Magnetic field dependent specific heat and enhanced Wilson ratio in strongly correlated layered cobalt oxide

Abstract : We have investigated the low-temperature specific-heat properties as a function of magnetic field in the strongly correlated layered cobalt oxide BiBa 0.66 K 0.36 O 2 CoO 2. These measurements reveal two kinds of magnetic field dependent contributions in qualitative agreement with the presence of a previously inferred magnetic quantum critical point QCP. First, the coefficient of the low-temperature T 3 behavior of the specific heat turns out to sizably decrease near a magnetic field consistent with the critical value reported in a recent paper. In addition, a moderate but significant enhancement of the Sommerfeld coefficient is found in the vicinity of the QCP suggesting a slight increase in the electronic effective mass. This result contrasts with the divergent behavior of the previously reported Pauli susceptibility. Thus, a strongly enhanced Wilson ratio is deduced, suggesting efficient ferromagnetic fluctuations in the Fermi-liquid regime which could explain the unusual magnetic field dependent specific heat. As a strong check, the high magnetic field Wilson ratio asymptotically recovers the universal limit of the local Fermi liquid against ferromagnetism. Transition-metal oxides have demonstrated over the last decades how the strong correlations could lead to unantici-pated electronic properties. Outstanding examples 1 are super-conducting cuprates, manganites with their colossal negative magnetoresistance, 2 vanadates displaying the Mott metal-insulator transition, 3 and the layered cobalt oxides which exhibit an unexpected large thermopower at room temperature. 4 Most of these oxides share in common that they are doped Mott insulator, i.e., their metallicity originates from the introduction of charge carriers by doping; otherwise , the strong Coulomb repulsion would localize electrons to form a Mott insulating state. 1,5 Belonging to this class of materials the layered cobalt oxides have revealed, besides their enhanced room-temperature thermopower, 6 a very rich phase diagram as well as striking properties 7-9 including large negative magnetoresistance in some compounds 10 or giant electron-electron scattering in Na 0.7 CoO 2. 11 Interestingly , the latter observation has already led to conjecture a possible influence of a magnetic QCP in the aforementioned compound. Density-functional calculations have also predicted at the local spin-density approximation level weak itinerant ferromagnetic state competing with weak itinerant antiferromagnetic state, favoring then quantum critical fluctuations. 12 Within this context, susceptibility measurements have recently demonstrated in the strongly correlated layered cobalt oxide BiBa 0.66 K 0.36 O 2 CoO 2 the existence of a magnetic quantum critical point QCP governing the electronic properties. 13 The investigated susceptibility has revealed a scaling behavior with both the temperature T and the magnetic field B ranging from a high-T non-Fermi liquid down to a low-T Fermi liquid. In the latter Fermi-liquid regime, the Pauli susceptibility has exhibited a divergent behavior with a power-law dependence as b −0.6 with b = B − B C which measures the distance from the QCP and the critical magnetic field B C 0.176 T. While several scenarios could explain this result, this behavior may in particular originate from either an enhancement of the electronic effective mass due to the vicinity of the QCP or because of the presence of efficient ferromagnetic fluctuations increasing the Pauli susceptibility by a Stoner factor. In order to put these scenarios under experimental test, we have investigated the low-temperature specific-heat properties as a function of magnetic field in the layered cobalt oxide BiBa 0.66 K 0.36 O 2 CoO 2 , which we report on in this paper. Similarly to Na x CoO 2 , the structure of the layered cobalt oxide BiBa 0.66 K 0.36 O 2 CoO 2 abbreviated hereafter as BBCO contains single CoO 2 layer of CdI 2 type stacked with four rocksalt-type layers, instead of a sodium deficient layer, which act as a charge reservoir. 14 The reported measurements have been performed on a single crystal with a mass of 35 mg which was grown using standard flux method. 15 The specific heat has been determined with a calo-rimeter of a Quantum Design physical properties measurement system using a relaxation method with a temperature rise on the order of 2% of the sample temperature. It is worthy to note that the calorimeter, including the thermometers , has been calibrated with each magnetic field up to 9 T. In addition, all the measurements have been duplicated without the sample for each magnetic field in order to compensate both the temperature and magnetic field dependences of the grease used to ensure a good thermal contact between the sample and the calorimeter platform. We also mention that the calorimeter's parameter which indicates the quality of the thermal contact between the sample and the platform, the so-called sample coupling, has remained between 97% and 100% during each measurement below 100 K, ensuring thus the reliability of the results. Figure 1 displays the temperature dependence of the specific heat over the range from 300 K down to 1.9 K on a double-logarithmic scale in order to show both the low-and the high-temperature behaviors. As frequently observed, the PHYSICAL REVIEW B 82, 035123 2010
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P. Limelette, H. Muguerra, S. Hebert. Magnetic field dependent specific heat and enhanced Wilson ratio in strongly correlated layered cobalt oxide. Physical Review B : Condensed matter and materials physics, American Physical Society, 2010, 82 (3), ⟨10.1103/physrevb.82.035123⟩. ⟨hal-01870095⟩

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