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Manipulating a crystalline material's configurational entropy through the introduction of unique atomic species can produce novel materials with desirable mechanical and electrical properties. From a thermal transport perspective, large differences between elemental properties such as mass and interatomic force can reduce the rate at which phonons carry heat and thus reduce the thermal conductivity. Recent advances in materials synthesis are enabling the fabrication of entropy-stabilized ceramics, opening the door for understanding the implications of extreme disorder on thermal transport. Measuring the structural, mechanical, and thermal properties of single-crystal entropy-stabilized oxides, it is shown that local ionic charge disorder can effectively reduce thermal conductivity without compromising mechanical stiffness. These materials demonstrate similar thermal conductivities to their amorphous counterparts, in agreement with the theoretical minimum limit, resulting in this class of material possessing the highest ratio of elastic modulus to thermal conductivity of any isotropic crystal. CeramicsHigh-entropy alloys (HEAs), consisting of five or more approximately equimolar compositions of elements, [1,2] have proven to exhibit unique physical properties such as high hardness, [3] thermal stability, [4] structural stability, [5] as well as corrosion, oxidation, and wear resistance. [6][7][8] While microstructure and mechanical properties have been extensively studied, thermal

We investigate thickness-limited size effects on the thermal conductivity of amorphous silicon thin films ranging from 3 -1636 nm grown via sputter deposition. While exhibiting a constant value up to ∼100 nm, the thermal conductivity increases with film thickness thereafter. This trend is in stark contrast with previous thermal conductivity measurements of amorphous systems, which have shown thickness-independent thermal conductivities. The thickness dependence we demonstrate is ascribed to boundary scattering of long wavelength vibrations and an interplay between the energy transfer associated with propagating modes (propagons) and nonpropagating modes (diffusons). A crossover from propagon to diffuson modes is deduced to occur at a frequency of ∼1.8 THz via simple analytical arguments. These results provide empirical evidence of size effects on the thermal conductivity of amorphous silicon and systematic experimental insight into the nature of vibrational thermal transport in amorphous solids.

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In this study, we present a method to calculate the temperature and heat flux profiles as a function of depth and radius for bulk, homogeneous materials and samples with layered thin-film structures, including geometries supporting bidirectional heat fluxes, during pulsed and continuous wave (CW) laser heating. We calculate the temperature profiles for both modulated and unmodulated heating events to reveal that the thermal penetration depth (defined as the depth at which temperature decays to 1/e of the surface temperature) for a pulsed laser is highly dependent on time and repetition rate. In the high repetition rate limit, the temperature profile relaxes to that of a CW source profile, while in the opposite extreme, a single pulse response is observed such that the concept of the thermal penetration depth loses any practical meaning. For modulated heating events such as those used in time-and frequency-domain thermoreflectance, we show that there is a limit to the thermal penetration depth obtainable in an experiment, such that simple analytical expressions commonly used to determine thermal penetration depth break down. This effect is further compounded in samples with multiple layers, including the case when a $100 nm metallic transducer is deposited onto a bulk substrate, revealing that many recent studies relying on this estimation significantly over-predict the thermal penetration depth. Considering a bidirectional heat flow geometry (e.g., substrate/metal film/liquid), we find that heating from an unmodulated source results in an asymmetric heat flux about the plane of laser absorption to preserve a symmetric temperature profile when interfacial thermal resistance is negligible. However, the modulated case reveals a temperature asymmetry such that the thermal penetration depths in each side fall in line with those resulting from an insulated boundary condition. Published by AIP Publishing.

The role of interfacial nonidealities and disorder on thermal transport across interfaces is traditionally assumed to add resistance to heat transfer, decreasing the thermal boundary conductance (TBC). However, recent computational studies have suggested that interfacial defects can enhance this thermal boundary conductance through the emergence of unique vibrational modes intrinsic to the material interface and defect atoms, a finding that contradicts traditional theory and conventional understanding. By manipulating the local heat flux of atomic vibrations that comprise these interfacial modes, in principle, the TBC can be increased. In this work, experimental evidence is provided that interfacial defects can enhance the TBC across interfaces through the emergence of unique high-frequency vibrational modes that arise from atomic mass defects at the interface with relatively small masses. Ultrahigh TBC is demonstrated at amorphous SiOC:H/SiC:H interfaces, approaching 1 GW m K and are further increased through the introduction of nitrogen defects. The fact that disordered interfaces can exhibit such high conductances, which can be further increased with additional defects, offers a unique direction to manipulate heat transfer across materials with high densities of interfaces by controlling and enhancing interfacial thermal transport.

We demonstrate a steady-state thermoreflectance-based optical pump-probe technique to measure the thermal conductivity of materials using a continuous wave laser heat source. The technique works in principle by inducing a steady-state temperature rise in a material via long enough exposure to heating from a pump laser. A probe beam is then used to detect the resulting change in reflectance, which is proportional to the change in temperature at the sample surface. Increasing the power of the pump beam to induce larger temperature rises, Fourier’s law is used to determine the thermal conductivity. We show that this technique is capable of measuring the thermal conductivity of a wide array of materials having thermal conductivities ranging from 1 to >2000 W m−1 K−1, in excellent agreement with literature values.