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            Broadband photodetectors (PDs) have great applications in both industrial and scientific sectors. In this study, solution-processed broadband PDs with an “inverted” vertical photodiode device structure without incorporating transparent conductive oxides electrodes, fabricated by bulk heterojunction (BHJ) composites composed of a low optical gap conjugated polymer blended with highly electrically conductive PbS quantum dots (QDs), operated at room temperature, are reported. The low optical gap conjugated polymer incorporated with PbS QDs contributes to the spectral response from the ultraviolet (UV)-visible to the infrared (IR) range. To realize the IR spectral response and to circumvent the weak IR transparency of the transparent oxide electrodes, the implementation of a photodiode with an “inverted” vertical device structure with the Au anode and the Ba/Al bilayer semitransparent cathode passivated with the MgF 2 layer is demonstrated. Photoinduced charge carrier transfer occurring within the BHJ composite gave rise to decent photocurrent, resulting in detectivities greater than 10 12 Jones (cm Hz 1/2 /W) over the wavelength from the UV-visible to the IR range under low applied bias. Thus, our findings of the utilization of the BHJ composites and an “inverted” vertical photodiode without the incorporation of the transparent conductive oxide electrodes provide a facile way to realize broadband PDs.more » « less
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            Abstract Halide perovskites show ubiquitous presences in growing fields at both fundamental and applied levels. Discovery, investigation, and application of innovative perovskites are heavily dependent on the synthetic methodology in terms of time-/yield-/effort-/energy- efficiency. Conventional wet chemistry method provides the easiness for growing thin film samples, but represents as an inefficient way for bulk crystal synthesis. To overcome these, here we report a universal solid state-based route for synthesizing high-quality perovskites, by means of simultaneously applying both electric and mechanical stress fields during the synthesis, i.e., the electrical and mechanical field-assisted sintering technique. We employ various perovskite compositions and arbitrary geometric designs for demonstration in this report, and establish such synthetic route with uniqueness of ultrahigh yield, fast processing and solvent-free nature, along with bulk products of exceptional quality approaching to single crystals. We exemplify the applications of the as-synthesized perovskites in photodetection and thermoelectric as well as other potentials to open extra chapters for future technical development.more » « less
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            Future advancements in three-dimensional (3D) electronics require robust thermal management methodology. Thermoelectric coolers (TECs) are reliable and solid-state heat pumping devices with high cooling capacity that can meet the requirements of emerging 3D microelectronic devices. Here, we first provide the design of TECs for electronics cooling using a computational model and then experimentally validate the main predictions. Key device parameters such as device thickness, leg density, and contact resistance were studied to understand their influence on the performance of TECs. Our results show that it is possible to achieve high cooling power density through optimization of TE leg height and packing density. Scaling of TECs is shown to provide ultra-high cooling power density.more » « less
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            Conjugated molecules have been typically utilized as either hole or electron extraction layers to boost the device performance of perovskite solar cells (PSCs), formed from three-dimensional (3D) perovskites, due to their high charge carrier mobility and electrical conductivity. However, the passivating role of conjugated molecules in creating two-dimensional (2D) perovskites has rarely been reported. In this study, we report novel conjugated aniline 3-phenyl-2-propen-1-amine (PPA) based 2D perovskites and further demonstrate efficient and stable PSCs containing a (PPA) x (MAPbI 3 ) 1− x /MAPbI 3 bilayer thin film (where MA is CH 3 NH 3 + ). The (PPA) x (MAPbI 3 ) 1− x /MAPbI 3 bilayer thin film possesses superior crystallinity and passivated trap states, resulting in enhanced charge transport and suppressed charge carrier recombination compared to those of a 3D MAPbI 3 thin film. As a result, PSCs containing the (PPA) x (MAPbI 3 ) 1− x /MAPbI 3 bilayer thin film exhibit a power conversion efficiency (PCE) of 21.98%, which is approximately a 25% enhancement compared to that of the MAPbI 3 thin film. Moreover, un-encapsulated PSCs containing the (PPA) x (MAPbI 3 ) 1− x /MAPbI 3 bilayer thin film retain 50% of their initial PCE after 1200 hours in an ambient atmosphere (25 °C, and 30 ± 10 humidity), whereas PSCs with the 3D MAPbI 3 thin film show significant degradation after 100 hours and a degradation of more than 50% of their original PCE after 500 hours. These results demonstrate that the incorporation of conjugated molecules as organic spacer cations to create 2D perovskites on top of 3D perovskites is an effective way to approach high-performance PSCs.more » « less
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