromagnetic interactions in certain configurations., Comment: See "Note added to arXiv version" in text

We report evidence for a close relation between the thermal activation of the rattling motion of the filler guest atoms, and inhomogeneous spin dynamics of the Eu2+ spins. The spin dynamics is probed directly by means of Eu2+ electron spin resonance (ESR), performed in both X-band (9.4 GHz) and Q-band (34 GHz) frequencies in the temperature interval 4.2 < T < 300 K. A comparative study with ESR measurements on the Beta-Eu8Ga16Ge30 clathrate compound is presented. Our results point to a correlation between the rattling motion and the spin dynamics which may be relevant for the general understanding of the dynamics of cage systems., Comment: 6 pages, 4 figures, accepted for publication in Phys. Rev. B

With a terahertz time-domain spectrometer (0.3 - 3.0 THz) we have measured the optical conductivity of the type-I clathrate Ba$_8$Ga$_{16}$Sn$_{30}$ at temperatures from 300 K down to 7 K. Independent six spectra superimposed on the Drude conductivity are identified to infrared active vibrational modes of guest Ba ions and the cages. While the spectra of five higher-frequency modes depend hardly on temperature, the lowest-lying spectrum with a peak at 0.72 THz due to the Ba(2) ion's off-centering vibration in the oversized cage changes with temperature characteristically. With lowering temperature, the spectral shape of this so-called rattling phonon continues to become so broad that the line-width amounts to be comparable to the peak frequency. Furthermore, below about 100 K, the single broad peak tends to split into two subpeaks. While this splitting can be explained by assuming a multi-well anharmonic potential, the strong enhancement of the line-width broadening toward low temperature, cannot be understood, since the Boltzmann factor generally sharpens the low-temperature spectra., Comment: 5 pages, 4 figures

Electron Spin Resonance (ESR) measurements performed on the filled skutterudite system Ce1-x$YbxFe4P12 (x< 0.003) unequivocally reveal the coexistence of two Yb3+ resonances, associated with sites of considerably different occupations and temperature behaviors. Detailed analysis of the ESR data suggests a scenario where the fraction of oversized (Fe2P3)4 cages that host Yb ions are filled with a low occupation of on-center Yb3+ sites and a highly occupied T-dependent distribution of off-center Yb3+ sites. Analysis of the 171Yb3+ (I=1/2) isotope hyperfine splittings reveal that these two sites are associated with a low (~ 1 GHz) and a high (> 15 GHz) rattling frequency, respectively. Our findings introduce Yb3+ in Th symmetry systems and uses the Yb3+ ESR as a sensitive microscopic probe to investigate the Yb3+ ions dynamics., Comment: 5 pages, 3 figures, final version publisehd in PRB

We report on the electrical resistivity, magnetic susceptibility and heat-capacity measurements on a new intermetallic compound CePd5Al2, crystallizing in the ZrNi2Al5-type tetragonal structure, with lattice parameters a = 4.156 A and c = 14.883 A. The compound presents Kondo lattice behavior and an easy-plane antiferromagnetic ground state with two magnetic transitions at 2.9 K and 3.9 K. The Sommerfeld coefficient is estimated as 60 mJ/mol K^2., Comment: 9 pages, 4 figures, submitted to J. Phys. Soc. Jpn

We present a systematic study of thermal conductivity, specific heat, electrical resistivity, thermopower and x-ray diffraction measurements performed on single-crystalline samples of the pseudoquaternary type-I clathrate system Sr8Ga16Si30-xGex, in the full range of 0 < x < 30. All the samples show metallic behavior with n-type majority carriers. However, the thermal conductivity and specific heat strongly depend on x. Upon increasing x from 0 to 30, the lattice parameter increases by 3%, from 10.446 to 10.726 A, and the localized vibrational energies of the Sr guest ions in the tetrakaidekahedron (dodecahedron) cages decrease from 59 (120) K to 35 (90) K. Furthermore, the lattice thermal conductivity at low temperatures is largely suppressed. In fact, a crystalline peak found at 15 K for x = 0 gradually decreases and disappears for x > 20, evolving into the anomalous glass-like behavior observed for x = 30. It is found that the increase of the free space for the Sr guest motion directly correlates with a continuous transition from on-center harmonic vibration to off-center anharmonic vibration, with consequent increase in the coupling strength between the guest's low-energy modes and the cage's acoustic phonon modes., Comment: 7 pages, 7 figures, submitted to PRB

