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J. G. Sereni

Publications and source records attributed to J. G. Sereni.

At least 19 recordsLinked to original sources

Specific heat of Gd$^{3+}$ and Eu$^{2+}$-based magnetic compounds

We have studied theoretically the specific heat of a large number of non-frustrated magnetic structures described by the Heisenberg model for systems with total angular momentum $J=7/2$, corresponding to the 4f$^7$ configuration of Gd$^{+3}$ and Eu$^{+2}$. For a given critical temperature (determined by the magnitude of the exchange interactions), we find that, to a high degree of accuracy, the specific heat is governed by two primary parameters: the effective number of neighbors $z$, which dictates the extent of spatial and quantum fluctuations, and the axial anisotropy $K$. The universality of $z$ (its ability to describe specific heat across diverse lattices) holds robustly for systems where exchange interactions do not strongly increase with distance and in the absence of frustration. Otherwise, deviations from universality emerge. Using these two parameters we fit the specific heat of four Gd compounds and two Eu compounds, achieving a remarkable agreement. The present approach enables the extraction of magnetic interaction parameters not accessible through mean-field theory, offering a powerful tool for interpreting specific heat data in 4f$^7$ systems.

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I. Magnetic, thermal and transport properties of YbCu$_{5-x}$Zn$_x$ alloys

Within the family of cubic YbCu$_4$X compounds ($X$ = Ni, Au and Zn), we have investigated the YbCu$_{5-x}$Zn$_x$ ($1\geq x \geq 0.7$) alloys by means of structural, magnetic, thermal and transport measurements. In the $τ1-$ YbCu$_{5-x}$Zn$_x$ (cubic AuBe$_5$ type, $0.7 \leq x \leq 1.5$) structural phase, Yb ion is in its Yb$^{3+}$ magnetic configuration. However, by increasing Zn content the unit cell grows faster than a reference computed as a Cu by Zn atoms substitution, which indicates a shift of Yb ions towards the larger Yb$^{2+}$ configuration. The magnetic behavior confirms such tendency with a clear decrease of the saturation magnetization and effective moment between $x=0.7$ and $x=1$. The specific heat at low temperature shows a logarithmic dependence characteristic for a non-fermi-liquid behavior. The characteristic energies of all studied parameters, including magneto resistivity, show notably low values as an indication that these alloys are close to a quantum critical point, which is approached from the non-magnetic side as the Zn content decreases.

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Hyperfine electro-nuclear coupling at the quantum criticality of YbCu4Zn

An increasing number of Yb-based compounds fulfill the conditions for the investigation of hyperfine electro-nuclear coupling effects related to 171-Yb and 173-Yb isotopes. Among them, the lack of magnetic order down to the milikelvin range in compounds with robust localized electronic moments and their nuclear magnetism. Although reminiscences of short range magnetic interactions may be observed below 1K, such perturbation can be dodged investigating compounds located close to a quantum critical point (QCP), where quantum fluctuations prevent the development of magnetic correlations to develop. Within the family of cubic YbCu4M compounds (M = Ni, Au and Zn), we have investigated YbCu4Zn that shows a logarithmic temperature dependence: C_P /T ~ ln(T/TQ) in its electronic specific heat, as predicted for a QCP. Simultaneously, no signs of RKKY interactions are detected down to 0.03K. Due to the low Kondo temperature of its doublet ground state, the localized 4f electrons weakly couple with conduction electrons, allowing the coupling between nuclear and 4f electron moments to become relevant. However, the reminder Kondo interaction acts on the electronic hyperfine field producing a small deviation from the standard nuclear C_N ~ 1/T^2 dependence into a n < 2 power law. The expected n = 2 dependence is progressively recovered under applied magnetic field.

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Electronuclear Quantum Criticality

We present here a rare example of electronuclear quantum criticality in a metal. The compound YbCu4.6Au0.4 is located at an unconventional quantum critical point (QCP). In this material the relevant Kondo and RKKY exchange interactions are very weak, of the order of 1 K. Furthermore, there is strong competition between antiferromagnetic and ferromagnetic correlations, possibly due to geometrical frustration within the fcc Yb sublattice. This causes strong spin fluctuations which prevent the system to order magnetically. Because of the very low Kondo temperature the Yb3+ 4f-electrons couple weakly with the conduction electrons allowing the coupling to the nuclear moments of the 171Yb and 173Yb isotopes to become important. Thus, the quantum critical fluctuations observed at the QCP do not originate from purely electronic states but from entangled electronuclear states. This is evidenced by the anomalous temperature and field dependence of the specific heat at low temperatures.

