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1. All‐Printed Ultrahigh‐Responsivity MoS ₂ Nanosheet Photodetectors Enabled by Megasonic Exfoliation

   https://doi.org/10.1002/adma.202203772  

   Kuo, Lidia; Sangwan, Vinod_K; Rangnekar, Sonal_V; Chu, Ting‐Ching; Lam, David; Zhu, Zhehao; Richter, Lee_J; Li, Ruipeng; Szydłowska, Beata_M; Downing, Julia_R; et al (July 2022, Advanced Materials)

   Abstract Printed 2D materials, derived from solution‐processed inks, offer scalable and cost‐effective routes to mechanically flexible optoelectronics. With micrometer‐scale control and broad processing latitude, aerosol‐jet printing (AJP) is of particular interest for all‐printed circuits and systems. Here, AJP is utilized to achieve ultrahigh‐responsivity photodetectors consisting of well‐aligned, percolating networks of semiconducting MoS₂nanosheets and graphene electrodes on flexible polyimide substrates. Ultrathin (≈1.2 nm thick) and high‐aspect‐ratio (≈1 μm lateral size) MoS₂nanosheets are obtained by electrochemical intercalation followed by megasonic atomization during AJP, which not only aerosolizes the inks but also further exfoliates the nanosheets. The incorporation of the high‐boiling‐point solvent terpineol into the MoS₂ink is critical for achieving a highly aligned and flat thin‐film morphology following AJP as confirmed by grazing‐incidence wide‐angle X‐ray scattering and atomic force microscopy. Following AJP, curing is achieved with photonic annealing, which yields quasi‐ohmic contacts and photoactive channels with responsivities exceeding 10³ A W⁻¹that outperform previously reported all‐printed visible‐light photodetectors by over three orders of magnitude. Megasonic exfoliation coupled with properly designed AJP ink formulations enables the superlative optoelectronic properties of ultrathin MoS₂nanosheets to be preserved and exploited for the scalable additive manufacturing of mechanically flexible optoelectronics. 

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2. Cascade synthesis and optoelectronic applications of intermediate bandgap Cu3VSe4 nanosheets

   https://doi.org/10.1038/s41598-020-78649-9  

   Liu, Mimi; Lai, Cheng-Yu; Zhang, Meng; Radu, Daniela R. (December 2020, Scientific Reports)

   Abstract Two-dimensional (2D) ternary materials recently generated interest in optoelectronics and energy-related applications, alongside their binary counterparts. To date, only a few naturally occurring layered 2D ternary materials have been explored. The plethora of benefits owed to reduced dimensionality prompted exploration of expanding non-layered ternary chalcogenides into the 2D realm. This work presents a templating method that uses 2D transition metal dichalcogenides as initiators to be converted into the corresponding ternary chalcogenide upon addition of copper, via a solution-phase synthesis, conducted in high boiling point solvents. The process starts with preparation of VSe₂nanosheets, which are next converted into Cu₃VSe₄sulvanite nanosheets (NSs) which retain the 2D geometry while presenting an X-ray diffraction pattern identical with the one for the bulk Cu₃VSe₄. Both the scanning electron microscopy and transmission microscopy electron microscopy show the presence of quasi-2D morphology. Recent studies of the sulfur-containing sulvanite Cu₃VS₄highlight the presence of an intermediate bandgap, associated with enhanced photovoltaic (PV) performance. The Cu₃VSe₄nanosheets reported herein exhibit multiple UV–Vis absorption peaks, related to the intermediate bandgaps similar to Cu₃VS₄and Cu₃VSe₄nanocrystals. To test the potential of Cu₃VSe₄NSs as an absorber for solar photovoltaic devices, Cu₃VSe₄NSs thin-films deposited on FTO were subjected to photoelectrochemical testing, showing p-type behavior and stable photocurrents of up to ~ 0.036 mA/cm². The photocurrent shows a ninefold increase in comparison to reported performance of Cu₃VSe₄nanocrystals. This proves that quasi-2D sulvanite nanosheets are amenable to thin-film deposition and could show superior PV performance in comparison to nanocrystal thin-films. The obtained electrical impedance spectroscopy signal of the Cu₃VSe₄ NSs-FTO based electrochemical cell fits an equivalent circuit with the circuit elements of solution resistance (R_s), charge-transfer resistance (R_ct), double-layer capacitance (C_dl), and Warburg impedance (W). The estimated charge transfer resistance value of 300 Ω cm²obtained from the Nyquist plot provides an insight into the rate of charge transfer on the electrode/electrolyte interface. 

