We develop a computational framework, based on the Boltzmann transport equation (BTE), with the ability to compute thermal transport in nanostructured materials of any geometry using, as the only input, the bulk cumulative thermal conductivity. The main advantage of our method is twofold. First, while the scattering times and dispersion curves are unknown for most materials, the phonon mean free path (MFP) distribution can be directly obtained by experiments. As a consequence, a wider range of materials can be simulated than with the frequency-dependent (FD) approach. Second, when the MFP distribution is available from theoretical models, our approach allows one to include easily the material dispersion in the calculations without discretizing the phonon frequencies for all polarizations thereby reducing considerably computational effort. Furthermore, after deriving the ballistic and diffusive limits of our model, we develop a multiscale method that couples phonon transport across different scales, enabling efficient simulations of materials with wide phonon MFP distributions length. After validating our model against the FD approach, we apply the method to porous silicon membranes and find good agreement with experiments on mesoscale pores. By enabling the investigation of thermal transport in unexplored nanostructured materials, our method has the potential to advance high-efficiency thermoelectric devices.

This study aims to investigate the specific heat capacity of a carbonate salt eutectic-based multiwalled carbon nanomaterial (or high temperature nanofluids). The specific heat capacity of the nanomaterials was measured both in solid and liquid phase using a differential scanning calorimetry (DSC). The effect of the carbon nanotube (CNT) concentrations on the specific heat capacity was examined in this study. The carbonate molten salt eutectic with a high melting point around 490 °C, which consists of lithium carbonate of 62% and potassium carbonate of 38% by the molar ratio, was used as a base material. Multiwalled CNTs were dispersed in the carbonate salt eutectic. A surfactant, sodium dodecyl sulfate (SDS) was utilized to obtain homogeneous dispersion of CNT into the eutectic. Four different concentrations (0.1, 0.5, 1, and 5 wt.%) of CNT were employed to explore the specific heat capacity enhancement of the nanomaterials as the concentrations of the nanotubes varies. In result, it was observed that the specific heat capacity was enhanced by doping with the nanotubes in both solid and liquid phase. Additionally, the enhancements in the specific heat capacity were increased with increase of the CNT concentration. In order to check the uniformity of dispersion of the nanotubes in the salt, scanning electron microscopy (SEM) images were obtained for pre-DSC and post-DSC samples. Finally, the specific heat capacity results measured in present study were compared with the theoretical prediction.

Anomalous enhancements in the specific heat capacity values of nanomaterials were measured in this study. Silica nanoparticles (∼2–20 nm) were dispersed into eutectic of lithium carbonate and potassium carbonate (62:38 by molar ratio) at 1.5% mass concentration. The specific heat capacity measurements were performed using a differential scanning calorimeter (DSC). The specific heat capacity of the silica nanocomposite (solid phase) was enhanced by 38–54% and the specific heat of the silica nanofluid (liquid phase) was enhanced by 118–124% over that of the pure eutectic. Electron microscopy of the samples shows that the nanoparticles induce phase change (forms a higher density “compressed phase”) within the solvent material. Hence, a new model is proposed to account for the contribution of the compressed phase to the total specific heat capacity of the nanomaterials. The proposed model is found to be in good agreement with the experimental data. These results have wide ranging implications, such as for the development of efficient thermal storage systems that can enable significant reduction in the cost of solar thermal power.

Superlattices with thermal-insulating behaviors have been studied to design thermoelectric materials but affect heat transfer in only one main direction and often show many cracks and dislocations near their layer interfaces. Quantum-dot (QD) self-assembly is an emerging epitaxial technology to design ultradense arrays of germanium QDs in silicon for many promising electronic and photonic applications such as quantum computing, where accurate QD positioning is required. We theoretically demonstrate that high-density three-dimensional (3D) arrays of molecular-size self-assembled Ge QDs in Si can also show very low thermal conductivity in the three spatial directions. This physical property can be considered in designing new silicon-based crystalline thermoelectric devices, which are compatible with the complementary metal-oxide-semiconductor (CMOS) technologies. To obtain a computationally manageable model of these nanomaterials, we investigate their thermal-insulating behavior with atomic-scale 3D phononic crystals: A phononic-crystal period or supercell consists of diamond-cubic (DC) Si cells. At each supercell center, we substitute Si atoms by Ge atoms in a given number of DC unit cells to form a boxlike nanoparticle (i.e., QD). The nanomaterial thermal conductivity can be reduced by several orders of magnitude compared with bulk Si. A part of this reduction is due to the significant decrease in the phonon group velocities derived from the flat dispersion curves, which are computed with classical lattice dynamics. Moreover, according to the wave-particle duality at small scales, another reduction is obtained from multiple scattering of the particlelike phonons in nanoparticle clusters, which breaks their mean free paths (MFPs) in the 3D nanoparticle array. However, we use an incoherent analytical model of this particlelike scattering. This model leads to overestimations of the MFPs and thermal conductivity, which is nevertheless lower than the minimal Einstein limit of bulk Si and is reduced by a factor of at least 165 compared with bulk Si in an example nanomaterial. We expect an even larger decrease in the thermal conductivity than that predicted in this paper owing to multiple scattering, which can lead to a Z T much larger than unity.

Low-dimensional nanostructured materials are promising candidates for high efficiency solid-state cooling devices based on the Peltier effect. Thermal transport in these low-dimensional materials is a key factor for device performance since the thermoelectric figure of merit is inversely proportional to thermal conductivity. Therefore, understanding thermal transport in nanostructured materials is crucial for engineering high performance devices. Thermal transport in semiconductors is dominated by lattice vibrations called phonons, and phonon transport is often markedly different in nanostructures than it is in bulk materials for a number of reasons. First, as the size of a structure decreases, its surface area to volume ratio increases, thereby increasing the importance of boundaries and interfaces. Additionally, at the nanoscale the characteristic length of the structure approaches the phonon wavelength, and other interesting phenomena such as dispersion relation modification and quantum confinement may arise and further alter the thermal transport. In this paper we discuss phonon transport in semiconductor superlattices and nanowires with regards to applications in solid-state cooling devices. Systematic studies on periodic multilayers called superlattices disclose the relative importance of acoustic impedance mismatch, alloy scattering, and crystalline imperfections at the interfaces. Thermal conductivity measurements of mono-crystalline silicon nanowires of different diameters reveal the strong effects of phonon-boundary scattering. Experimental results for Si/SiGe superlattice nanowires indicate that different phonon scattering mechanisms may disrupt phonon transport at different frequencies. These experimental studies provide insight regarding the dominant mechanisms for phonon transport in nanostructures. Finally, we also briefly discuss Peltier coolers made from nanostructured materials that have shown promising cooling performance.