Thermopower and Entropy: lessons from Sr₂RuO₄

We calculate the in-plane Seebeck coefficient of Sr$_2$RuO$_4$ within a framework combining electronic structure and dynamical mean-field theory. We show that its temperature-dependence is consistent with entropic considerations embodied in the Kelvin formula, and that it provides a meaningful probe of the crossover out of the Fermi liquid regime into an incoherent metal. This crossover proceeds in two stages: the entropy of spin degrees of freedom is released around room-temperature while orbital degrees of freedom remain quenched up to much higher temperatures. This is confirmed by a direct calculation of the corresponding susceptibilities, and is a hallmark of `Hund's metals'. We also calculate the c-axis thermopower, and predict that it exceeds substantially the in-plane one at high-temperature, a peculiar behaviour which originates from an interlayer 'hole-filtering' mechanism.