Enhanced electronic effective mass in the anomalous Pb1-xTlxTe superconductor

The thermoelectric material PbTe, besides providing an alternative for power generation and refrigeration, also presents a series of unusual and poorly understood low-temperature electronic properties when appropriately doped. Of particular relevance to the present work, Tl substitution yields a metallic state, with no carrier freeze out to the lowest temperatures, and a superconducting ground-state for concentrations x > xc ~ 0.3%. The critical temperature increases linearly with the concentration of Tl dopants, with maximum values (Tc ~ 1.4 K) that are anomalously high for the given carrier density of about 1020 holes/cm3. Significantly, Tl is the only dopant to cause superconductivity in this material, so, for example, the analogous case of hole doping via Na substitution does not lead to superconductivity down to the lowest investigated temperature. It has therefore been conjectured that the special nature of the Tl impurities plays a prominent role.

We perform a thorough optical investigation of Pb1-xTlxTe over a very broad spectral range and contrast its normal-state, complete excitation spectrum with the optical response of the non-superconducting analog Na-doped PbTe. We address their electronic structure and uncover the formation of an impurity band upon doping with Tl, which evolves into a resonant state for large doping. This implies a large density of states and an enhancement of the optical effective mass m*/me of the itinerant charge carriers (Fig. 1.12).

Enlarged view: Fig. 1.12
Fig. 1.12: Optical mass m*/me and charge carrier concentration n as a function of the doping content in Pb1-xTlxTe (a,c) and Pb1-yNayTe (b,d). The measured pHall values from Hall data are shown as comparison. The vertical thin dashed line in panels (a) and (c) marks xc ~ 0.3%. The dashed lines in all panels are spline data interpolations as a guide to the eye. The scheme in panel (a) sketches the proposed DOS, with the formation of the resonant impurity band.

Even though the overall optical response for both Na- and Tl-doped PbTe shares rather common, similar features, it clearly emerges from our investigation that the effective optical mass m*/me is the key quantity somehow discriminating between the two investigated PbTe compositions. We provide evidence for a stronger enhancement of the optical effective mass in Pb1-xTlxTe for x > xc than in Pb1-yNayTe. Our results advance the intriguing possibility that superconductivity may result from the pairing of 'heavy' quasiparticles associated to charged valence-states, compatible with recent theoretical ideas based on the charge-Kondo scenario.

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