Inorganic lead halide perovskite nanocrystals (NCs) have attracted great interest owing to their superior luminescence and optoelectronic properties. In comparison to cubic CsPbX3 (X = Cl, Br, or I) that has visible luminescence, trigonal Cs4PbX6 has a much larger bandgap and distinct optical properties. Little has been known about the luminescence properties of the Cs4PbX6 NCs. In this study, we synthesize the well-crystallized Cs4PbCl6 NCs with sizes of 2.2–11.8 nm, which exhibit stable and near-UV luminescence (with a lifetime of 19.7–24.2 ns) with a remarkable quantum confinement effect at room temperature. In comparison to the negligible Stokes shift in the CsPbCl3 NCs, the Stokes shift of the Cs4PbCl6 NCs is very large (0.91 eV). The experimental results in combination with the first-principles calculations reveal that the near-UV luminescence of the Cs4PbCl6 NCs stems from the Frenkel excitons self-trapped in the isolated PbCl64– octahedrons. This is different from the CsPbCl3 NCs whose luminescence originates from the free Wannier excitons. The theoretical model based on the lattice relaxation is proposed to account for the large Stokes shift and its abnormal decrease with the decreasing particle size.

Effect of elemental composition and size on electron confinement in self-assembled SiC quantum dots: A combinatorial approach

Our understanding of crystal growth mechanisms has changed deeply in the past few decades. Particularly, the oriented attachment of intermediate nanoparticles has been accepted to be a crucial crystal growth mechanism that is distinct from the traditional one involving nucleation and Ostwald ripening. However the details of the oriented attachment process are not readily observed experimentally, and little is known about the driving force and the dynamics involved in oriented attachment. In this respect, ZnO is an ideal material because it possesses strong spontaneous polarization which may easily drive oriented attachment during its crystal growth. We study experimentally and theoretically the complete crystal growth process (from primitive amorphous nanoclusters to ultimate single nanocrystals) of one-dimensional ZnO nanocrystals growing in water/ethanol at high temperatures. The results reveal that both axial (along the direction of the polarization axis) and lateral oriented attachment of the intermediates occurs during the growth process of the one-dimensional ZnO nanocrystals. Calculation based on the force and interaction model reveals that the axial oriented attachment driven by the spontaneous polarization force dominates the crystal growth of ZnO nanocrystals, and the van der Waals force also plays a role in driving oriented attachment. The study shows that oriented attachment of intermediate nanoparticle ensembles induces formation of the symmetric twin-nanorods. These results improve our understanding of the growth mechanism of nanocrystals in a liquid medium.

The quantum confinement effect is one of the crucial physical effects that discriminate a quantum material from its bulk material. It remains a mystery why the 6H-SiC quantum dots (QDs) do not exhibit an obvious quantum confinement effect. We study the photoluminescence of the coupled colloidal system of SiC QDs and Ag nanoparticles. The experimental result in conjunction with the theoretical calculation reveals that there is strong coupling between the localized electron-hole pair in the SiC QD and the localized surface plasmon in the Ag nanoparticle. It results in resonance energy transfer between them and resultant quenching of the blue surface-defect luminescence of the SiC QDs, leading to uncovering of a hidden near-UV emission band. This study shows that this emission band originates from the interband transition of the 6H-SiC QDs and it exhibits a remarkable quantum confinement effect.

People know little experimentally about the physical properties of the SiC nanoclusters with sizes of a couple of angstroms. Herein, we study the electronic structure and light absorption/emission properties of the SiC nanoclusters with an average diameter of 7 Å that are fabricated by diminishing the sizes of the SiC microcrystals under high pressure and high temperature. The results reveal that the SiC nanoclusters have an indirect energy gap of 5.1 eV. Unlike the case of larger SiC nanocrystals, the luminescence of the SiC nanoclusters is dominated by two types of oxygen-related surface defects, and the maximum of their photoluminescence/photoluminescence excitation spectrum lies at 4.1/3.3 and 3.8/3.0 eV, respectively. The energy gap of the SiC nanoparticles with reference to bulk value is found to be inversely proportional to the diameter to the power 0.97, which shows slower increase of energy gap with decreasing size than what is predicted by using the first-principles calculations.

Directly linearly polarized light emission from organic light‐emitting diodes (OLEDs), as an important functional expansion, is an intriguing and attractive research topic due to its increasing importance in various applications. Until now, however, the limited efficiency and inadequate polarization ratio constitute two major hurdles for real application. In this work, high‐efficiency linearly polarized white OLEDs with an ultrahigh polarization ratio are achieved by using integrated dielectric/metal nanograting and nanorelief speckle image holography metasurfaces. In the devices, the integrated grating behave as a polarizer to select the transverse magnetic wave (TM) component and simultaneously reflect the transverse electric wave (TE) counterpart over the whole emission spectrum, while the metasurfaces gather the otherwise waste TE‐polarized light reflected by the grating and transform it into reusable TM‐polarized light. This synergistic energy‐light recycling system leads to dramatically boosted device efficiency and polarization ratio, i.e., a power efficiency 21.4 lm W−1 (@ 1000 cd m−2), and an extinction ratio of 17.8 dB (@ V = 5 V) for the polarized white OLEDs. The presented paradigm for simultaneous polarization controlling and efficiency boosting in white OLEDs is expected to advance the OLED techniques in device reconfigurability for future multifunctional applications.

All-day passive radiative cooling has recently attracted broader attention for its potential as a viable energy technology. Although tremendous progress has been achieved, the design and fabrication of low-cost high-efficiency radiators for all-day passive radiative cooling remains a challenge. Herein, we report a new type of flexible composite radiator film with built-in artificial opal-like structures for all-day passive radiative cooling. Using artificial opal structure concepts, the proposed polydimethylsiloxane (PDMS) radiator film with embedded polystyrene (PS) microsphere photonic crystals exhibits a sufficiently high solar reflectance of ∼92.7% when in a direct sunlight region, and a thermal emittance of ∼93.6% within the atmospheric window. Without the need for traditional reflectors like silver or aluminum foils, this composite film realizes subambient temperature reduction of ∼4.8 °C in direct sunlight and ∼8.5 °C during the night. This work provides a new fabrication approach for the low-cost production of structural polymer films for high performance and potential real word applications.

No abstract