2D Heterostructures for Ubiquitous Electronics and Optoelectronics: Principles, Opportunities, and Challenges.

A grand family of two-dimensional (2D) materials and their heterostructures have been discovered through the extensive experimental and theoretical efforts of chemists, material scientists, physicists, and technologists. These pioneering works contribute to realizing the fundamental platforms to explore and analyze new physical/chemical properties and technological phenomena at the micro-nano-pico scales. Engineering 2D van der Waals (vdW) materials and their heterostructures via chemical and physical methods with a suitable choice of stacking order, thickness, and interlayer interactions enable exotic carrier dynamics, showing potential in high-frequency electronics, broadband optoelectronics, low-power neuromorphic computing, and ubiquitous electronics. This comprehensive review addresses recent advances in terms of representative 2D materials, the general fabrication methods, and characterization techniques and the vital role of the physical parameters affecting the quality of 2D heterostructures. The main emphasis is on 2D heterostructures and 3D-bulk (3D) hybrid systems exhibiting intrinsic quantum mechanical responses in the optical, valley, and topological states. Finally, we discuss the universality of 2D heterostructures with representative applications and trends for future electronics and optoelectronics (FEO) under the challenges and opportunities from physical, nanotechnological, and material synthesis perspectives.

Current crowding in graphene-silicon schottky diodes.

The performance of the Graphene/Si (Gr/Si) Schottky interface and its potential in future electronics strongly rely on the quality of interconnecting contacts with external circuitry. In this work, we investigate the dominating and limiting factors of Gr/Si interfaces designed for high light absorption, paying particular attention to the nature of the contact failure under high electrostatic discharge (ESD) conditions. Our findings indicate that severe current crowding at contact edges of the graphene is the dominating factor for the device breakdown. Material degradation and electrical breakdown are systematically analyzed by atomic force, Raman, scanning electron, and energy-dispersive x-ray spectroscopies. This work enlists the robustness and limitations of Gr/Si junction in photodiode architecture under high ESD conditions that can be used as general guidelines for 2D-3D electronic and optoelectronic devices.

In-Situ Monitoring of Reciprocal Charge Transfer and Losses in Graphene-Silicon CCD Pixels.

Charge-coupled devices (CCD) allow imaging by photodetection, charge integration, and serial transfer of the stored charge packets from multiple pixels to the readout node. The functionality of CCD can be extended to the non-destructive and in-situ readout of the integrated charges by replacing metallic electrodes with graphene in the metal-oxide-semiconductors (MOS) structure of a CCD pixel. The electrostatic capacitive coupling of graphene with the substrate allows the Fermi level tuning that reflects the integrated charge density in the depletion well. This work demonstrates the in-situ monitoring of the serial charge transfer and interpixel transfer losses in a reciprocating manner between two adjacent Gr-Si CCD pixels by benefitting the electrostatic and gate-to-gate couplings. We achieved the maximum charge transfer efficiency (CTE) of 92.4%, which is mainly decided by the inter-pixel distance, phase clock amplitudes, switching slopes, and density of surface defects. The discussion on overcoming transfer losses and improving CTE by realizing a graphene-electron multiplication CCD is also presented. The proof of the concept of the in-situ readout of the out-of-plane avalanche in a single Gr-Si CCD pixel is also demonstrated, which can amplify the photo packet in a pre-transfer manner.

Photophysics and energy transfer studies of Alq3 confined in the voids of nanoporous anodic alumina.

We report on a hierarchical nanoarchitecture wherein distinct chromophores are deterministically placed at two different types of sites in a nanoporous metal oxide framework. One chromophore, namely Tris(8-hydroxyquinoline)aluminium(III) (Alq3), is embedded in the 1-2 nm sized nanovoids of anodic aluminum oxide (AAO) and another chromophore (carboxyfluorescein or pyrenebutyric acid) is anchored in the form of a monolayer to the surface of the walls of the cylindrical nanopores (- 20 nm in diameter) of AAO. We found the luminescence maximum to occur at 492 nm, blueshifted by at least 18 nm from the value in solutions and thin films. The excited state decay of Alq3 molecules in nanovoids was found to be biexponential with a fast component of 338 ps and a slower component of 2.26 ns, different from Alq3 thin films and solutions. Using a combination of steady state and time-resolved luminescence studies, we found that efficient Forster-type resonance energy transfer (FRET) from Alq3 in the nanovoids to the carboxyfluorescein monolayer could be used to pump the emission of surface-bound chromophores. Conversely, the emission of nanovoid-confined Alq3 could be pumped by energy transfer from a pyrenebutyric acid monolayer. Such intra-nanoarchitecture interactions between chromophores deterministically placed in different spatial locations are important in applications such as organic light emitting diodes, chemical sensors, energy transfer fluorescent labels, light harvesting antennas and organic spintronics.

Neuromorphic device based on silicon nanosheets.

Silicon is vital for its high abundance, vast production, and perfect compatibility with the well-established CMOS processing industry. Recently, artificially stacked layered 2D structures have gained tremendous attention via fine-tuning properties for electronic devices. This article presents neuromorphic devices based on silicon nanosheets that are chemically exfoliated and surface-modified, enabling self-assembly into hierarchical stacking structures. The device functionality can be switched between a unipolar memristor and a feasibly reset-able synaptic device. The memory function of the device is based on the charge storage in the partially oxidized SiNS stacks followed by the discharge activated by the electric field at the Au-Si Schottky interface, as verified in both experimental and theoretical means. This work further inspired elegant neuromorphic computation models for digit recognition and noise filtration. Ultimately, it brings silicon - the most established semiconductor - back to the forefront for next-generation computations.

Bidirectional mid-infrared communications between two identical macroscopic graphene fibres.

Among light-based free-space communication platforms, mid-infrared (MIR) light pertains to important applications in biomedical engineering, environmental monitoring, and remote sensing systems. Integrating MIR generation and reception in a network using two identical devices is vital for the miniaturization and simplification of MIR communications. However, conventional MIR emitters and receivers are not bidirectional due to intrinsic limitations of low performance and often require cryogenic cooling. Here, we demonstrate that macroscopic graphene fibres (GFs) assembled from weakly-coupled graphene layers allow room-temperature MIR detection and emission with megahertz modulation frequencies due to the persistence of photo-thermoelectric effect in millimeter-length and the ability to rapidly modulate gray-body radiation. Based on the dual-functionality of GFs, we set up a system that conducts bidirectional data transmission by switching modes between two identical GFs. The room-temperature operation of our systems and the potential to produce GFs on industrial textile-scale offer opportunities for simplified and wearable optical communications.

Approaching the Collection Limit in Hot Electron Transistors with Ambipolar Hot Carrier Transport.

Hot electron transistors (HETs) containing two-dimensional (2D) materials promise great potential in high-frequency analog and digital applications. Here, we experimentally demonstrate all-2D van der Waals (vdW) HETs formed by graphene, hBN, and WSe2, in which the polarity of carriers could be tuned by changing bias conditions. We proposed a theoretical model to distinguish hot hole and hot electron components in the ambipolar vdW HET. Importantly, both hot hole and hot electron modes are achieved with pronounced saturation behavior as well as record-high collection efficiency approaching theoretical limits (99.9%) at room temperature. The vdW HETs show a maximum output current density of 400 A/cm2. The observed ambipolar hot carrier transport with high collection efficiency is promising for high-speed nanoelectronics and 2D hot electron spectroscopy.