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Evidences for magnetic dimers and skyrmion lattice formation in Eu$_2$Pd$_2$Sn

Magnetic, thermal and transport properties of the non-centrosymmetric compound Eu$_2$Pd$_2$Sn are revisited after including new measurements. In its paramagnetic phase, the outstanding feature of this compound is the formation of Eu$^{2+}$ dimers that allows to understand the deviation of the magnetic susceptibility $χ(T)$ from the C-W law below about 70\,K, the field dependent magnetization $M(B)$ variation below $\approx 80$\,K and the reduced entropy at the ordering temperature $S(T_N)= 0.64R\ln(8)$. A significant change of the exchange interactions occurs between $T\approx 70$\,K (where $θ_P = 18$\,K) and $T_N = 13.3$\,K (where $θ_P =-4.5$\,K). The strong electronic overlap, arising from the reduced Eu-Eu spacing compared with that of pure Eu$^{2+}$ is expected to power these quasiparticles formation, inducing a significant reformulation of the magnetic structure. A rich magnetic phase diagram is obtained from the analysis of the derivatives of the magnetic parameters: $\partial χ/\partial T$ and $\partial M/\partial B$, and the field dependence of the specific heat. Two critical points are recognized and a tentative description of the magnetic structures is proposed. The possible formation of a skyrmion lattice, that arises from the presence of magnetically frustrated pockets in the phase diagram, is suggested by theoretical studies on hexagonal structures exhibiting similar interactions pattern.

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Physical properties of CeIrSi with trillium-lattice frustrated magnetism

Magnetic ($χ$), transport ($ρ$) and heat capacity ($C_m$)properties of CeIrSi are investigated to elucidate the effect of geometric frustration in this compound with trillium type structure because, notwithstanding its robust effective moment, $μ_{\rm eff}\approx 2.46μ_B$, this Ce-lattice compound does not undergo a magnetic transition. In spite of that it shows broad $C_m(T)/T$ and $χ(T)$ maxima centered at $T_{max}\approx 1.5$\,K, while a $ρ\propto T^2$ thermal dependence, characteristic of electronic spin coherent fluctuations, is observed below $T_{coh} \approx 2.5$\,K. Magnetic field does not affect significantly the position of the mentioned maxima up to $\approx 1$\,T, though $χ(T)$ shows an incipient structure that completely vanishes at $μ_0 H \approx 1$\,T. Concerning the $ρ\propto T^2$ dependence, it is practically not affected by magnetic field up to $μ_0 H = 9$\,T, with the residual resistivity $ρ_0(H)$ slightly decreasing and $T_{coh}(H)$ increasing. These results are compared with the physical properties observed in other frustrated intermetallic compounds

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Strong magnetoelastic effect in CeCo$_{1-x}$Fe$_{x}$Si as Néel order is suppressed

A very strong magnetoelastic effect in the CeCo$_{1-x}$Fe$_{x}$Si alloys is reported. The strength of the magnetostrictive effect can be tuned upon changing $x$. The moderate low-temperature linear magnetostriction observed at low Fe concentrations becomes very large ($\frac {ΔL}{L} \left(16 T,2 K\right) =$ 3$\times$10$^{-3}$) around the critical concentration ($x_c \approx$ 0.23) at which the long-range antiferromagnetic order vanishes. Upon increasing doping through the non-magnetic region ($x > x_c$), the magnetostriction strength gradually weakens again. Remarkably the low-temperature magnetostriction at the critical concentration shows a pronounced $S$-like shape (centered at $B_m \sim$ 6 T) resembling other well-known Ce-based metamagnetic systems like CeRu$_2$Si$_2$ and CeTiGe. Unlike what is observed in these compounds, however, the field dependence of the magnetization shows only a minor upturn around $B_m$ vaguely resembling a metamagnetic behavior. The subtle interplay between magnetic order and the Kondo screening seems to originate an enhanced valence susceptibility slightly changing the Ce ions valence, ultimately triggering the large magnetostriction observed around the critical concentration.

