We report the design, fabrication, and characterization of colloidal PbSe nanocrystal (NC)-based photovoltaic test structures that exhibit an excitonic solar cell mechanism. Charge extraction from the NC active layer is driven by a photoinduced chemical potential energy gradient at the nanostructured heterojunction. By minimizing perturbation to PbSe NC energy levels and thereby gaining insight into the "intrinsic" photovoltaic properties and charge transfer mechanism of PbSe NC, we show a direct correlation between interfacial energy level offsets and photovoltaic device performance. Size dependent PbSe NC energy levels were determined by cyclic voltammetry and optical spectroscopy and correlated to photovoltaic measurements. Photovoltaic test structures were fabricated from PbSe NC films sandwiched between layers of ZnO nanoparticles and PEDOT:PSS as electron and hole transporting elements, respectively. The device current-voltage characteristics suggest a charge separation mechanism that is distinct from previously reported Schottky devices and consistent with signatures of excitonic solar cells. Remarkably, despite the limitation of planar junction structure, and without film thickness optimization, the best performing device shows a 1-sun power conversion efficiency of 3.4%, ranking among the highest performing NC-based solar cells reported to date.

Internanocrystal coupling induced excitons dissociation in lead salt nanocrystal assemblies is investigated. By combining transient photoluminescence spectroscopy, grazing incidence small-angle X-ray scattering, and time-resolved electric force microscopy, we show that excitons can dissociate, without the aid of an external bias or chemical potential gradient, via tunneling through a potential barrier when the coupling energy is comparable to the exciton binding energy. Our results have important implications for the design of nanocrystal-based optoelectronic devices.

Neuromorphic computing, which emulates the biological neural systems could overcome the high‐power consumption issue of conventional von‐Neumann computing. State‐of‐the‐art artificial synapses made of two‐terminal memristors, however, show variability in filament formation and limited capacity due to their inherent single presynaptic input design. Here, a memtransistor‐based artificial synapse is realized by integrating a memristor and selector transistor into a multiterminal device using monolayer polycrys‐talline‐MoS2 grown by a scalable chemical vapor deposition (CVD) process. Notably, the memtransistor offers both drain‐ and gate‐tunable nonvolatile memory functions, which efficiently emulates the long‐term potentiation/depression, spike‐amplitude, and spike‐timing‐dependent plasticity of biological synapses. Moreover, the gate tunability function that is not achievable in two‐terminal memristors, enables significant bipolar resistive states switching up to four orders‐of‐magnitude and high cycling endurance. First‐principles calculations reveal a new resistive switching mechanism driven by the diffusion of double sulfur vacancy perpendicular to the MoS2 grain boundary, leading to a conducting switching path without the need for a filament forming process. The seamless integration of multiterminal memtransistors may offer another degree‐of‐freedom to tune the synaptic plasticity by a third gate terminal for enabling complex neuromorphic learning.

The colloidal synthesis of SnSe nanoparticles is accomplished through the injection of bis[bis(trimethylsilyl)amino]tin(II) into hot trioctylphosphine:selenium in the presence of oleylamine. Through the manipulation of reaction temperature particles are grown with the average diameter reliably tuned to 4-10 nm. Quantum confinement is examined by establishing a relationship between particle size and band gap while the in depth growth dynamics are illuminated through UV-vis-NIR spectroscopy. Surface chemistry effects are explored, including the demonstration of useful ligand exchanges and the development of routes toward anisotropic particle growth. Finally, transient current-voltage properties of SnSe nanocrystal films in the dark and light are examined.

Cu2O and CuO are attractive photocatalytic materials for water splitting due to their earth abundance and low cost. In this paper, we report the deposition of Cu2O and CuO thin films by a sol-gel spin-coating process. Sol-gel deposition has distinctive advantages such as low-cost solution processing and uniform film formation over large areas with a precise stoichiometry and thickness control. Pure-phase Cu2O and CuO films were obtained by thermal annealing at 500 °C in nitrogen and ambient air, respectively. The films were successfully incorporated as photocathodes in a photoelectrochemical (PEC) cell, achieving photocurrents of -0.28 mA cm(-2) and -0.35 mA cm(-2) (for Cu2O and CuO, respectively) at 0.05 V vs. a reversible hydrogen electrode (RHE). The Cu2O photocurrent was enhanced to -0.47 mA cm(-2) upon incorporation of a thin layer of a NiOx co-catalyst. Preliminary stability studies indicate that CuO may be more stable than Cu2O as a photocathode for PEC water-splitting.

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The cost‐effective, robust, and efficient electrocatalysts for photoelectrochemical (PEC) water‐splitting has been extensively studied over the past decade to address a solution for the energy crisis. The interesting physicochemical properties of CuO have introduced this promising photocathodic material among the few photocatalysts with a narrow bandgap. This photocatalyst has a high activity for the PEC hydrogen evolution reaction (HER) under simulated sunlight irradiation. Here, the recent advancements of CuO‐based photoelectrodes, including undoped CuO, doped CuO, and CuO composites, in the PEC water‐splitting field, are comprehensively studied. Moreover, the synthesis methods, characterization, and fundamental factors of each classification are discussed in detail. Apart from the exclusive characteristics of CuO‐based photoelectrodes, the PEC properties of CuO/2D materials, as groups of the growing nanocomposites in photocurrent‐generating devices, are discussed in separate sections. Regarding the particular attention paid to the CuO heterostructure photocathodes, the PEC water splitting application is reviewed and the properties of each group such as electronic structures, defects, bandgap, and hierarchical structures are critically assessed.

Single-layer molybdenum disulfide (MoS) has attracted significant attention due to its electronic and physical properties, with much effort invested toward obtaining large-area high-quality monolayer MoS films. In this work, we demonstrate a reactive-barrier-based approach to achieve growth of highly homogeneous single-layer MoS on sapphire by the use of a nickel oxide foam barrier during chemical vapor deposition. Due to the reactivity of the NiO barrier with MoO, the concentration of precursors reaching the substrate and thus nucleation density is effectively reduced, allowing grain sizes of up to 170 μm and continuous monolayers on the centimeter length scale being obtained. The quality of the monolayer is further revealed by angle-resolved photoemission spectroscopy measurement by observation of a very well resolved electronic band structure and spin-orbit splitting of the bands at room temperature with only two major domain orientations, indicating the successful growth of a highly crystalline and well-oriented MoS monolayer.