The present controversy over the origin of glasslike thermal conductivity observed in certain crystalline materials is addressed by studies on single-crystal x-ray diffraction, thermal conductivity k(T) and specific heat Cp(T) of carrier-tuned Ba8Ga16X30 (X = Ge, Sn) clathrates. These crystals show radically different low-temperature k(T) behaviors depending on whether their charge carriers are electrons or holes, displaying the usual crystalline peak in the former case and an anomalous glasslike plateau in the latter. In contrast, Cp(T) above 4 K and the general structural properties are essentially insensitive to carrier tuning. We analyze these combined results within the framework of a Tunneling/Resonant/Rayleigh scatterings model, and conclude that the evolution from crystalline to glasslike k(T) is accompanied by an increase both in the effective density of tunnelling states and in the resonant scattering level, while neither one of these contributions can solely account for the observed changes in the full temperature range. This suggests that the most relevant factor which determines crystalline or glasslike behavior is the coupling strength between the guest vibrational modes and the frameworks with different charge carriers., Comment: 8 pages, 4 figures, 4 tables, submitted to Phys. Rev. B

We have grown single crystals of YbFe6Ge6 and LuFe6Ge6 and characterized their anisotropic behaviour through low field magnetic susceptibility, field-dependent magnetization, resistivity and heat capacity measurements. The Yb+3 valency is confirmed by LIII XANES measurements. YbFe6Ge6 crystals exhibit a field-dependent, sudden reorientation of the Fe spins at about 63 K, a unique effect in the RFe6Ge6 family (R = rare earths) where the Fe ions order anti-ferromagnetically with Neel temperatures above 450 K and the R ions' magnetism appears to behave independently. The possible origins of this unusual behaviour of the ordered Fe moments in this compound are discussed., Comment: 12 pages, 8 figures, accepted in J. Phys.: Cond. Matter

We have grown single crystals of the type-VIII intermetallic clathrate Ba8Ga16Sn30 from both Sn and Ga flux, evaluated their compositions through electron microprobe analysis and studied their transport properties through measurements on temperature dependent resistivity, thermopower and Hall coefficient. Crystals grown in Sn flux show n-type carriers and those from Ga flux show p-type carriers, whereas all measured compositions remain very close to the stoichiometric 8:16:30 proportion of Ba:Ga:Sn, expected from charge-balance principles. Our results indicate a very high sensitivity of the charge carrier nature and density with respect to the growth conditions, leading to relevant differences in transport properties which point to the importance of tuning this material for optimal thermoelectric performance., Comment: Revised version accepted in J. Phys.: Cond. Mat

We report the electrical resistivity, Hall coefficient, thermoelectric power, specific heat, and thermal conductivity on single crystals of the type-VIII clathrate Ba8Ga16Sn30 grown from Sn-flux. Negative S and R_H over a wide temperature range indicate that electrons dominate electrical transport properties. Both rho(T) and S(T) show typical behavior of a heavily doped semiconductor. The absolute value of S increases monotonically to 243 uV/K with increasing temperature up to 550 K. The large S may originate from the low carrier concentration n=3.7x10^19 cm^(-3). Hall mobility u_H shows a maximum of 62 cm^2/Vs around 70 K. The analysis of temperature dependence of u_H suggests a crossover of dominant scattering mechanism from ionized impurity to acoustic phonon scattering with increasing temperature. The existence of local vibration modes of Ba atoms in cages composed of Ga and Sn atoms is evidenced by analysis of experimental data of structural refinement and specific heat, which give an Einstein temperature of 50 K and a Debye temperature of 200 K. This local vibration of Ba atoms should be responsible for the low thermal conductivity (1.1 W/m K at 150 K). The potential of type-VIII clathrate compounds for thermoelectric application is discussed., Comment: 6 pages, 6 figures, submitted to Phys. Rev. B