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Suppression of Shastry-Sutherland phase driven by electronic concentration reduction in magnetically frustrated Ce$_2$Pd$_2$Sn$_{1-y}$In$_y$ alloys

Shastry-Sutherland lattice was observed as alternative ground state in Rare Earth intermetallic with Mo$_2$B$_2$Fe and U$_2$Pt$_2$Sn anisotropic structures where magnetic frustration is favored. In the case of Ce$_2$Pd$_2$Sn, it was shown that such phase can be suppressed by the application of magnetic field and, in this work, its stability is studied as a function of the electronic concentration by doping the Sn(4+) lattice with In(3+) atoms. Magnetic and specific heat measurements show that around 50\% substitution the Shastry Sutherland lattice vanishes in a critical point. This result confirms the strong dependence of that phase on the electron density because a recent investigation on the Pd rich solid solution Ce$_{2+ε}$Pd$_{2-ε}$In$_{1-x}$Sn$_x$ (with $ε< 0$) demonstrates that atomic disorder dominates the phase diagram at intermediate Sn/In concentration inhibiting magnetic frustration effects. In the alloys investigated in this work, the $ε>0$ character stabilizes the ferromagnetic ground state all along the concentration, allowing the Shastry Sutherland lattice formation on the Sn rich side.

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YbPd$_2$In: a promising candidate to strong entropy accumulation at very low temperature

We report on synthesis, crystal structure, magnetic, thermodynamic and transport properties of the new compound YbPd$_2$In, crystallizing as a Heusler structure type. A trivalent state of the rare earth was determined by fitting the magnetic susceptibility with a Curie-Weiss law. This compound is characterized by showing very weak magnetic interactions and a negligible Kondo effect. A specific heat jump was observed at $T\approx 250$ mK, followed at higher temperature by a power law decrease of $C_P(T)/T$. The resulting large electronic entropy increase at very low temperature is rapidly shifted to higher temperature by the application of magnetic field. This magnetocaloric effect places YbPd$_2$In as a very good candidate for adiabatic demagnetization cooling processes.

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Suppression of ferromagnetic order by Ag-doping: A neutron scattering investigation on Ce2(Pd1-xAgx)2In (x = 0.20, 0.50)

The ground state magnetic behaviour of Ce2(Pd0.8Ag0.2)2In and Ce2(Pd0.5Ag0.5)2In, found in the ferromagnetic branch of Ce2Pd2In, has been investigated by neutron powder diffraction at low temperature. Ce2(Pd0.8Ag0.2)2In is characterized by a ferromagnetic structure with the Ce moments aligned along the c-axis and values of 0.96(2) mB. The compound retains the P4/mbm throughout the magnetic transition, although the magnetic ordering is accompanied by a significant decrease of the lattice strain along [00l], suggesting a magnetostructural contribution. The magnetic behaviour of Ce2(Pd0.5Ag0.5)2In is very different; this compound exhibits an extremely reduced magnetic scattering contribution in the diffraction pattern, that can be ascribed to a different kind of ferromagnetic ordering, with extremely reduced magnetic moments (~ 0.1 mB) aligned along [0l0]. These results point to a competition between different types of magnetic correlations induced by Ag-substitution, giving rise to a magnetically frustrated scenario in Ce2(Pd0.5Ag0.5)2In.

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Physical properties of the very heavy fermion YbCu4Ni

The physical properties of the very heavy fermion YbCu$_4$Ni were characterized through structural, magnetic, thermal and transport studies along nearly four decades of temperature ranging between 50 milikelvin and 300 K. At high temperature, the crystal electric field levels splitting was determined with $Δ_1 (Γ_6)= 85$ K and $Δ_2 (Γ_8) \approx 200$ K, the latter being a quartet in this cubic symmetry. An effective magnetic moment $μ_{eff} \approx 3μ_B$ is evaluated for the $Γ_7$ ground state, while at high temperature the value for a Yb$^{3+}$ ion is observed. At low temperature this compounds shows the typical behavior of a magnetically frustrated system undergoing a change of regime at a characteristic temperature $T^*\approx 200$ mK into a sort of Fermi-liquid type 'plateau'of the specific heat: $C_m/T|_{T\to 0}$ = const. The change in the temperature dependence of the specific heat coincides with a maximum and a discontinuity in respective inductive and dissipative components of the ac-susceptibility. More details from the nature of this ground state are revealed by the specific heat behavior under applied magnetic field.

