Near-Complete Suppression of NIR-II Luminescence Quenching in Halide Double Perovskites for Surface Functionalization Through Facet Engineering.

Lanthanide-based NIR-II-emitting materials (1000-1700 nm) show promise for optoelectronic devices, phototherapy, and bioimaging. However, one major bottleneck to prevent their widespread use lies in low quantum efficiencies, which are significantly constrained by various quenching effects. Here, a highly oriented (222) facet is achieved via facet engineering for Cs2NaErCl6 double perovskites, enabling near-complete suppression of NIR-II luminescence quenching. The optimally (222)-oriented Cs2Ag0.10Na0.90ErCl6 microcrystals emit Er3+ 1540 nm light with unprecedented high quantum efficiencies of 90 ± 6% under 379 nm UV excitation (ultralarge Stokes shift >1000 nm), and a record near-unity quantum yield of 98.6% is also obtained for (222)-based Cs2NaYb0.40Er0.60Cl6 microcrystallites under 980 nm excitation. With combined experimental and theoretical studies, the underlying mechanism of facet-dependent Er3+ 1540 nm emissions is revealed, which can contribute to surface asymmetry-induced breakdown of parity-forbidden transition and suppression of undesired non-radiative processes. Further, the role of surface quenching is reexamined by molecular dynamics based on two facets, highlighting the drastic two-phonon coupling effect of a hydroxyl group to 4I13/2 level of Er3+. Surface-functionalized facets will provide new insights for tunable luminescence in double perovskites, and open up a new avenue for developing highly efficient NIR-II emitters toward broad applications.

Lead-Free Double Perovskite Cs2NaErCl6: Li+ as High-Stability Anodes for Li-Ion Batteries.

Halide perovskite materials have been used in the field of lithium-ion batteries because of their excellent ion migration characteristics and defect tolerance. However, the current lead-based perovskites used for lithium-ion batteries are highly toxic, which may hinder the pace of further commercialization. Therefore, it is still necessary to develop a new type of stable and pollution-free perovskite anode material. Herein, we for the first time use a high-concentration lithium-ion doped rare-earth-based double perovskite Cs2NaErCl6:Li+ as the negative electrode material for a lithium-ion battery. Thanks to its excellent structure stability, the assembled battery also has high cycle stability, with a specific capacity of 120 mAh g-1 at 300 mA g-1 after 500 cycles with a Coulomb efficiency of nearly 100%. The introduction of a rare earth element in a lead-free double perovskite paves a new way for the development of novel promising anode materials in the field of lithium storage applications.

NaCl substrates for high temperature processing and transfer of ultrathin materials.

Ultrathin materials often require high temperatures for growth and processing, which cannot be withstood by the substrate underneath. For example, polymers are widely used as a supporting layer but unfortunately have low strain-point temperatures. This is the case of polyethylene terephthalate (PET) which has glass transition and melting temperatures of 76 and 250 °C, respectively. In this paper we propose to use polished salt, a material that can withstand high temperatures during fabrication and, at the same time, can be sacrificed during the transfer onto the final substrates. More specifically, we demonstrate thermal dewetting of Au ultrathin metal films and growth of MoS2 on NaCl at 750 and 650 °C, respectively, and subsequent transfer onto PET films, after which the salt is easily dissolved by water. We believe that the proposed technique can be extended to fabrication of other ultrathin materials, e.g. graphene, as well as final substrates for a wide range of applications, including flexible electronic and optoelectronic devices.

The synthesis of a perovskite CsPbBr3 quantum dot superlattice in borosilicate glass.

For the first-time we have synthesised perovskite CsPbBr3 quantum dot (QD) superlattices in borosilicate glass, which play a key role in controllable network structure connectivity. The structural and optical properties of the CsPbBr3 QD superlattices embedded in borosilicate glass were investigated.

Large-area, flexible imaging arrays constructed by light-charge organic memories.

Existing organic imaging circuits, which offer attractive benefits of light weight, low cost and flexibility, are exclusively based on phototransistor or photodiode arrays. One shortcoming of these photo-sensors is that the light signal should keep invariant throughout the whole pixel-addressing and reading process. As a feasible solution, we synthesized a new charge storage molecule and embedded it into a device, which we call light-charge organic memory (LCOM). In LCOM, the functionalities of photo-sensor and non-volatile memory are integrated. Thanks to the deliberate engineering of electronic structure and self-organization process at the interface, 92% of the stored charges, which are linearly controlled by the quantity of light, retain after 20000 s. The stored charges can also be non-destructively read and erased by a simple voltage program. These results pave the way to large-area, flexible imaging circuits and demonstrate a bright future of small molecular materials in non-volatile memory.

Two-stage metal-catalyst-free growth of high-quality polycrystalline graphene films on silicon nitride substrates.

By using two-stage, metal-catalyst-free chemical vapor deposition (CVD), it is demonstrated that high-quality polycrystalline graphene films can directly grow on silicon nitride substrates. The carrier mobility can reach about 1500 cm(2) V(-1) s(-1) , which is about three times the value of those grown on SiO(2) /Si substrates, and also is better than some examples of metal-catalyzed graphene, reflecting the good quality of the graphene lattice.

