Heterostructure core-shell semiconductor nanowires (NWs) have attracted tremendous interest recently due to their remarkable properties and potential applications as building blocks for nanodevices. Among their unique traits, thermal properties would play a significant role in thermal management of future heterostructure NW-based nanoelectronics, nanophotonics, and energy conversion devices, yet have been explored much less than others. Similar to their electronic counterparts, phonon spectrum and thermal transport properties could be modified by confinement effects and the acoustic mismatch at the core-shell interface in small diameter NWs (<20 nm). However, fundamental thermal measurement on thin core shell NWs has been challenging due to their small size and their expected low thermal conductivity (κ). Herein, we have developed an experimental technique with drastically improved sensitivity capable of measuring thermal conductance values down to ∼10 pW/K. Thermal conductivities of Ge and Ge-Si core-shell NWs with diameters less than 20 nm have been measured. Comparing the experimental data with Boltzmann transport models reveals that thermal conductivities of the sub-20 nm diameter NWs are further suppressed by the phonon confinement effect beyond the diffusive boundary scattering limit. Interestingly, core-shell NWs exhibit different temperature dependence in κ and show a lower κ from 300 to 388 K compared to Ge NWs, indicating the important effect of the core-shell interface on phonon transport, consistent with recent molecular dynamics studies. Our results could open up applications of Ge-Si core shell NWs for nanostructured thermoelectrics, as well as a new realm of tuning thermal conductivity by "phononic engineering".
We experimentally studied the thermoelectric power factor of hole gas in individual Ge-Si core-shell nanowires with Ge core diameters ranging from 11 to 25 nm. The Ge cores are dopant-free, but the Fermi level in the cores is pinned by surface and defect states in the epitaxial Si shell thereby doping the cores into the degenerate regime. This doping mechanism avoids the high concentration of dopants usually encountered in bulk thermoelectric materials and provides a unique opportunity to enhance the carrier mobility with suppressed ionized impurity scattering. Moreover, the carrier concentration in small diameter nanowires has also been effectively modulated by field effect, allowing one to probe the electrical conductivity and thermopower within a wide range of carrier concentrations, which is crucial to understand the thermoelectric transport behavior. We found that the thermopower of nanowires with Ge core diameters down to 11 nm still follows the behavior of bulk Ge. As a result, the power factor is found to be closely correlated with the carrier mobility, which is higher than that of bulk Ge in one of the core-shell nanowires studied here.
Polyacrylonitrile (PAN) and PAN/carbon nanotube (CNT) based carbon fibers at various CNT content have been processed and their structural development was investigated using high resolution transmission electron microscope (HR-TEM). For CNT containing carbon fibers, the CNTs act as templating agents for the graphitic carbon structure development in their vicinity at the carbonization temperature of 1450 o C, which is far below the graphitization temperature of PAN based carbon fiber (>2200 o C). The addition of 1 wt% CNT in the gel spun precursor fiber results in carbon fibers with a 68% higher thermal conductivity when compared to the control gel spun PAN based carbon fiber, and a 103% and 146% increase over commercially available IM7 and T300 carbon fibers, respectively. The electrical conductivity of the gel spun PAN/CNT based carbon fibers also showed improvement over the investigated commercially available carbon fibers. Increases in thermal and electrical conductivities are attributed to the formation of the highly ordered graphitic structure observed in the HR-TEM images. Direct observation of the graphitic structure, along with improved transport properties in the PAN/CNT based carbon fiber suggest new applications for these materials.
Thermal transport in multilayers (MLs) has attracted significant interest and shows promising applications. Unlike their single-component counterparts, MLs exhibit a thermal conductivity that can be effectively engineered by both the number density of the layers and the interfacial thermal resistance between layers, with the latter being highly tunable via the contrast of acoustic properties of each layer. In this work, we experimentally demonstrated an ultralow thermal conductivity of 0.33 ± 0.04 W m(-1) K(-1) at room temperature in MLs made of Au and Si with a high interfacial density of ∼0.2 interface nm(-1). The measured thermal conductivity is significantly lower than the amorphous limit of either Si or Au and is also much lower than previously measured MLs with a similar interfacial density. With a Debye temperature ratio of ∼3.9 for Au and Si, the Au/Si MLs represent the highest mismatched system in inorganic MLs measured to date. In addition, we explore the prior theoretical prediction that full phonon dispersion could better model the interfacial thermal resistance involving materials with low Debye temperatures. Our results demonstrate that MLs with highly dissimilar Debye temperatures represent a rational approach to achieve ultralow thermal conductivity in inorganic materials and can also serve as a platform for investigating interfacial thermal transport.
The thermal atomic vibrations of amorphous solids can be distinguished by whether they propagate as elastic waves or do not propagate due to lack of atomic periodicity. In a-Si, prior works concluded that nonpropagating waves are the dominant contributors to heat transport, with propagating waves being restricted to frequencies less than a few THz and scattered by anharmonicity. Here, we present a lattice and molecular dynamics analysis of vibrations in a-Si that supports a qualitatively different picture in which propagating elastic waves dominate the thermal conduction and are scattered by local fluctuations of elastic modulus rather than anharmonicity. We explicitly demonstrate the propagating nature of waves up to around 10 THz, and further show that pseudoperiodic structures with homogeneous elastic properties exhibit a marked temperature dependence characteristic of anharmonic interactions. Our work suggests that most heat is carried by propagating elastic waves in a-Si and demonstrates that manipulating local elastic modulus variations is a promising route to realize amorphous materials with extreme thermal properties.
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