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Remarkable magnetostructural coupling around the magnetic transition in CeCo$_{0.85}$Fe$_{0.15}$Si

We report a detailed study of the magnetic properties of CeCo$_{0.85}$Fe$_{0.15}$Si under high magnetic fields (up to 16 Tesla) measuring different physical properties such as specific heat, magnetization, electrical resistivity, thermal expansion and magnetostriction. CeCo$_{0.85}$Fe$_{0.15}$Si becomes antiferromagnetic at $T_N \approx$ 6.7 K. However, a broad tail (onset at $T_X \approx$ 13 K) in the specific heat precedes that second order transition. This tail is also observed in the temperature derivative of the resistivity. However, it is particularly noticeable in the thermal expansion coefficient where it takes the form of a large bump centered at $T_X$. A high magnetic field practically washes out that tail in the resistivity. But surprisingly, the bump in the thermal expansion becomes a well pronounced peak fully split from the magnetic transition at $T_N$. Concurrently, the magnetoresistance also switches from negative to positive just below $T_X$. The magnetostriction is considerable and irreversible at low temperature ($\frac {ΔL}{L} \left(16 T\right) \sim$ 4$\times$10$^{-4}$ at 2 K) when the magnetic interactions dominate. A broad jump in the field dependence of the magnetostriction observed at low $T$ may be the signature of a weak ongoing metamagnetic transition. Taking altogether, the results indicate the importance of the lattice effects in the development of the magnetic order in these alloys.

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Emerging frustration effects in ferromagnetic Ce_2[Pd_{1-x}Ag_x]_2In alloys

Magnetic and thermal properties of Ferromagnetic (FM) Ce_{2.15}(Pd_{1-x}Ag_x)_{1.95}In_{0.9} alloys were studied in order to determine the Quantum Critical Point (QCP) at T_C => 0. The increase of band electrons produced by Pd/Ag substitution depresses T_C(x) from 4.1K down to T_C(x=0.5)=1.1K, with a QCP extrapolated to x_{QCP}~ 0.6. Magnetic susceptibility from T>30K indicates an effective moment slightly decreasing from μ_{eff}=2.56μ_B to 2.4μ_B at x=0.5. These values and the paramagnetic temperature θ_P~ -10K exclude significant Kondo screening effects. The T_C(x) reduction is accompanied by a weakening of the FM magnetization and the emergence of a specific heat C_m(T) anomaly at T*~ 1K, without signs of magnetism detected from AC-susceptibility. The magnetic entropy collected around 4K (i.e. the T_C of the x=0 sample) practically does not change with Ag concentration: S_m(4K)~ 0.8 Rln2, suggesting a progressive transfer of FM degrees of freedom to the non-magnetic (NM) component. No antecedent was found concerning any NM anomaly emerging from a FM system at such temperature. The origin of this anomaly is attributed to an 'entropy bottleneck' originated in the nearly divergent power law dependence for T>T*.

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Local character of the highest antiferromagnetic Ce-system CeTi{1-x}Sc{x} Ge

The highest antiferromagnetic (AFM) temperature in Ce based compounds has been reported for CeScGe with Tn=47K, but its local or itinerant nature was not deeply investigated yet. In order to shed more light into this unusually high ordering temperature we have investigated structural, magnetic, transport and thermal properties of CeTi{1-x}Sc{x}Ge alloys within the range of stability of the CeScSi-type structure: 0.25<x<1. Along this concentration range, this strongly anisotropic system presents a complex magnetic phase diagram with a continuous modification of its magnetic behavior, from ferromagnetism (FM)for 0.25<x<0.50 (with 7K<Tc<16K) to AFM for 0.60<x<1 (with 19K<Tn<47K). The onset of the AFM phase is associated to a metamagnetic transition with a critical field increasing from H{cr}=0 at x~0.55 to ~6Tesla at x=1, coincident with an increasing contribution of the first excited crystal electric field doublet. At a critical point x{cr}=0.65 a second transition appears at Tl<Tn. In contrast to observations in itinerant systems like CeRh{2}Si{2} or CeRh{3}B{2}, no evidences for significant hybridization of the 4f electrons at large Sc contents were found. Therefore, the exceptionally large Tn of CeScGe can be attributed to an increasing RKKY inter-layer interaction as Sc content grows.