We report on the structural, thermodynamic and transport properties of high-quality single crystals of YbNiSi3 grown by the flux method. This compound crystallizes in the SmNiGe3 layered structure type of the Cmmm space group. The general physical behavior is that of a Kondo lattice showing an antiferromagnetic ground state below T_N = 5.1 K. This is among the highest ordering temperatures for a Yb-based intermetallic, indicating strong exchange interaction between the Yb ions, which are close to +3 valency based on the effective moment of 4.45 mu_B/f.u. The compound has moderately heavy-electron behavior with Sommerfeld coefficient 190 mJ/mol K^2. Resistivity is highly anisotropic and exhibits the signature logarithmic increase below a local minimum, followed by a sharp decrease in the coherent/magnetically ordered state, resulting in residual resistivity of 1.5 micro Ohm cm and RRR = 40. Fermi-liquid behavior consistent with a ground-state doublet is clearly observed below 1 K., Comment: 4 pages, 4 figures, submitted to PRB

We address the nature of the ligandal disorder leading to local redistributions of Kondo temperatures, manifested as annealing-induced changes in the transport behavior of the heavy fermion system YbNi2B2C. The anomalous transport behavior was fully characterized by temperature dependent resistivity measurements in an extended range of 0.4 < T < 1000 K for as-grown and optimally annealed single crystals, and microstructural changes between these two types of samples were investigated by single-crystal x-ray diffraction and transmission electron microscopy. Our results point to lattice dislocations as the most likely candidate to be affecting the surrounding Yb ions, leading to a distribution of Kondo temperatures. This effect combined with the ability to control defect density with annealing offers the possibility of further understanding of the more general problem of the enhanced sensitivity of hybridized Kondo states to disorder, particularly above the coherence temperature., Comment: 7 pages, 5 figures, submitted to Phys. Rev. B

We have grown RFe2Ge2 single crystals for R = Y and ten members of the lanthanide series (Pr, Nd, Sm, Gd-Tm, Lu) using Sn flux as the solvent. The method yields clean, high quality crystal plates as evidenced by residual resistivities and RRR values in the range of 3-12 uOhm cm and 20-90 respectively. The crystals are also virtually free of magnetic impurities or secondary phases, allowing the study of the intrinsic anisotropic magnetic behavior of each compound. Characterization was made with X-Ray diffraction, and temperature and field dependent magnetization, specific heat and resistivity. Very strong anisotropies arising mostly from CEF effects were observed for all magnetic rare earths except Gd. Antiferromagnetic ordering occurred at temperatures between 16.5 K (Nd) and 1.1 K (Ho) that roughly scale with the de Gennes factor for the heavy rare earths. For some members there is also a lower temperature transition associated with changes in the magnetic structure. Tm did not order down to 0.4 K, and appears to be a van Vleck paramagnet. All members which ordered above 2 K showed a metamagnetic transition at 2 K for fields below 70 kOe. The calculated effective moments per rare earth atom are close to the expected free ion values of R^3+ except for Sm which displays anomalous behavior in the paramagnetic state. The non-magnetic members of this series (Y, Lu) are characterized by an unusually large electronic specific heat coefficient (gamma ~ 60 mJ/mol K^2) and temperature-independent susceptibility term (chi_0 ~ 0.003 emu/mol), indicative of a relatively large density of states at the Fermi surface., Comment: 34 pages, 13 figures, 1 table, submitted to J. Magn. Magn. Mater

We report temperature and field dependent measurements of the magnetic susceptibility, specific heat and resistivity of sintered YbB2 pellets, prepared via two distinct reaction routes, utilizing different temperatures, pressures and sintering times. Sample behavior is affected by the preparation procedure, as a consequence of different secondary phases, most of which were identified via x-ray diffraction. These experiments show that YbB2 is a metal with the Yb atoms in or very close to their 3+ state. YbB2 appears to order anti-ferromagnetically at TN ~ 5.6 K, which can be considered a relatively high ordering temperature for an ytterbium-based intermetallic compound., Comment: 16 pages, 8 figures, submitted to J. Alloys Compnds

We report temperature dependent resistivity, specific heat, magnetic susceptibility and thermoelectric power measurements made on the heavy fermion system YbNi2B2C, for both as grown and annealed single crystals. Our results demonstrate a significant variation in the temperature dependent electrical resistivity and thermoelectric power between as grown crystals and crystals that have undergone optimal (150 hour, 950 C) annealing, whereas the thermodynamic properties: (c_p(T) and chi(T)) remain almost unchanged. We interpret these results in terms of redistributions of local Kondo temperatures associated with ligandal disorder for a small (~ 1%) fraction of the Yb sites., Comment: 5 pages, 4 figures, submitted to PRB