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Contrasting magnetic behavior of fine particles of some Kondo Lattices

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 Publication date 2011
  fields Physics
and research's language is English




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We have investigated the magnetic behavior of ball-milled fine particles of well-known Kondo lattices, CeAu2Si2, CePd2Si2 and CeAl2, by magnetization and heat-capacity studies in order to understand the magnetic behavior when the particle size is reduced. These compounds have been known to order antiferromagnetically in the bulk form near (TN=) 10, 10 and 3.8 K respectively. We find that the features due to magnetic ordering get suppressed to temperatures below 1.8 K in the case of fine particles of ternary alloys, though trivalence of Ce as inferred from the effective moment remains unchanged. In contrast to this, in CeAl2, there appears to be a marginal enhancement of TN, when the particle size is reduced to less than a micron. These results can be consistently understood by proposing that there is relatively more 4f-localization as the particle size is reduced, resulting in weakening of exchange interaction strength.



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Despite intense research in the field of strongly correlated electron behavior for the past few decades, there has been very little effort to understand this phenomenon in nano particles of the Kondo lattices. In this article, we review the results of our investigation on the fine particles (less than 1 micron) of some of the alloys obtained by high-energy ball-milling to bring out that this synthetic method paves a way to study strong electron correlations in nanocrystals of such alloys. We primarily focus on the alloys of the series, CeRu(2-x)Rh(x)Si2, lying at different positions in Doniachs magnetic phase diagram. While CeRu2Si2, a bulk paramagnet, appears to become magnetic (of a glassy type) below about 8 K in fine particle form, in CeRh2Si2, an antiferromagnet (T_N= 36 K) in bulk form, magnetism is destroyed (at least down to 0.5 K) in fine particles. In the alloy, CeRu(0.8)Rh(1.2)Si2, at the quantum critical point, no long range magnetic ordering is found
The magnetic behavior of the quaternary compounds, RCr2Si2C (R = La, Ce), has been investigated by magnetization (M) and heat-capacity (C) measurements (1.8-300 K) in the bulk polycrystals and nano forms (<1 {mu}m) obtained by high-energy balling. Our finding is that Cr appears to exhibit magnetic ordering of an itinerant type at low temperatures (<20 K) in the bulk form, as inferred from a combined look at all the data. The magnetic ordering gets gradually suppressed with increasing milling time. Evidence for a mixed-valence state of Ce for the bulk form is obtained from the tendency of magnetic susceptibility to exhibit a maximum above 300 K. However, this feature vanishes in the nano form, which exhibits a Curie-Weiss behavior above 200 K as though Ce tends towards trivalency in these fine particles; in addition, there is a weak upturn in C/T below 10 K in the bulk, which becomes very prominent in the milled Ce-based specimens at lower temperatures, as though heavy-fermion behavior gets stronger in smaller particles.
We report magnetic behavior of two intermetallics-based kagome lattices, Tb3Ru4Al12 and Er3Ru4Al12, crystallizing in the Gd3Ru4Al12-type hexagonal crystal structure, by measurements in the range 1.8-300 K with bulk experimental techniques (ac and dc magnetization, heat-capacity and magnetoresistance). The main finding is that the Tb compound, known to order antiferromagnetically below (T_N=) 22 K, shows glassy characteristics at lower temperatures (<15K), thus characterizing this compound as a re-entrant spin-glass. The data reveal that glassy phase is quite complex and is of a cluster type. Since the glassy behavior was not seen for the Gd analogue in the past literature, this finding for the Tb compound emphasizes that this kagome family could provide an opportunity to explore the role of higher order (such as quadrupole) in bringing out magnetic frustration. Additional findings reported here for this compound are: (i) The temperature dependence of magnetic susceptibility and electrical resistivity in the range 12 - 20 K are found to be hysteretic leading to a magnetic phase in this temperature range, mimicking disorder-induced first-order magnetic phase-transition. (ii) Features attributable to an interesting magnetic phase co-existence phenomenon in the magnetoresistance in zero field, after cycling across metamagnetic transition fields, are observed. With respect to the Er compound, we do not find any evidence for long-range magnetic ordering down to 2 K, but this appears to be on the verge of magnetic order at 2 K.
In this study we report the results of study of novel ternary $Np_2PtGa_3$ compound. The x-ray-powder diffraction analysis reveals that the compound crystallizes in the orthorhombic CeCu$_2$-type crystal structure (space group Imma) with lattice parameters $a$ = 0.4409(2) nm, $b$ = 0.7077(3) nm and $c$ = 0.7683(3) nm at room temperature. The measurements of dc magnetization, specific heat and electron transport properties in the temperature range 1.7 - 300 K and in magnetic fields up to 9 T imply that this intermetallic compound belongs to a class of ferromagnetic Kondo systems. The Curie temperature of $T_C sim$ 26 K is determined from the magnetization and specific heat data. An enhanced coefficient of the electronic specific heat of $gamma$ = 180 mJ/(mol at. Np K$^2$) and -lnT dependence of the electrical resistivity indicate the presence of Kondo effect, which can be described in terms of the S = 1 underscreened Kondo-lattice model. The estimated Kondo temperature $T_K sim$ 24 K, Hall mobility of $sim$ 16.8 cm$^2$/Vs and effective mass of $sim$ 83 $m_e$ are consistent with assumption that the heavy-fermion state develops in $Np_2PtGa_3$ at low temperatures. We compare the observed properties of $Np_2PtGa_3$ to that found in $Np_2PtGa_3$ and discuss their difference in regard to change in the exchange interaction between the conduction and localized 5f electrons. We have used the Fermi wave vector $k_F$ to evaluate the Rudermann-Kittel-Kasuya-Yosida (RKKY) exchange. Based on experimental data of the (U, Np)$_2$(Pd, Pt)Ga$_3$ compounds we suggest that the evolution of the magnetic ground states in these actinide compounds can be explained within the RKKY formalism.
The Kondo model predicts that both the valence at low temperatures and its temperature dependence scale with the characteristic energy T_K of the Kondo interaction. Here, we study the evolution of the 4f occupancy with temperature in a series of Yb Kondo lattices using resonant X-ray emission spectroscopy. In agreement with simple theoretical models, we observe a scaling between the valence at low temperature and T_K obtained from thermodynamic measurements. In contrast, the temperature scale T_v at which the valence increases with temperature is almost the same in all investigated materials while the Kondo temperatures differ by almost four orders of magnitude. This observation is in remarkable contradiction to both naive expectation and precise theoretical predictions of the Kondo model, asking for further theoretical work in order to explain our findings. Our data exclude the presence of a quantum critical valence transition in YbRh2Si2.
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