Ultralow Glassy Thermal Conductivity and Controllable, Promising Thermoelectric Properties in Crystalline o-CsCu5S3.

We thoroughly investigated the anharmonic lattice dynamics and microscopic mechanisms of the thermal and electronic transport characteristics in orthorhombic o-CsCu5S3 at the atomic level. Taking into account the phonon energy shifts and the wave-like tunneling phonon channel, we predict an ultralow κL of 0.42 w/mK at 300 K with an extremely weak temperature dependence following ∼T-0.33. These findings agree well with experimental values along with the parallel to the Bridgman growth direction. The κL in o-CsCu5S3 is suppressed down to the amorphous limit, primarily due to the unconventional Cu-S bonding induced by the p-d hybridization antibonding state coupled with the stochastic oscillation of Cs atoms. The nonstandard temperature dependence of κL can be traced back to the critical or dominant role of wave-like tunneling of phonon contributions in thermal transport. Moreover, the p-d hybridization of Cu(3)-S bonding results in the formation of a valence band with "pudding-mold" and high-degeneracy valleys, ensuring highly efficient electron transport characteristics. By properly adjusting the carrier concentration, excellent thermoelectric performance is achieved with a maximum thermoelectric conversion efficiency of 18.4% observed at 800 K in p-type o-CsCu5S3. Our work not only elucidates the anomalous electronic and thermal transport behavior in the copper-based chalcogenide o-CsCu5S3 but also provides insights for manipulating its thermal and electronic properties for potential thermoelectric applications.

High-throughput identification of spin-photon interfaces in silicon.

Color centers in host semiconductors are prime candidates as spin-photon interfaces for quantum applications. Finding an optimal spin-photon interface in silicon would move quantum information technologies toward a mature semiconducting host. However, the space of possible charged defects is vast, making the identification of candidates from experiments alone extremely challenging. Here, we use high-throughput first-principles computational screening to identify spin-photon interfaces among more than 1000 charged defects in silicon. The use of a single-shot hybrid functional approach is critical in enabling the screening of many quantum defects with a reasonable accuracy. We identify three promising spin-photon interfaces as potential bright emitters in the telecom band: [Formula: see text], [Formula: see text], and [Formula: see text]. These candidates are excited through defect-bound excitons, stressing the importance of such defects in silicon for telecom band operations. Our work paves the way to further large-scale computational screening for quantum defects in semiconductors.

A Highly Transparent Photo-Electro-Thermal Film with Broadband Selectivity for All-Day Anti-/De-Icing.

A photo- and electro-thermal film can convert sunlight and electricity into heat to solve icing problems. Combination of them provides an efficient strategy for all-day anti-/de-icing. However, only opaque surfaces have been reported, due to the mutual exclusiveness between photon absorption and transmission. Herein, a highly transparent and scalable solution-processed photo-electro-thermal film is reported, which exhibits an ultra-broadband selective spectrum to separate the visible light from sunlight and a countertrend suppress of emission in longer wavelength. It absorbs ≈ 85% of invisible sunlight (ultraviolet and near-infrared) for light-heat conversion, meanwhile maintains luminous transmittance > 70%. The reflection of mid-infrared leads to low emissivity (0.41), which further preserves heat on the surface for anti-/de-icing purpose. This ultra-broadband selectivity enables temperature elevation > 40 °C under 1-sun illumination and the mutual support between photo-thermal and electro-thermal effects contributes to > 50% saving of electrical consumption under weak solar exposure (0.4-sun) for maintaining unfrozen surfaces at -35 °C environment. The reverberation from photo-electro-thermal and super-hydrophobic effects illustrates a lubricating removal of grown ice in short time (< 120 s). The self-cleaning ability and the durability under mechanical, electrical, optical, and thermal stresses render the film stable for long-term usage in all-day anti-/de-icing applications.

Experimental Evidence of Superdiffusive Thermal Transport in Si0.4Ge0.6 Thin Films.

Superdiffusive thermal transport represents a unique phenomenon in heat conduction, which is characterized by a size (L) dependence of thermal conductivity (κ) in the form of κ ∝ Lß with a constant ß between 0 and 1. Although superdiffusive thermal transport has been theoretically predicted for SiGe alloys, direct experimental evidence is still lacking. Here, we report on a systematic experimental study of the thickness-dependent thermal conductivity of Si0.4Ge0.6 thin films grown by molecular beam epitaxy. The cross-plane thermal conductivity of Si0.4Ge0.6 thin films spanning a thickness range from 20 to 1120 nm was measured in the temperature range 120-320 K via a differential three-omega method. Results show that the thermal conductivity follows a consistent κ ∝ t0.26 power law with the film thickness (t) at different temperatures, providing direct experimental evidence that alloy-scattering dominated thermal transport in SiGe is superdiffusive.

