Self-referencing for quasi shot-noise-limited widefield transient microscopy.

Many applications of ultrafast and nonlinear optical microscopy require the measurement of small differential signals over large fields-of-view. Widefield configurations drastically reduce the acquisition time; however, they suffer from the low frame rates of two-dimensional detectors, which limit the modulation frequency, making the measurement sensitive to excess laser noise. Here we introduce a self-referenced detection configuration for widefield differential imaging. Employing regions of the field of view with no differential signal as references, we cancel probe fluctuations and increase the signal-to-noise ratio by an order of magnitude reaching noise levels only a few percent above the shot noise limit. We anticipate broad applicability of our method to transient absorption, stimulated Raman scattering and photothermal-infrared microscopies.

Thermally Driven Multilevel Non-Volatile Memory with Monolayer MoS2 for Brain-Inspired Artificial Learning.

The demands of modern electronic components require advanced computing platforms for efficient information processing to realize in-memory operations with a high density of data storage capabilities toward developing alternatives to von Neumann architectures. Herein, we demonstrate the multifunctionality of monolayer MoS2 memtransistors, which can be used as a high-geared intrinsic transistor at room temperature; however, at a high temperature (>350 K), they exhibit synaptic multilevel memory operations. The temperature-dependent memory mechanism is governed by interfacial physics, which solely depends on the gate field modulated ion dynamics and charge transfer at the MoS2/dielectric interface. We have proposed a non-volatile memory application using a single Field Effect Transistor (FET) device where thermal energy can be ventured to aid the memory functions with multilevel (3-bit) storage capabilities. Furthermore, our devices exhibit linear and symmetry in conductance weight updates when subjected to electrical potentiation and depression. This feature has enabled us to attain a high classification accuracy while training and testing the Modified National Institute of Standards and Technology datasets through artificial neural network simulation. This work paves the way toward reliable data processing and storage using 2D semiconductors with high-packing density arrays for brain-inspired artificial learning.

Laterally Grown Strain-Engineered Semitransparent Perovskite Solar Cells with 16.01% Efficiency.

Hybrid organometallic halide perovskite-based semitransparent solar cell research has garnered significant attention recently due to their promising applications for smart windows, tandem devices, wearable electronics, displays, and sustainable internet-of-things. Though considerable progress has been made, stability, controlling the crystalline qualities, and growth orientation in perovskite thin films play crucial roles in improving the photovoltaic (PV) performance. Recently, strain modulation within the perovskite gathers an immense interest that is achieved by the ex situ process. However, little work is reported on in situ strain modulation, which is presented here. Apart from the challenges in the fabrication of high-efficiency perovskite solar cell (PSC) devices under ambient conditions, the stability of organic hole-transporting materials needs urgent attention. Herein, a single-step deposition of formamidiniumchloride (FACl)-mediated CH3NH3PbI3 (MAPbI3) thin films without an inert atmosphere and CuI as the inorganic hole-transporting material is demonstrated for their potential application toward semitransparent PSCs. The FACl amount in MAPbI3 (mg/mL) plays a critical role in controlling the crystallinity, growth orientations, and in situ strains, which modulate the charge carrier transport dynamics, thereby improving the efficiency of the PSC device. A photoconversion efficiency of 16.01% has been achieved from MAPbI3 with 20 mg/mL of FACl additive incorporation. The modification of the structural, electronic, and optical properties and the origin of strain in the as-synthesized MAPbI3 domains due to the addition of FACl are further validated with experimental findings in detail using density functional theory simulations.

Challenges and opportunities in 2D heterostructures for electronic and optoelectronic devices.

Two-dimensional (2D) materials such as graphene, transition metal dichalcogenides (TMDs), and their heterojunctions are prospective materials for future electronics, optoelectronics, and quantum technologies. Assembling different 2D layers offers unique ways to control optical, electrical, thermal, magnetic, and topological phenomena. Controlled fabrications of electronic grade 2D heterojunctions are of paramount importance. Here, we enlist novel and scalable strategies to fabricate 2D vertical and lateral heterojunctions, consisting of semiconductors, metals, and/or semimetals. Critical issues that need to be addressed are the device-to-device variations, reliability, stability, and performances of 2D heterostructures in electronic and optoelectronic applications. Also, stacking order-dependent formation of moiré excitons in 2D heterostructures are emerging with exotic physics and new opportunities. Furthermore, the realization of 2D heterojunction-based novel devices, including excitonic and valleytronic transistors, demands more extensive research efforts for real-world applications. We also outline emergent phenomena in 2D heterojunctions central to nanoelectronics, optoelectronics, spintronics, and energy applications.

Tunable Conductance of MoS2 and WS2 Quantum Dots by Electron Transfer with Redox-Active Quinone.

Due to their uniqueness in tunable photophysics, transition metal dichalcogenide (TMD) based quantum dots (QDs) have emerged as the next-generation quantum materials for technology-based semiconductor applications. This demands frontline research on the rational synthesis of the TMD QDs with controlled shape, size, nature of charge migration at the interface, and their easy integration in optoelectronic devices. In this article, with a controlled solution-processed synthesis of MoS2 and WS2 QDs, we demonstrate the disparity in their structural, optical, and electrical characteristics in bulk and confinement. With a series of steady-state and time-resolved spectroscopic measurements in different media, we explore the uncommon photophysics of MoS2 and WS2 QDs such as excitation-dependent photoluminescence and assess their excited state charge transfer kinetics with a redox-active biomolecule, menadione (MQ). In comparison to the homogeneous aqueous medium, photoinduced charge transfer between the QDs and MQ becomes more plausible in encapsulated cetyltrimethylammonium bromide (CTAB) micelles. Current sensing atomic force microscopy (CS-AFM) measurements at a single molecular level reveal that the facilitated charge transfer of QDs with MQ strongly correlates with an enhancement in their charge transport behavior. An increase in charge transport further depends on the density of states of the QDs directing a change in Schottky emission to Fowler-Nordheim (FN) type of tunneling across the metal-QD-metal junction. The selective response of the TMD QDs while in proximity to external molecules can be used to design advanced optoelectronic devices and applications involving rectifiers and tunnel diodes for future quantum technology.

Bilayer Lateral Heterostructures of Transition-Metal Dichalcogenides and Their Optoelectronic Response.

Two-dimensional lateral heterojunctions based on monolayer transition-metal dichalcogenides (TMDs) have received increasing attention given that their direct band gap makes them very attractive for optoelectronic applications. Although bilayer TMDs present an indirect band gap, their electrical properties are expected to be less susceptible to ambient conditions, with higher mobilities and density of states when compared to monolayers. Bilayers and few-layers single domain devices have already demonstrated higher performance in radio frequency and photosensing applications. Despite these advantages, lateral heterostructures based on bilayer domains have been less explored. Here, we report the controlled synthesis of multi-junction bilayer lateral heterostructures based on MoS2-WS2 and MoSe2-WSe2 monodomains. The heterojunctions are created via sequential lateral edge-epitaxy that happens simultaneously in both the first and the second layers. A phenomenological mechanism is proposed to explain the growth mode with self-limited thickness that happens within a certain window of growth conditions. With respect to their as-grown monolayer counterparts, bilayer lateral heterostructures yield nearly 1 order of magnitude higher rectification currents. They also display a clear photovoltaic response, with short circuit currents ∼103 times larger than those extracted from the as-grown monolayers, in addition to room-temperature electroluminescence. The improved performance of bilayer heterostructures significantly expands the potential of two-dimensional materials for optoelectronics.