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3. Ultrathin Bi ₂ O ₂ S nanosheet near-infrared photodetectors

   https://doi.org/10.1039/D0NR02991B  

   Chitara, Basant; Limbu, Tej B.; Orlando, Jason D.; Tang, Yongan; Yan, Fei (January 2020, Nanoscale)

   Recently, a zipper two-dimensional (2D) material Bi 2 O 2 Se belonging to the layered bismuth oxychalcogenide (Bi 2 O 2 X: X = S, Se, Te) family, has emerged as an alternate candidate to van der Waals 2D materials for high-performance electronic and optoelectronic applications. This hints towards exploring the other members of the Bi 2 O 2 X family for their true potential and bismuth oxysulfide (Bi 2 O 2 S) could be the next member for such applications. Here, we demonstrate for the first time, the scalable room-temperature chemical synthesis and near-infrared (NIR) photodetection of ultrathin Bi 2 O 2 S nanosheets. The thickness of the freestanding nanosheets was around 2–3 nm with a lateral dimension of ∼80–100 nm. A solution-processed NIR photodetector was fabricated from ultrathin Bi 2 O 2 S nanosheets. The photodetector showed high performance, under 785 nm laser illumination, with a photoresponsivity of 4 A W −1 , an external quantum efficiency of 630%, and a normalized photocurrent-to-dark-current ratio of 1.3 × 10 10 per watt with a fast response time of 100 ms. Taken together, the findings suggest that Bi 2 O 2 S nanosheets could be a promising alternative 2D material for next-generation large-area flexible electronic and optoelectronic devices. 

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4. Solution‐Processed Flexible Broadband Photodetectors with Solution‐Processed Transparent Polymeric Electrode

   https://doi.org/10.1002/adfm.201909487  

   Zhu, Tao; Yang, Yongrui; Zheng, Luyao; Liu, Lei; Becker, Matthew_L; Gong, Xiong (February 2020, Advanced Functional Materials)

   Abstract Room‐temperature solution‐processed flexible photodetectors with spectral response from 300 to 2600 nm are reported. Solution‐processed polymeric thin film with transparency ranging from 300 to 7000 nm and superior electrical conductivity as the transparent electrode is reported. Solution‐processed flexible broadband photodetectors with a “vertical” device structure incorporating a perovskite/PbSe quantum dot bilayer thin film based on the above solution‐processed transparent polymeric electrode are demonstrated. The utilization of perovskite/PbSe quantum dot bilayer thin film as the photoactive layer extends spectral response to infrared region and boosts photocurrent densities in both visible and infrared regions through the trap‐assisted photomultiplication effect. Operated at room temperature and under an external bias of ‐1 V, the solution‐processed flexible photodetectors exhibit over 230 mA W^‐1responsivity, over 1011 cm Hz1/2/W photodetectivity from 300 to 2600 nm and ≈70 dB linear dynamic ranges. It is also found that the solution‐processed flexible broadband photodetectors exhibit fast response time and excellent flexibility. All these results demonstrate that this work develop a facile approach to realize room‐temperature operated ultrasensitive solution‐processed flexible broadband photodetectors with “vertical” device structure through solution‐processed transparent polymeric electrode. 

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5. High broadband photoconductivity of few-layered MoS ₂ field-effect transistors measured using multi-terminal methods: effects of contact resistance

   https://doi.org/10.1039/D0NR07311C  

   Das, Priyanka; Nash, Jawnaye; Webb, Micah; Burns, Raelyn; Mapara, Varun N.; Ghimire, Govinda; Rosenmann, Daniel; Divan, Ralu; Karaiskaj, Denis; McGill, Stephen A.; et al (January 2020, Nanoscale)

   null (Ed.)

   Among the layered two dimensional semiconductors, molybdenum disulfide (MoS 2 ) is considered to be an excellent candidate for applications in optoelectronics and integrated circuits due to its layer-dependent tunable bandgap in the visible region, high ON/OFF current ratio in field-effect transistors (FET) and strong light–matter interaction properties. In this study, using multi-terminal measurements, we report high broadband photocurrent response ( R ) and external quantum efficiency (EQE) of few-atomic layered MoS 2 phototransistors fabricated on a SiO 2 dielectric substrate and encapsulated with a thin transparent polymer film of Cytop. The photocurrent response was measured using a white light source as well as a monochromatic light of wavelength λ = 400 nm–900 nm. We measured responsivity using a 2-terminal configuration as high as R = 1 × 10 3 A W −1 under white light illumination with an optical power P opt = 0.02 nW. The R value increased to 3.5 × 10 3 A W −1 when measured using a 4-terminal configuration. Using monochromatic light on the same device, the measured values of R were 10 3 and 6 × 10 3 A W −1 under illumination of λ = 400 nm when measured using 2- and 4-terminal methods, respectively. The highest EQE values obtained using λ = 400 nm were 10 5 % and 10 6 % measured using 2- and 4-terminal configurations, respectively. The wavelength dependent responsivity decreased from 400 nm to the near-IR region at 900 nm. The observed photoresponse, photocurrent–dark current ratio (PDCR), detectivity as a function of applied gate voltage, optical power, contact resistances and wavelength were measured and are discussed in detail. The observed responsivity is also thoroughly studied as a function of contact resistance of the device. 

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