Printable Nanocomposite FeS₂–PbS Nanocrystals/Graphene Heterojunction Photodetectors for Broadband Photodetection

Colloidal nanocrystals are attractive materials for optoelectronics applications because they offer a compelling combination of low-cost solution processing, printability, and spectral tunability through the quantum dot size effect. Here we explore a novel nanocomposite photosensitizer consisting of colloidal nanocrystals of FeS₂ and PbS with complementary optical and microstructural properties for broadband photodetection. Using a newly developed ligand exchange to achieve high-efficiency charge transfer across the nanocomposite FeS₂–PbS sensitizer and graphene on the FeS₂–PbS/graphene photoconductors, an extraordinary photoresponsivity in exceeding ∼10⁶ A/W was obtained in an ultrabroad spectrum of ultraviolet (UV)-visible-near-infrared (NIR). This is in contrast to the nearly 3 orders of magnitude reduction of the photoresponsivity from ∼10⁶ A/W at UV to 10³ A/W at NIR on their counterpart of FeS₂/graphene detectors. This illustrates the combined advantages of the nanocomposite sensitizers and the high charge mobility in FeS₂–PbS/graphene van der Waals heterostructures for nanohybrid optoelectronics with high performance, low cost, and scalability for commercialization

Heat-Assisted Inkjet Printing of Tungsten Oxide for High-Performance Ultraviolet Photodetectors

An ammonium metatungstate precursor (WO₃Pr) ink was printed for tungsten oxide (WO₃) UV detectors on SiO₂/Si wafers with prefabricated Au electrodes. A systematic study was carried out on the printing parameters including substrate temperatures in the range of 22–80 °C, WO₃Pr molar concentrations of 0.01, 0.02, and 0.03 M, and printing scan numbers up to 7 to understand their effects on the resulted WO₃ film morphology and optoelectronic properties. It has been found that the printing parameters can sensitively affect the WO₃ film morphology, which in turn impacts the WO₃ photodetector performance. In particular, the printed films experienced a systematic change from discontinuous droplets at below 40 °C to continuous films at 40–60 °C of the substrate temperature. At higher temperatures, the excessive heat from the substrate not only caused drastic evaporation of the printed ink, resulting in highly nonuniform films, but also detrimental heating of the ink in the printer nozzle in proximity of the substrate, preventing continuous printing operation. An optimal printing window of the substrate temperature of 45–55 °C at a molar concentration of 0.02 M of ammonium metatungstate and three printing scans was obtained for the best UV detector performance. A large on/off ratio of 3538 and a high responsivity up to 2.70 A/W at 5 V bias (0.54 A/W·V) represent a significant improvement over the best report of ∼0.28 μA/W·V on WO_<i>X</i> photodetectors, which indicates that the printed WO₃ films are promising for various applications of optoelectronics and sensors

Interface Nanojunction Engineering of Electron-Depleted Tungsten Oxide Nanoparticles for High-Performance Ultraviolet Photodetection

This work reports a general and facile route, i.e., thermal decomposition of a precursor followed by ultrafast thermal annealing (TDP-UTA), to the in situ fabrication of a nanojunction-interlinked tungsten oxide nanoparticle (WO₃-NP) networks for extraordinary ultraviolet (UV) photodetection. TDP leads a spin-coated ammonium metatungstate thin layer to in situ self-assemble into a highly crystalline WO₃-NP mesoporous film on SiO₂/Si substrates with prepatterned electrodes. The as-synthesized WO₃-NPs have dimensions comparable to the Debye length (≈43 nm), which is critical to the optimal electron-depletion effect for high gain in photodetection. UTA creates the NP–NP interface nanojunctions between neighboring WO₃-NPs, which is the key to high-efficiency electron transport with minimized charge recombination in optoelectronic processes. The photodetectors based on such nanojunction-interlinked WO₃-NP networks exhibit a photocurrent-to-dark-current ratio of 5600, the highest value for any WO_<i>x</i>-based photodetectors ever reported. Moreover, the obtained photoresponsivity is up to 139 A/W (or 27.8 A/W·V) upon 360 nm illumination, which is over 1 order of magnitude higher than that of any previously reported WO_<i>x</i>-nanostructure film photodetectors. These results demonstrate that the TDP-UTA route is a low-cost, robust, and scalable pathway to the in situ fabrication of interlinked semiconducting-nanostructure networks for high-performance optoelectronics and sensors