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Artificially engineered 2D materials offer unique physical properties for thermal management, surpassing naturally occurring materials. Here, using van der Waals epitaxy, we demonstrate the ability to engineer extremely insulating ultra-thin thermal metamaterials based on crystalline lattice-mismatched Bi2Se3/MoSe2 superlattices and graphene/PdSe2 heterostructures with exceptional thermal resistances (70-202 m^2K/GW) and ultralow cross-plane thermal conductivities (0.01-0.07 Wm^-1K^-1) at room temperature, comparable to those of amorphous materials. Experimental data obtained using frequency-domain thermoreflectance and low-frequency Raman spectroscopy, supported by tight-binding phonon calculations, reveal the impact of lattice mismatch, phonon-interface scattering, size effects, temperature and interface thermal resistance on cross-plane heat dissipation, uncovering different thermal transport regimes and the dominant role of long-wavelength phonons. Our findings provide essential insights into emerging synthesis and thermal characterization methods and valuable guidance for the development of large-area heteroepitaxial van der Waals films of dissimilar materials with tailored thermal transport characteristics., Comment: 25 page 4 figures

Phonons play a key role in the physical properties of materials, and have long been a topic of study in physics. While the effects of phonons had historically been considered to be a hindrance, modern research has shown that phonons can be exploited due to their ability to couple to other excitations and consequently affect the thermal, dielectric, and electronic properties of solid state systems, greatly motivating the engineering of phononic structures. Advances in nanofabrication have allowed for structuring and phonon confinement even down to the nanoscale, drastically changing material properties. Despite developments in fabricating such nanoscale devices, the proper manipulation and characterization of phonons continues to be challenging. However, a fundamental understanding of these processes could enable the realization of key applications in diverse fields such as topological phononics, information technologies, sensing, and quantum electrodynamics, especially when integrated with existing electronic and photonic devices. Here, we highlight seven of the available methods for the excitation and detection of acoustic phonons and vibrations in solid materials, as well as advantages, disadvantages, and additional considerations related to their application. We then provide perspectives towards open challenges in nanophononics and how the additional understanding granted by these techniques could serve to enable the next generation of phononic technological applications., Comment: 50 pages

We present a comparative investigation of the influence of crystallinity and film thickness on the acoustic and thermal properties of 2D layered PtSe2 thin films of varying thickness (0.6-24 nm) by combining a set of experimental techniques, namely, frequency domain thermo-reflectance, low-frequency Raman and pump-probe coherent phonon spectroscopy. We find a 35% reduction in the cross-plane thermal conductivity of polycrystalline films with thickness larger than 12 nm compared to the crystalline films of the same thickness due to phonon grain boundary scattering. Density functional theory calculations are in good agreement with the experiments and further reveal the ballistic nature of cross-plane heat transport in PtSe2 up to a certain thickness (~20 nm). In addition, our experiments revealed strong interlayer interactions in PtSe2, short acoustic phonon lifetimes in the range of picoseconds, out-of-plane elastic constant C33=31.8 GPa and layer-dependent group velocity ranging from 1340 m/s in bilayer PtSe2 to 1873 m/s in 8 layers of PtSe2. The potential of tuning the lattice cross-plane thermal conductivity of layered 2D materials with the level of crystallinity and the real-time observation of coherent phonon dynamics, which have direct implications on the cooling and transport of electrons, open a new playground for research in 2D thermoelectric devices and provide guidelines for thermal management in 2D electronics., Comment: 32 pages

Controlling thermal energy transfer at the nanoscale has become critically important in many applications and thermal properties since it often limits device performance. In this work, we study the effects on thermal conductivity arising from the nanoscale structure of free-standing nanocrystalline silicon films and the increasing surface-to-volume ratio when fabricated into suspended optomechanical nanobeams. We characterize thermal transport in structures with different grain sizes and elucidate the relative impact of grain size and geometrical dimensions on thermal conductivity. We use a micro-time-domain thermoreflectance method to study the impact of the grain size distribution, from 10 to 400 nm, on the thermal conductivity in free-standing nanocrystalline silicon films considering surface phonon and grain boundary scattering. We find a drastic reduction in the thermal conductivity, down to values of 10 W.m^{-1}.K^{-1} and below, which is just a fraction of the conductivity of single crystalline silicon. Decreasing the grain size further decreases the thermal conductivity. We also observe that this effect is smaller in OM nanostructures than in membranes due to the competition of surface scattering in decreasing thermal conductivity. Finally, we introduce a novel versatile contactless characterization technique that can be adapted to any structure supporting a thermally shifted optical resonance and use it to evaluate the thermal conductivity. This method can be used with optical resonances exhibiting different mode profiles and the data is shown to agrees quantitatively with the thermoreflectance measurements. This work opens the way to a more generalized thermal characterization of optomechanical cavities and to create hot-spots with engineered shapes at desired position in the structures as a means to study thermal transport in coupled photon-phonon structures.

Nanocrystalline materials exhibit properties that can differ substantially from those of their single crystal counterparts. As such, they provide ways to enhance and optimise their functionality for devices and applications. Here we report on the optical, mechanical and thermal properties of nanocrystalline silicon probed by means of optomechanical nanobeams to extract information of the dynamics of optical absorption, mechanical losses, heat generation and dissipation. The optomechanical nanobeams are fabricated using nanocrystalline films prepared by annealing amorphous silicon layers at different temperatures. The resulting crystallite sizes and the stress in the films can be controlled by the annealing temperature and time and, consequently, the properties of the films can be tuned relatively freely, as demonstrated here by means of electron microscopy and Raman scattering. We show that the nanocrystallite size and the volume fraction of the grain boundaries play a key role in the dissipation rates through non-linear optical and thermal processes. Promising optical (13000) and mechanical (1700) quality factors were found in the optomechanical cavity realised in the nanocrystalline Si resulting from annealing at 950 C. The enhanced absorption and recombination rates via the intra-gap states and the reduced thermal conductivity boost the potential to exploit these non-linear effects in applications, including NEMS, phonon lasing and chaos-based devices., Comment: 31 pages, 5 figures

The quest to improve the thermoelectric figure of merit has mainly followed the roadmap of lowering the thermal conductivity while keeping unaltered the power factor of the material. Ideally an electron-crystal phonon-glass system is desired. In this work, we report an extraordinary reduction of the cross-plane thermal conductivity in crystalline (TiNiSn):(HfNiSn) half-Heusler superlattices. We create SLs with thermal conductivities below the effective amorphous limit, which is kept in a large temperature range (120-300 K). We measured thermal conductivity at room temperature values as low as 0.75 W/(m K), the lowest thermal conductivity value reported so far for half-Heusler compounds. By changing the deposition conditions, we also demonstrate that the thermal conductivity is highly impacted by the way the single segments of the superlattice grow. These findings show a huge potential for thermoelectric generators where an extraordinary reduction of the thermal conductivity is required but without losing the crystal quality of the system., Comment: 35 pages, include SI

In this work, we show a phenomenological alloy-like fit of the thermal conductivity of (A)d1:(B)d2 superlattices with d1 /= d2, i.e. non-symmetric structure. The presented method is a generalization of the Norbury rule of the summation of thermal resistivities in alloy compounds. Namely, we show that this approach can be also extended to describe the thermal properties of crystalline and ordered-system composed by two or more elements, and, has a potentially much wider application range. Using this approximation we estimate that the interface thermal resistance depends on the period and the ratio of materials that form the superlattice structure, Comment: 11 pages, 3 figures