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Polymers, despite their desirable structural properties, suffer from low thermal conductivity, which restricts their use. Previous studies have indicated that the strong bond-stretching and angular-bending interactions along the chain are believed to have saturated the maximum achievable thermal conductivity in the along-the-chain direction. Contrary to this belief, our results show an improvement in thermal conductivity. By increasing the bond and angle potential, we studied the effect on the thermal conductivity of polyethylene using non-equilibrium molecular dynamics simulations. In comparison to restricting the bond stretching, we found that restricting angular bending freedom plays a crucial role in improving the thermal transport along the chain. We observed significant changes in the morphology of the polyethylene chains when the angle potential was increased. We also found a remarkable increase in the phonon group velocity accompanied by large shifts in the longitudinal acoustic branch of the dispersion curve. These results when coupled with the structural changes strongly support the argument that thermal conductivity can be controlled by restricting the angular bending freedom.

Several models have been employed in the past to estimate interfacial thermal conductance (ITC) for different material interfaces, of which the diffuse mismatch model (DMM) has been generally accepted as reliable for rough material interfaces at high temperature. Even though the DMM has been shown to predict the correct order of magnitude in isotropic material interfaces, it is unable to reproduce the same accuracy for low-dimensional anisotropic layered materials, which have many potential applications. Furthermore, the use of approximated dispersion curves tends to overestimate the ITC. In this work, we propose a new method that utilizes a mode-to-mode comparison within the DMM framework to predict ITC. We employed this model to calculate ITC between layered materials such as MoS2 and graphite and metals such as Al, Au, and Cr. We then compared our values with previous literature data that employ linear dispersion relations and experimental data from time-domain thermoreflectance measurements. This new framework was then used to visualize the phonon focusing effect in anisotropic materials. Further analysis revealed that counting only the three acoustic modes and neglecting the low-frequency optical modes lead to significant underestimation of the ITC using DMM. Our findings indicate that it is imperative to use the exact full phonon dispersion relations in evaluating the ITC for low-dimensional layered materials.

We use the Boltzmann transport equation under the relaxation time approximation to investigate the effect of minority blocking on the transport properties of nanocomposites (NCs). Taking p-type Bi0.5Sb1.5Te3 NCs as an example, we find that the thermally excited minority carriers can be strongly scattered by engineered interfacial potential barriers. Such scattering phenomena suppress the bipolar effect, which is helpful to enhance the Seebeck coefficient and reduce the electronic thermal conductivity, especially at high temperatures. Further combining with the majority carriers low-energy filtering effect, the power factor and the figure of merit (ZT) can be significantly enhanced over a large temperature range from 300 K to 500 K. Such an improvement of ZT is attributed to the majority carriers low-energy filtering effect at low temperatures and to the minority carriers blocking effect at high temperatures. A principle that is helpful to provide guidance on the thermoelectric device design is identified: (1) blocking the minority carriers as often as possible and (2) filtering the majority carriers whose energy is lower than 2–3kBT near the cold end.

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