Multilayer graphene-coated atomic force microscopy tips for molecular junctions.

Multilayer graphene tips are developed for conducting probe atomic force microscopy for the formation of molecular junctions. Molecular junctions using graphene tips show very small tip-to-tip variance, excellent operational stability, good endurance, and long shelf-life. These properties, together with high yield and the simple processing involved, suggest that commercial mass-production of graphene tips is viable for molecular electronic applications.

Quantitative analysis of the role of the first layer in p- and n-type organic field-effect transistors with graphene electrodes.

Efficient field-effect mobilities measured from both p- and n-type organic monolayer field-effect transistors that utilize graphene electrodes permit quantitative analysis of the role of the first layer. Information about the relationship between the kinetics of the diffusion process and film morphology of the first layer during the increasing substrate temperature, and correlations of field-effect mobilities of the first monolayer and the substrate temperature is obtained.

Inkjet printing high-resolution, large-area graphene patterns by coffee-ring lithography.

Taking advantage of the "coffee-ring" effect, graphene electrodes with channel lengths as low as 1-2 micrometers are patterned by inkjet printing. Organic thin film transistors and complementary inverters are also fabricated using these graphene electrodes and show excellent performance.

Oxygen-aided synthesis of polycrystalline graphene on silicon dioxide substrates.

We report the metal-catalyst-free synthesis of high-quality polycrystalline graphene on dielectric substrates [silicon dioxide (SiO(2)) or quartz] using an oxygen-aided chemical vapor deposition (CVD) process. The growth was carried out using a CVD system at atmospheric pressure. After high-temperature activation of the growth substrates in air, high-quality polycrystalline graphene is subsequently grown on SiO(2) by utilizing the oxygen-based nucleation sites. The growth mechanism is analogous to that of growth for single-walled carbon nanotubes. Graphene-modified SiO(2) substrates can be directly used in transparent conducting films and field-effect devices. The carrier mobilities are about 531 cm(2) V(-1) s(-1) in air and 472 cm(2) V(-1) s(-1) in N(2), which are close to that of metal-catalyzed polycrystalline graphene. The method avoids the need for either a metal catalyst or a complicated and skilled postgrowth transfer process and is compatible with current silicon processing techniques.

Recent progress in n-channel organic thin-film transistors.

Particular attention has been focused on n-channel organic thin-film transistors (OTFTs) during the last few years, and the potentially cost-effective circuitry-based applications in flexible electronics, such as flexible radiofrequency identity tags, smart labels, and simple displays, will benefit from this fast development. This article reviews recent progress in performance and molecular design of n-channel semiconductors in the past five years, and limitations and practicable solutions for n-channel OTFTs are dealt with from the viewpoint of OTFT constitution and geometry, molecular design, and thin-film growth conditions. Strategy methodology is especially highlighted with an aim to investigate basic issues in this field.

Effect of dielectric layers on device stability of pentacene-based field-effect transistors.

We report stable organic field-effect transistors (OFETs) based on pentacene. It was found that device stability strongly depends on the dielectric layer. Pentacene thin-film transistors based on the bare or polystyrene-modified SiO(2) gate dielectrics exhibit excellent electrical stabilities. In contrast, the devices with the octadecyltrichlorosilane (OTS)-treated SiO(2) dielectric layer showed the worst stabilities. The effects of the different dielectrics on the device stabilities were investigated. We found that the surface energy of the gate dielectric plays a crucial role in determining the stability of the pentacene thin film, device performance and degradation of electrical properties. Pentacene aggregation, phase transfer and film morphology are also important factors that influence the device stability of pentacene devices. As a result of the surface energy mismatch between the dielectric layer and organic semiconductor, the electronic performance was degraded. Moreover, when pentacene was deposited on the OTS-treated SiO(2) dielectric layer with very low surface energy, pentacene aggregation occurred and resulted in a dramatic decrease of device performance. These results demonstrated that the stable OFETs could be obtained by using pentacene as a semiconductor layer.

Fused-ring pyrazine derivatives for n-type field-effect transistors.

Three new fused-ring pyrazine derivatives end-functionalized with trifluoromethylphenyl groups have been synthesized. The effect of a fused-ring pyrazine core on the thermal, electronic, optical, thin film morphology, and organic field-effect transistor (OFET) properties was investigated both experimentally and theoretically. Electrochemistry measurements and density functional theory calculations suggest that the pyrazine core plays a significant role in tuning the electron affinities of these compounds. The optical absorption and fluorescence properties are also sensitive to the pyrazine core. The OFET devices based on the fused-ring pyrazine compounds exhibit electron mobilities as high as ca. 0.03 cm(2) V(-1) s(-1) under nitrogen, and their performance is sensitive to the pyrazine core. The larger pyrazine core leads to a lower LUMO level and lower reorganization energy, to more ordered thin film morphology with larger grain size, and finally to higher mobilities.

Bulky 4-tritylphenylethynyl substituted boradiazaindacene: pure red emission, relatively large Stokes shift and inhibition of self-quenching.

Bulky 4-tritylphenylethynyl substituted boradiazaindacene with pure red emission, relatively large Stokes shift, high fluorescence quantum yield, and low self-quenching was efficiently synthesized and qualified as a potential EL dopant.