A novel liquid-phase exfoliation of layered crystals enables the production of defect-free and high quality 2D-crystal dispersions on a large scale.

The miniaturization of energy storage units is pivotal for the development of next-generation portable electronic devices. Micro-supercapacitors (MSCs) hold great potential to work as on-chip micro-power sources and energy storage units complementing batteries and energy harvester systems. Scalable production of supercapacitor materials with costeffective and high-throughput processing methods is crucial for the widespread application of MSCs. Here, wet-jet milling exfoliation of graphite is reported to scale up the production of graphene as a supercapacitor material. The formulation of aqueous/alcohol-based graphene inks allows metal-free, flexible MSCs to be screen-printed. These MSCs exhibit areal capacitance (C areal ) values up to 1.324 mF cm −2 (5.296 mF cm −2 for a single electrode), corresponding to an outstanding volumetric capacitance (C vol ) of 0. 490 F cm −3 (1.961 F cm −3 for a single electrode). The screen-printed MSCs can operate up to a power density above 20 mW cm −2 at an energy density of 0.064 µWh cm −2 . The devices exhibit excellent cycling stability over chargedischarge cycling (10 000 cycles), bending cycling (100 cycles at a bending radius of 1 cm) and folding (up to angles of 180°). Moreover, ethylene vinyl acetate-encapsulated MSCs retain their electrochemical properties after a home-laundry cycle, providing waterproof and washable properties for prospective application in wearable electronics.

Fermi level pinning in doped metal oxide (MO) nanocrystals (NCs) results in the formation of depletion layers, which affect their optical and electronic properties, and ultimately their application in smart optoelectronics, photocatalysis, or energy storage. For a precise control over functionality, it is important to understand and control their electronic bands at the nanoscale. Here, we show that depletion layer engineering allows designing the energetic band profiles and predicting the optoelectronic properties of MO NCs. This is achieved by shell thickness tuning of core–shell Sn:In2O3–In2O3 NCs, resulting in multiple band bending and multi-modal plasmonic response. We identify the modification of the band profiles after the light-induced accumulation of extra electrons as the main mechanism of photodoping and enhance the charge storage capability up to hundreds of electrons per NC through depletion layer engineering. Our experimental results are supported by theoretical models and are transferable to other core-multishell systems as well.

o Dip.to di Scienze Fisiche e Chimiche -Via Vetoio -67010 Coppito (AQ), Italy Optical parametric amplification is a second-order nonlinear process whereby an optical signal is amplified by a pump via the generation of an idler field. It is the key ingredient of tunable sources of radiation that play an important role in several photonic applications. This mechanism is inherently related to spontaneous parametric down-conversion that currently constitutes the building block for entangled photon pair generation, which has been exploited in modern quantum technologies ranging from computing to communications and cryptography. Here we demonstrate singlepass optical parametric amplification at the ultimate thickness limit; using semiconducting transition-metal dichalcogenides, we show that amplification can be attained over a propagation through a single atomic layer. Such a second-order nonlinear interaction at the 2D limit bypasses phase-matching requirements and achieves ultrabroad amplification bandwidths. The amplification process is independent on the in-plane polarization of the impinging signal and pump fields. First-principle calculations confirm the observed polarization invariance and linear relationship between idler and pump powers. Our results pave the way for the development of atom-sized tunable sources of radiation with applications in nanophotonics and quantum information technology.

Layered semiconductors of the IIIA-VIA group have attracted considerable attention in (opto)electronic applications thanks to their atomically thin structures and their thickness-dependent optical and electronic properties, which promise ultrafast response and high sensitivity. In particular, 2D indium selenide (InSe) has emerged as a promising candidate for the realization of thin-film field effect transistors and phototransistors due to its high intrinsic mobility (>10 2 cm 2 V −1 s −1 ) and the direct optical transitions in an energy range suitable for visible and near-infrared light detection. A key requirement for the exploitation of large-scale (opto)electronic applications relies on the development of low-cost and industrially relevant 2D material production processes, such as liquid phase exfoliation, combined with the availability of high-throughput device fabrication methods. Here, a β polymorph of indium selenide (β-InSe) is exfoliated in isopropanol and spray-coated InSe-based photodetectors are demonstrated, exhibiting high responsivity to visible light (maximum value of 274 A W −1 under blue excitation 455 nm) and fast response time (15 ms). The devices show a gate-dependent conduction with an n-channel transistor behavior.Overall, this study establishes that liquid phase exfoliated β-InSe is a valid candidate for printed high-performance photodetectors, which is critical for the development of industrial-scale 2D material-based optoelectronic devices.

