Isolating lattice from electronic contributions in thermal transport measurements of metals and alloys above ambient temperature and an adiabatic model

Abstract

From femtosecond spectroscopy (fs-spectroscopy) of metals, electrons and phonons reequilibrate nearly independently, which contrasts with models of heat transfer at ordinary temperatures ([Formula: see text] K). These electronic transfer models only agree with thermal conductivity [Formula: see text] data at a single temperature, but do not agree with thermal diffusivity [Formula: see text] data. To address the discrepancies, which are important to problems in solid state physics, we separately measured electronic (ele) and phononic (lat) components of [Formula: see text] in many metals and alloys over [Formula: see text]290–1100 K by varying measurement duration and sample length in laser-flash experiments. These mechanisms produce distinct diffusive responses in temperature versus time acquisitions because carrier speeds [Formula: see text] and heat capacities [Formula: see text] differ greatly. Electronic transport of heat only operates for a brief time after heat is applied because [Formula: see text] is high. High [Formula: see text] is associated with moderate [Formula: see text], long lengths, low electrical resistivity, and loss of ferromagnetism. Relationships of [Formula: see text] and [Formula: see text] with physical properties support our assignments. Although [Formula: see text] reaches [Formula: see text] near 470 K, it is transient. Combining previous data on [Formula: see text] with each [Formula: see text] provides mean free paths and lifetimes that are consistent with [Formula: see text] K fs-spectroscopy, and new values at high [Formula: see text]. Our findings are consistent with nearly-free electrons absorbing and transmitting a small fraction of the incoming heat, whereas phonons absorb and transmit the majority. We model time-dependent, parallel heat transfer under adiabatic conditions which is one-dimensional in solids, as required by thermodynamic law. For noninteracting mechanisms, [Formula: see text]. For metals, this reduces to [Formula: see text] above [Formula: see text]20 K, consistent with our measurements, and shows that Meissner’s equation [Formula: see text] is invalid above [Formula: see text]20 K. For one mechanism with multiple, interacting carriers, [Formula: see text]. Thus, certain dynamic behaviors of electrons and phonons in metals have been misunderstood. Implications for theoretical models and technological advancements are briefly discussed.