Dynamical Symmetry-Reduction-Induced Giant Anharmonicity in IV-VI Compounds: Role of Cation Lone-Pair s Electrons.

The low thermal conductivity of group IV-VI semiconductors is often attributed to the soft phonons and giant anharmonicity observed in these materials. However, there is still no broad consensus on the fundamental origin of this giant anharmonic effect. Utilizing first-principles calculations and group symmetry analysis, we find that the cation lone-pairs s electrons in IV-VI materials cause a significant coupling between occupied cation s orbitals and unoccupied cation p orbitals due to the symmetry reduction when atoms vibrate away from their equilibrium positions under heating. This leads to an electronic energy gain, consequently flattening the potential energy surface and causing soft phonons and strong anharmonic effects. Our findings provide an intrinsic understanding of the low thermal conductivity in IV-VI compounds by connecting the anharmonicity with the dynamical electronic structures, and can also be extended to a large family of hybrid systems with lone-pair electrons, for promising thermoelectric applications and predictive designs.

The six-degrees-of-freedom attitude measurement instrument for the large aperture mirror using the prepressing sensors and flexible supporting.

To achieve precise measurement of a large aperture mirror, a six-degrees-of-freedom (6-DOF) measurement instrument is designed to monitor and calculate the real-time attitude of the mirror. Magnetoelectric displacement sensors are prepressed, and a flexible sensor supporting is designed to achieve high-accuracy measurement. The relationship between 6-DOF displacements of the mirror and the six sensor values can be obtained using the coordinate system transformation and Jacobian matrix. The Newton's iteration method is used to decouple the strong coupling measurement system, and 6-DOF displacements are obtained. The displacements directly measured by using laser sensors are compared with the calculated values in the experiments, the minimum average error of the measured displacement is 1.87%, and the mean difference of the displacement is 0.43 µm.

Band offset trends in IV-VI layered semiconductor heterojunctions.

The band offsets between semiconductors are significantly associated with the optoelectronic characteristics and devices design. Here, we investigate the band offset trends of few-layer and bulk IV-VI semiconductors MX and MX2(M = Ge, Sn; X = S, Se, Te). For common-cation (anion) systems, as the atomic number increases, the valence band offset of MX decreases, while that of MX2has no distinct change, and the physical origin can be interpreted using band coupling mechanism and atomic potential trend. The band edges of GeX2system straddle redox potentials of water, making them competitive candidates for photocatalyst. Moreover, layer number modulation can induce the band offset of GeSe/SnS and GeSe2/GeS2heterojunction undergoing a transition from type I to type II, which makes them suitable for optoelectronic applications.

Decoupling of the Electrical and Thermal Transports in Strongly Coupled Interlayer Materials.

Thermoelectric materials which enable heat-to-electricity conversion are fundamentally important for heat management in semiconductor devices. Achieving high thermoelectric performance requires blocking the thermal transport and maintaining the high electronic transport, but it is a challenge to satisfy both criteria simultaneously. We propose that tuning the interlayer distance can effectively modulate the electrical and thermal conductivities. We find group IV-VI and V semiconductors with a moderate interlayer distance can exhibit high thermoelectric performance. Taking SnSe as an example, we reveal that in the out-of-plane direction the delocalized pz orbitals combined with the relatively small interlayer distance lead to overlapping of the antibonding state wave functions, which is beneficial for high electronic transport. However, because of the breakdown of the chemical bond, the out-of-plane thermal conductivity is small. This study provides a strategy to enhance electrical conductivity without increasing thermal conductivity and thus sheds light on the design of thermoelectric devices.

Phonon-driven electron scattering and magnetothermoelectric effect in two-dimensional tin selenide.

The bulk tin selenide (SnSe) is the best thermoelectric material currently with the highest figure-of-merit due to strong phonon-phonon interactions. We investigate the effect of electron-phonon coupling (EPC) on the transport properties of a two-dimensional (2D) SnSe sheet. We demonstrate that EPC plays a key role in the scattering rate when the constant relaxation time approximation is deficient. The EPC strength is especially large in contrast to that of pristine graphene. The scattering rate depends sensitively on the system temperatures and the carrier densities when the Fermi energy approaches the band edge. We also investigate the magnetothermoelectric effect of the 2D SnSe. It is found that at low temperatures there is enormous magnetoelectrical resistivity and magnetothermal resistivity above 200%, suggesting possible potential applications in device design. Our results agree qualitatively well with the experimental data.

Classical to quantum transition of heat transfer between two silica clusters.

Heat transfer between two silica clusters is investigated by using the nonequilibrium Green's function method. In the gap range between 4 Å and 3 times the cluster size, the thermal conductance decreases as predicted by the surface charge-charge interaction. Above 5 times the cluster size, the volume dipole-dipole interaction predominates. Finally, when the distance becomes smaller than 4 Å, a quantum interaction where the electrons of both clusters are shared takes place. This quantum interaction leads to the dramatic increase of the thermal coupling between neighbor clusters due to strong interactions. This study finally provides a description of the transition between radiation and heat conduction in gaps smaller than a few nanometers.

Thermal transport in hexagonal boron nitride nanoribbons.

The thermal transport properties of hexagonal boron nitride nanoribbons (BNNRs) are investigated. By calculating the phonon spectrum and thermal conductance, it is found that the BNNRs possess excellent thermal transport properties. The thermal conductance of BNNRs can be comparable to that of graphene nanoribbons (GNRs) and even exceed the latter below room temperature. A fitting formula is obtained to describe the features of thermal conductance in BNNRs, which reveals a critical role of the T(1.5) dependence in determining the thermal transport. In addition, an obviously anisotropic thermal transport phenomenon is observed in the nanoribbons. The thermal conductivity of zigzag-edged BNNRs is shown to be about 20% larger than that of armchair-edged nanoribbons at room temperature. The findings indicate that the BNNRs can be applied as important components of excellent thermal devices.