Transition metal dichalcogenide (TMDCs) monolayers make an excellent component in optoelectronic devices such as photodetectors and phototransistors. Selenide‐based TMDCs, specifically molybdenum diselenide (MoSe2) monolayers with low defect densities, show much faster photoresponses compared to their sulfide counterpart. However, the typically low absorption of the atomically thin MoSe2 monolayer and high exciton binding energy limit the photogeneration of charge carriers. Yet, integration of light‐harvesting materials with TMDCs can produce increased photocurrents via energy transfer. In this article, it is demonstrated that the interaction of cesium lead bromide (CsPbBr3) nanocrystals with MoSe2 monolayers results into an energy transfer efficiency of over 86%, as ascertained from the quenching and decay dynamics of the CsPbBr3 nanocrystals emission. Notably, the increase in the MoSe2 monolayer emission in the heterostructure accounts only for 33% of the transferred energy. It is found that part of the excess energy generates directly free carriers in the MoSe2 monolayer, as a result of the transfer of energy into the exciton continuum. The efficiency of the heterostructure via enhanced photocurrents with respect to the single material unit is proven. These results demonstrate a viable route to overcome the high exciton binding energy typical for TMDCs, as such having an impact on optoelectronic processes that rely on efficient exciton dissociation.

Two-dimensional (2D) transition-metal monochalcogenides have been recently predicted to be potential photo(electro)catalysts for water splitting and photoelectrochemical (PEC) reactions. Differently from the most established InSe, GaSe, GeSe, and many other monochalcogenides, bulk GaS has a large band gap of ∼2.5 eV, which increases up to more than 3.0 eV with decreasing its thickness due to quantum confinement effects. Therefore, 2D GaS fills the void between 2D small-band-gap semiconductors and insulators, resulting of interest for the realization of van der Waals type-I heterojunctions in photocatalysis, as well as the development of UV light-emitting diodes, quantum wells, and other optoelectronic devices. Based on theoretical calculations of the electronic structure of GaS as a function of layer number reported in the literature, we experimentally demonstrate, for the first time, the PEC properties of liquid-phase exfoliated GaS nanoflakes. Our results indicate that solution-processed 2D GaS-based PEC-type photodetectors outperform the corresponding solid-state photodetectors. In fact, the 2D morphology of the GaS flakes intrinsically minimizes the distance between the photogenerated charges and the surface area at which the redox reactions occur, limiting electron–hole recombination losses. The latter are instead deleterious for standard solid-state configurations. Consequently, PEC-type 2D GaS photodetectors display a relevant UV-selective photoresponse. In particular, they attain responsivities of 1.8 mA W –1 in 1 M H 2 SO 4 [at 0.8 V vs reversible hydrogen electrode (RHE)], 4.6 mA W –1 in 1 M Na 2 SO 4 (at 0.9 V vs RHE), and 6.8 mA W –1 in 1 M KOH (at 1.1. V vs RHE) under 275 nm illumination wavelength with an intensity of 1.3 mW cm –2 . Beyond the photodetector application, 2D GaS-based PEC-type devices may find application in tandem solar PEC cells in combination with other visible-sensitive low-band-gap materials, including transition-metal monochalcogenides recently established for PEC solar energy conversion applications.

Light-driven multi-charge accumulation (i.e., photodoping) of doped metal oxide nanocrystals opens the way to innovative solutions for the direct conversion and storage of the solar energy.