A combination of plasmonic nanoparticles (NPs) with semiconductor photocatalysts, called plasmonic photocatalysts, can be a good candidate for highly efficient photocatalysts using broadband solar light because it can greatly enhance overall photocatalytic efficiency by extending the working wavelength range of light from ultraviolet (UV) to visible. In particular, fixation of plasmonic photocatalysts on a floating porous substrate can have additional advantages for their recycling after water treatment. Here, we report on a floating porous plasmonic photocatalyst based on a polydimethylsiloxane (PDMS)−TiO 2 −gold (Au) composite sponge, in which TiO 2 and Au NPs are simultaneously immobilized on the surface of interconnected pores in the PDMS sponge. This can be easily fabricated by a simple sugar-template method with TiO 2 NPs and in situ reduction of Au NPs by the PDMS without extra chemicals. Its ability to decompose the organic pollutant rhodamine B in water was tested under UV and visible light, respectively. The results showed highly enhanced photocatalytic activity under both UV and visible light compared to the PDMS−TiO 2 sponge and the PDMS−Au sponge. Furthermore, its recyclability was also demonstrated for multiple cycles. The simplicity of fabrication and high photocatalytic performance of our PDMS−TiO 2 −Au sponge can be promising in environmental applications to treat water pollution.
Many crystals grow as banded spherulites from the melt with an optical rhythm indicative of helicoidal twisting. In this work, 23 of 41 charge transfer complexes (CTCs) are grown with twisted morphologies. As a group, CTCs more commonly twist (56%) than molecular crystals arbitrarily chosen in our previous research (31%). To analyze the effect of twisting on charge transport, three tetracyanoethylene-based CTCs with phenanthrene (PhT), pyrene (PyT), and perylene are characterized. PhT and PyT are subject to mobility measurements using organic field-effect transistors. The mobilities for twisted crystals are around three times higher than for crystals with no ostensible optical modulation, which are effectively straight. The differences in mobilities of straight and twisted crystals are considered computationally based on density functional theory. Straight crystal models built from crystallographic information files are calculated and present anisotropic hole and electron transport. For twisted crystal models, adjacent layers in the supercell are rotated by 0.01°around experimentally determined twisting directions. The modified transfer integrals lead to a slight increase (up to 25%) in the calculated mobilities of twisted crystals. Comparisons of model calculations on individual fibrils and measurements of ensembles of fibrils indicate that interfaces between single crystals are likely consequential.
We report the electrical and optical properties of ZnO/ZnS core/shell nanowire (NW) devices. The spatial separation of charge carriers due to their type II band structure together with passivation effect on ZnO/ZnS core/shell NWs not only enhanced their charge carrier transport characteristics by confining the electrons and reducing surface states in the ZnO channel but also increased the photocurrent under ultraviolet (UV) illumination by reducing the recombination probability of the photogenerated charge carriers. Here the efficacy of the type-II band structure and the passivation effect are demonstrated by showing the enhanced subthreshold swing (150 mV/decade) and mobility (17.2 cm2/(Vs)) of the electrical properties, as well as the high responsivity (4.4×10(6) A/W) in the optical properties of the ZnO/ZnS core/shell NWs, compared with the subthreshold swing (464 mV/decade), mobility (8.9 cm2/(Vs)) and responsivity (2.5×10(6) A/W) of ZnO NWs.
Plasmonic metal nanostructures with nanogaps have attracted great interest owing to their controllable optical properties and intense electromagnetic fields that can be useful for a variety of applications, but precise and reliable control of nanogaps in three-dimensional nanostructures remains a great challenge. Here, we report the control of nanojunctions of hollow porous gold nanoshell (HPAuNS) structures by a facile oxygen plasma-etching process and the influence of changes in nanocrevices of the interparticle junction on the optical and sensing characteristics of HPAuNSs. We demonstrate a high tunability of the localized surface plasmon resonance (LSPR) peaks and surface-enhanced Raman scattering (SERS) detection of rhodamine 6G (R6G) using HPAuNS structures with different nanojunctions by varying the degree of gold sintering. As the neck region of the nanojunction is further sintered, the main LSPR peak shifts from 785 to 1350 nm with broadening because the charge transfer plasmon mode becomes more dominant than the dipolar plasmon mode, resulting from the increase of conductance at the interparticle junctions. In addition, it is demonstrated that an increase in the sharpness of the nanojunction neck can enhance the SERS enhancement factor of the HPAuNS by up to 4.8-fold. This enhancement can be ascribed to the more intense local electromagnetic fields at the sharper nanocrevices of interparticle junctions. The delicate change of nanojunction structures in HPAuNSs can significantly affect their optical spectrum and electromagnetic field intensity, which are critical for their practical use in a SERS-based analytical sensor as well as multiple-wavelength compatible applications.
Optoelectronic properties of anisotropic crystals vary with direction requiring that the orientation of molecular organic semiconductor crystals is controlled in optoelectronic device active layers to achieve optimal performance. Here, a generalizable strategy to introduce periodic variations in the out‐of‐plane orientations of 5,11‐bis(triisopropylsilylethynyl)anthradithiophene (TIPS ADT) crystals is presented. TIPS ADT crystallized from the melt in the presence of 16 wt.% polyethylene (PE) forms banded spherulites of crystalline fibrils that twist in concert about the radial growth direction. These spherulites exhibit band‐dependent light absorption, photoluminescence, and Raman scattering depending on the local orientation of crystals. Mueller matrix imaging reveals strong circular extinction (CE), with TIPS ADT banded spherulites exhibiting domains of positive or negative CE signal depending on the crystal twisting sense. Furthermore, orientation‐dependent enhancement in charge injection and extraction in films of twisted TIPS ADT crystals compared to films of straight crystals is visualized in local conductive atomic force microscopy maps. This enhancement leads to 3.3‐ and 6.2‐times larger photocurrents and external quantum efficiencies, respectively, in photodetectors comprising twisted crystals than those comprising straight crystals.
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