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From itinerant to local transformation and critical point in Ni-rich Ce_2(Ni_{1-y}Pd_y)_2Sn

Structural, magnetic (M) and thermal (C_m) studies on Ce_2(Ni_{1-y}Pd_y)_2Sn alloys are presented within the 0<y<0.55 range of concentration, showing evidences for itinerant to local electronic transformation. At variance with RKKY type interactions between localized moments μ_{eff}, the substitution of Ni by isoelectronic Pd leads the antiferromagnetic transition to decrease from T_N~3.8K to ~1.2K between y=0 and 0.48, while M(H) measured at H=5Tesla and 1.8K rises from 0.12 up to 0.75μ_B/Ce-at. Furthermore, the C_m(T_N) jump increases with concentration whereas |θ_P| decreases. The magnetic entropy S_m(T) grows moderately with temperature for y=0 due to a significant contribution of excited levels at low energy, while at y=0.5 it shows a incipient plateau around S_m=Rln2. All these features reflect the progressive ground state transformation of from itinerant to a local character. Another peculiarity of this system is the nearly constant value of C_m(T_N) that ends in an "entropy bottleneck" as T_N decreases. Consequently, the system shows a critical point at y_{cr}~0.48 with signs of ferromagnetic behavior above H_{cr}~0.3T. A splitting of the C_m(T_N) maximum, tuned by field and concentration, indicates a competition between two magnetic phases, with respective peaks at T_N~1.2K and T_I~1.45K.

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Searching for a quantum critical point in YbCu5-xAux

Structural, magnetic, transport and thermal properties of YbCu5-xAux alloys with Au concentration between the limit of structural stability of AuBe5 type at x = 0.4 up to x = 0.7 are reported. The outstanding features of this system are: i) the constant and record high values of Cm /T 7J/molK^2 below a characteristic temperature T*, ranging between 150 mK and 350 mK. ii) A power law thermal dependence dependence Cm/T(T>T*)=A/T^q, with q = 1.3 +/- 0.1, and iii) an arising incoherent electronic scattering observed in the resistivity at T < 1K for x < 0.6 despite the fact that Yb magnetic atoms are placed in a lattice. Magnetic frustration, originated in the tetrahedral distribution of Yb atoms, appears as the responsible of the exotic behavior of this system.

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Exploring high temperature magnetic order in CeTi_1-xSc_xGe

Most of magnetic transitions related to Ce ordering are found below T_ord~12K. Among the few cases exceeding that temperature, two types of behaviors can be distinguished. One of them is related to the rare cases of Ce binary compounds formed in BCC structures, with a quartet ground state, whose degeneracy is reduced by undergoing different types of transitions mostly structural. The other group shows evidences of itinerant character with the outstanding example of CeRh_3B_2 showing the highest T_ord=115K. The second highest ordering temperature has been reported for CeScGe with T_ord=47K, but the nature of this magnetic state has not been investigated very deeply. In order to shed more light into this unusual high temperature ordering we studied the structural, magnetic, transport and thermal properties of CeTi_1-xSc_xGe alloys in the stability range of the CeScSi-type structure 0.25 0.65, the magnetic phase boundary splits into two transitions, with an intermediate phase presenting incommensurate spin density waves features.

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Interpretation of experimental results on Kondo systems with crystal field

We present a simple approach to calculate the thermodynamic properties of single Kondo impurities including orbital degeneracy and crystal field effects (CFE) by extending a previous proposal by K. D. Schotte and U. Schotte [Physics Lett. A 55, 38 (1975)]. Comparison with exact solutions for the specific heat of a quartet ground state split into two doublets shows deviations below $10\%$ in absence of CFE and a quantitative agreement for moderate or large CFE. As an application, we fit the measured specific heat of the compounds CeCu$_2$Ge$_2$, CePd$_{3}$Si$_{0.3}$, CePdAl, CePt, Yb$_2$Pd$_2$Sn and YbCo$_2$Zn$_{20}$. The agreement between theory and experiment is very good or excellent depending on the compound, except at very low temperatures due to the presence of magnetic correlations (not accounted in the model).

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