Mervin Zhao

Large-scale chemical assembly of atomically thin transistors and circuits

Next-generation electronics calls for new materials beyond silicon, aiming at increased functionality, performance and scaling in integrated circuits. In this respect, two-dimensional gapless graphene and semiconducting transition-metal dichalcogenides have emerged as promising candidates due to their atomic thickness and chemical stability. However, difficulties with precise spatial control during their assembly currently impede actual integration into devices. Here, we report on the large-scale, spatially controlled synthesis of heterostructures made of single-layer semiconducting molybdenum disulfide contacting conductive graphene. Transmission electron microscopy studies reveal that the single-layer molybdenum disulfide nucleates at the graphene edges. We demonstrate that such chemically assembled atomic transistors exhibit high transconductance (10 µS), on-off ratio (∼106) and mobility (∼17 cm2 V-1 s-1). The precise site selectivity from atomically thin conducting and semiconducting crystals enables us to exploit these heterostructures to assemble two-dimensional logic circuits, such as an NMOS inverter with high voltage gain (up to 70).Next-generation electronics calls for new materials beyond silicon for increased functionality, performance, and scaling in integrated circuits. Carbon nanotubes and semiconductor nanowires are at the forefront of these materials, but have challenges due to the complex fabrication techniques required for large-scale applications. Two-dimensional (2D) gapless graphene and semiconducting transition metal dichalcogenides (TMDCs) have emerged as promising electronic materials due to their atomic thickness, chemical stability and scalability. Difficulties in the assembly of 2D electronic structures arise in the precise spatial control over the metallic and semiconducting atomic thin films. Ultimately, this impedes the maturity of integrating atomic elements in modern electronics. Here, we report the large-scale spatially controlled synthesis of the single-layer semiconductor molybdenum disulfide (MoS2) laterally in contact with conductive graphene. Transition electron microscope (TEM) studies reveal that the single-layer MoS2 nucleates at the edge of the graphene, creating a lateral 2D heterostructure. We demonstrate such chemically assembled 2D atomic transistors exhibit high transconductance (10 uS), on-off ratios (10^6), and mobility (20 cm^2 V^-1 s^-1). We assemble 2D logic circuits, such as a heterostructure NMOS inverter with a high voltage gain, up to 70, enabled by the precise site selectivity from atomically thin conducting and semiconducting crystals. This scalable chemical assembly of 2D heterostructures may usher in a new era in two-dimensional electronic circuitry and computing.

Electrical generation and control of the valley carriers in a monolayer transition metal dichalcogenide

Electrically controlling the flow of charge carriers is the foundation of modern electronics. By accessing the extra spin degree of freedom (DOF) in electronics, spintronics allows for information processes such as magnetoresistive random-access memory. Recently, atomic membranes of transition metal dichalcogenides (TMDCs) were found to support unequal and distinguishable carrier distribution in different crystal momentum valleys. This valley polarization of carriers enables a new DOF for information processing. A variety of valleytronic devices such as valley filters and valves have been proposed, and optical valley excitation has been observed. However, to realize its potential in electronics it is necessary to electrically control the valley DOF, which has so far remained a significant challenge. Here, we experimentally demonstrate the electrical generation and control of valley polarization. This is achieved through spin injection via a diluted ferromagnetic semiconductor and measured through the helicity of the electroluminescence due to the spin-valley locking in TMDC monolayers. We also report a new scheme of electronic devices that combine both the spin and valley DOFs. Such direct electrical generation and control of valley carriers opens up new dimensions in utilizing both the spin and valley DOFs for next-generation electronics and computing.

Exciton-dominant electroluminescence from a diode of monolayer MoS2

We studied the microscopic origin of the electroluminescence from monolayer MoS2 fabricated on a heavily p-type doped silicon substrate. Auger recombination of the exciton-exciton annihilation of bound exciton emission is observed.

Crystalline Gibbs monolayers of DNA-capped nanoparticles at the air-liquid interface.

Using grazing-incidence small-angle X-ray scattering in a special configuration (parallel SAXS, or parSAXS), we mapped the crystallization of DNA-capped nanoparticles across a sessile droplet, revealing the formation of crystalline Gibbs monolayers of DNA-capped nanoparticles at the air-liquid interface. We showed that the spatial crystallization can be regulated by adjusting both ionic strength and DNA sequence length and that a modified form of the Daoud-Cotton model could describe and predict the resulting changes in interparticle spacing. Gibbs monolayers at the air-liquid interface provide an ideal platform for the formation and study of equilibrium nanostructures and may afford exciting routes toward the design of programmable 2D plasmonic materials and metamaterials.

Atomically phase-matched second-harmonic generation in a 2D crystal

Second-harmonic generation (SHG) has found extensive applications from hand-held laser pointers to spectroscopic and microscopic techniques. Recently, some cleavable van der Waals (vdW) crystals have shown SHG arising from a single atomic layer, where the SH light elucidated important information such as the grain boundaries and electronic structure in these ultra-thin materials. However, despite the inversion asymmetry of the single layer, the typical crystal stacking restores inversion symmetry for even numbers of layers leading to an oscillatory SH response, drastically reducing the applicability of vdW crystals such as molybdenum disulfide (MoS2). Here, we probe the SHG generated from the noncentrosymmetric 3R crystal phase of MoS2. We experimentally observed quadratic dependence of second-harmonic intensity on layer number as a result of atomically phase-matched nonlinear dipoles in layers of the 3R crystal that constructively interfere. By studying the layer evolution of the A and B excitonic transitions in 3R-MoS2 using SHG spectroscopy, we also found distinct electronic structure differences arising from the crystal structure and the dramatic effect of symmetry and layer stacking on the nonlinear properties of these atomic crystals. The constructive nature of the SHG in this 2D crystal provides a platform to reliably develop atomically flat and controllably thin nonlinear media.

Crystallization of DNA‐Capped Gold Nanoparticles in High‐Concentration, Divalent Salt Environments

The multiparametric nature of nanoparticle self-assembly makes it challenging to circumvent the instabilities that lead to aggregation and achieve crystallization under extreme conditions. By using non-base-pairing DNA as a model ligand instead of the typical base-pairing design for programmability, long-range 2D DNA-gold nanoparticle crystals can be obtained at extremely high salt concentrations and in a divalent salt environment. The interparticle spacings in these 2D nanoparticle crystals can be engineered and further tuned based on an empirical model incorporating the parameters of ligand length and ionic strength.

Excitons in atomically thin 2D semiconductors and their applications

Abstract The research on emerging layered two-dimensional (2D) semiconductors, such as molybdenum disulfide (MoS2), reveals unique optical properties generating significant interest. Experimentally, these materials were observed to host extremely strong light-matter interactions as a result of the enhanced excitonic effect in two dimensions. Thus, understanding and manipulating the excitons are crucial to unlocking the potential of 2D materials for future photonic and optoelectronic devices. In this review, we unravel the physical origin of the strong excitonic effect and unique optical selection rules in 2D semiconductors. In addition, control of these excitons by optical, electrical, as well as mechanical means is examined. Finally, the resultant devices such as excitonic light emitting diodes, lasers, optical modulators, and coupling in an optical cavity are overviewed, demonstrating how excitons can shape future 2D optoelectronics.