The applications of lanthanide-doped upconversion nanocrystals in biological imaging, photonics, photovoltaics and therapeutics have fuelled a growing demand for rational control over the emission profiles of the nanocrystals. A common strategy for tuning upconversion luminescence is to control the doping concentration of lanthanide ions. However, the phenomenon of concentration quenching of the excited state at high doping levels poses a significant constraint. Thus, the lanthanide ions have to be stringently kept at relatively low concentrations to minimize luminescence quenching. Here we describe a new class of upconversion nanocrystals adopting an orthorhombic crystallographic structure in which the lanthanide ions are distributed in arrays of tetrad clusters. Importantly, this unique arrangement enables the preservation of excitation energy within the sublattice domain and effectively minimizes the migration of excitation energy to defects, even in stoichiometric compounds with a high Yb(3+) content (calculated as 98 mol%). This allows us to generate an unusual four-photon-promoted violet upconversion emission from Er(3+) with an intensity that is more than eight times higher than previously reported. Our results highlight that the approach to enhancing upconversion through energy clustering at the sublattice level may provide new opportunities for light-triggered biological reactions and photodynamic therapy.
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.
Since the first isolation of graphene, new classes of two-dimensional (2D) materials have offered fascinating platforms for fundamental science and technology explorations at the nanometer scale. In particular, 2D transition metal dichalcogenides (TMD) such as MoS2 and WSe2 have been intensely investigated due to their unique electronic and optical properties, including tunable optical bandgaps, direct-indirect bandgap crossover, strong spin-orbit coupling, etc., for next-generation flexible nanoelectronics and nanophotonics applications. On the other hand, organics have always been excellent materials for flexible electronics. A plethora of organic molecules, including donors, acceptors, and photosensitive molecules, can be synthesized using low cost and scalable procedures. Marrying the fields of organics and 2D TMDs will bring benefits that are not present in either material alone, enabling even better, multifunctional flexible devices. Central to the realization of such devices is a fundamental understanding of the organic-2D TMD interface. Here, we review the organic-2D TMD interface from both chemical and physical perspectives. We discuss the current understanding of the interfacial interactions between the organic layers and the TMDs, as well as the energy level alignment at the interface, focusing in particular on surface charge transfer and electronic screening effects. Applications from the literature are discussed, especially in optoelectronics and p-n hetero- and homo-junctions. We conclude with an outlook on future scientific and device developments based on organic-2D TMD heterointerfaces.
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