Self-Protecting Aqueous Lithium-Ion Batteries.

Capacity degradation and destructive hazards are two major challenges for the operation of lithium-ion batteries at high temperatures. Although adding flame retardants or fire extinguishing agents can provide one-off self-protection in case of emergency overheating, it is desirable to directly regulate battery operation according to the temperature. Herein, smart self-protecting aqueous lithium-ion batteries are developed using thermos-responsive separators prepared through in situ polymerization on the hydrophilic separator. The thermos-responsive separator blocks the lithium ion transport channels at high temperature and reopens when the battery cools down; more importantly, this transition is reversible. The influence of lithium salts on the thermos-responsive behaviors of the hydrogels is investigated. Then suitable lithium salt (LiNO3 ) and concentration (1 m) are selected in the electrolyte to achieve self-protection without sacrificing battery performance. The shut-off temperature can be tuned from 30 to 80 °C by adjusting the hydrophilic and hydrophobic moiety ratio in the hydrogel for targeted applications. This self-protecting LiMn2 O4 /carbon coated LiTi2 (PO4 )3 (LMO/C-LTP) battery shows promise for smart energy storage devices with high safety and extended lifespan in case of high operating temperatures.

Novel insights into lattice thermal transport in nanocrystalline Mg3Sb2 from first principles: the crucial role of higher-order phonon scattering.

Zintl phase Mg3Sb2, which has ultra-low thermal conductivity, is a promising anisotropic thermoelectric material. It is worth noting that the prediction and experiment value of lattice thermal conductivity (κ) maintain a remarkable difference, troubling the development and application. Thus, we firstly included the four-phonon scattering processes effect and performed the Peierls-Boltzmann transport equation (PBTE) combined with the first-principles lattice dynamics to study the lattice thermal transport in Mg3Sb2. The results showed that our theoretically predicted κ is consistent with the experimentally measured, breaking through the limitations of the traditional calculation methods. The prominent four-phonon scatterings decreased phonon lifetime, leading to the κ of Mg3Sb2 at 300 K from 2.45 (2.58) W m-1 K-1 to 1.94 (2.19) W m-1 K-1 along the in (cross)-plane directions, respectively, and calculation accuracy increased by 20%. This study successfully explains the lattice thermal transport behind mechanism in Mg3Sb2 and implies guidance to advance the prediction accuracy of thermoelectric materials.

A Solution-Processed Inorganic Emitter with High Spectral Selectivity for Efficient Subambient Radiative Cooling in Hot Humid Climates.

Daytime radiative cooling provides an eco-friendly solution to space cooling with zero energy consumption. Despite significant advances, most state-of-the-art radiative coolers show broadband infrared emission with low spectral selectivity, which limits their cooling temperatures, especially in hot humid regions. Here, an all-inorganic narrowband emitter comprising a solution-derived SiOx Ny layer sandwiched between a reflective substrate and a self-assembly monolayer of SiO2 microspheres is reported. It shows a high and diffusive solar reflectance (96.4%) and strong infrared-selective emittance (94.6%) with superior spectral selectivity (1.46). Remarkable subambient cooling of up to 5 °C in autumn and 2.5 °C in summer are achieved under high humidity without any solar shading or convection cover at noontime in a subtropical coastal city, Hong Kong. Owing to the all-inorganic hydrophobic structure, the emitter shows outstanding resistance to ultraviolet and water in long-term durability tests. The scalable-solution-based fabrication renders this stable high-performance emitter promising for large-scale deployment in various climates.

Giant and bidirectionally tunable thermopower in nonaqueous ionogels enabled by selective ion doping.

Ionic thermoelectrics show great potential in thermal sensing owing to their ultrahigh thermopower, low cost, and ease in production. However, the lack of effective n-type ionic thermoelectric materials seriously hinders their applications. Here, we report giant and bidirectionally tunable thermopowers within an ultrawide range from −15 to +17 mV K−1 in solid ionic liquid­based ionogels. Particularly, a record high negative thermopower of −15 mV K−1 is achieved in the ternary ionogel, rendering it among the best n-type ionic thermoelectric materials under the same condition. A thermopower regulation strategy through ion doping to selectively induce ion aggregates to enhance ion-ion interactions is proposed. These selective ion interactions are found to be decisive in modulating the sign and magnitude of the thermopower in the ionogels. A prototype wearable device integrated with 12 p-n pairs is demonstrated with a total thermopower of 0.358 V K−1, showing promise for ultrasensitive thermal detection.