Extreme Reconfigurable Nanoelectronics at the CaZrO3/SrTiO3 Interface

Complex oxide heterostructures have fascinating emergent properties that originate from the properties of the bulk constituents as well as from dimensional confinement. The conductive behavior of the polar/nonpolar LaAlO₃/SrTiO₃ interface can be reversibly switched using conductive atomic force microscopy (c‐AFM) lithography, enabling a wide range of devices and physics to be explored. Here, extreme nanoscale control over the CaZrO₃/SrTiO₃ (CZO/STO) interface, which is formed from two materials that are both nonpolar, is reported. Nanowires with measured widths as narrow as 1.2 nm are realized at the CZO/STO interface at room temperature by c‐AFM lithography. These ultrathin nanostructures have spatial dimensions at room temperature that are comparable to single‐walled carbon nanotubes, and hold great promise for alternative oxide‐based nanoelectronics, as well as offer new opportunities to investigate the electronic structure of the complex oxide interfaces. The cryogenic properties of devices constructed from quasi‐1D channels, tunnel barriers, and planar gates exhibit gate‐tunable superconductivity, quantum oscillations, electron pairing outside of the superconducting regime, and quasi‐ballistic transport. This newly demonstrated ability to control the metal–insulator transition at nonpolar oxide interface greatly expands the class of materials whose behavior can be patterned and reconfigured at extreme nanoscale dimensions.     

Asymmetrically Encapsulated Vertical ITO/MoS2/Cu2O Photodetector with Ultrahigh Sensitivity

Strong light absorption, coupled with moderate carrier transport properties, makes 2D layered transition metal dichalcogenide semiconductors promising candidates for low intensity photodetection applications. However, the performance of these devices is severely bottlenecked by slow response with persistent photocurrent due to long lived charge trapping, and nonreliable characteristics due to undesirable ambience and substrate effects. Here ultrahigh specific detectivity (D*) of 3.2 × 10¹⁴ Jones and responsivity (R) of 5.77 × 10⁴ A W^?1 are demonstrated at an optical power density (P_op) of 0.26 W m^?2 and external bias (V_ext) of ?0.5 V in an indium tin oxide/MoS₂/copper oxide/Au vertical multi‐heterojunction photodetector exhibiting small carrier transit time. The active MoS₂ layer being encapsulated by carrier collection layers allows us to achieve repeatable characteristics over large number of cycles with negligible trap assisted persistent photocurrent. A large D* > 10¹⁴ Jones at zero external bias is also achieved due to the built‐in field of the asymmetric photodetector. Benchmarking the performance against existing reports in literature shows a viable pathway for achieving reliable and highly sensitive photodetectors for ultralow intensity photodetection applications.     

Interface Engineering with MoS2–Pd Nanoparticles Hybrid Structure for a Low Voltage Resistive Switching Memory

Metal oxide‐based resistive random access memory (RRAM) has attracted a lot of attention for its scalability, temperature robustness, and potential to achieve machine learning. However, a thick oxide layer results in relatively high program voltage while a thin one causes large leakage current and a small window. Owing to these fundamental limitations, by optimizing the oxide layer itself a novel interface engineering idea is proposed to reduce the programming voltage, increase the uniformity and on/off ratio. According to this idea, a molybdenum disulfide (MoS₂)–palladium nanoparticles hybrid structure is used to engineer the oxide/electrode interface of hafnium oxide (HfO_x)‐based RRAM. Through its interface engineering, the set voltage can be greatly lowered (from ?3.5 to ?0.8 V) with better uniformity under a relatively thick HfO_x layer (≈15 nm), and a 30 times improvement of the memory window can be obtained. Moreover, due to the atomic thickness of MoS₂ film and high transmittance of ITO, the proposed RRAM exhibits high transparency in visible light. As the proposed interface‐engineering RRAM exhibits good transparency, low SET voltage, and a large resistive switching window, it has huge potential in data storage in transparent circuits and wearable electronics with relatively low supply voltage.     

High-Mobility 2D Hole Gas at a SrTiO3 Interface

Strontium titanate (SrTiO₃ or STO) is important for oxide-based electronics as it serves as a standard substrate for a wide range of high-temperature superconducting cuprates, colossal magnetoresistive manganites, and multiferroics. Moreover, in its heterostructures with different materials, STO exhibits a broad spectrum of important physics such as superconductivity, magnetism, the quantum Hall effect, giant thermoelectric effect, and colossal ionic conductivity, most of which emerge in a two-dimensional (2D) electron gas (2DEG) formed at an STO interface. However, little is known about its counterpart system, a 2D hole gas (2DHG) at the STO interface. Here, a simple way of realizing a 2DHG with an ultrahigh mobility of 24 000 cm² V⁻¹ s⁻¹ is demonstrated using an interface between STO and a thin amorphous FeO_y layer, made by depositing a sub-nanometer-thick Fe layer on an STO substrate at room temperature. This mobility is the highest among those reported for holes in oxides. The carrier type can be switched from p-type (2DHG) to n-type (2DEG) by controlling the Fe thickness. This unprecedented method of forming a 2DHG at an STO interface provides a pathway to unexplored hole-related physics in this system and enables extremely low-cost and high-speed oxide electronics.     

Interface Modulation of MoS2/Metal Oxide Heterostructures for Efficient Hydrogen Evolution Electrocatalysis

Developing efficient earth‐abundant MoS₂ based hydrogen evolution reaction (HER) electrocatalysts is important but challenging due to the sluggish kinetics in alkaline media. Herein, a strategy to fabricate a high‐performance MoS₂ based HER electrocatalyst by modulating interface electronic structure via metal oxides is developed. All the heterostructure catalysts present significant improvement of HER electrocatalytic activities, demonstrating a positive role of metal oxides decoration in promoting the rate‐limited water dissociation step for the HER mechanism in alkaline media. The as‐obtained MoS₂/Ni₂O₃H catalyst exhibits a low overpotential of 84 mV at 10 mA cm^?2 and small charge‐transfer resistance of 1.5 Ω in 1 m KOH solution. The current density (217 mA cm^?2) at the overpotential of 200 mV is about 2 and 24 times higher than that of commercial Pt/C and bare MoS₂, respectively. Additionally, these MoS₂/metal oxides heterostructure catalysts show outstanding long‐term stability under a harsh chronopotentiometry test. Theoretical calculations reveal the varied sensitivity of 3d‐band in different transition oxides, in which Ni‐3d of Ni₂O₃H is evidently activated to achieve fast electron transfer for HER as the electron‐depletion center. Both electronic properties and energetic reaction trends confirm the high electroactivity of MoS₂/Ni₂O₃H in the adsorption and dissociation of H₂O for highly efficient HER in alkaline media.     

Anisotropic MoS2 Nanosheets Grown on Self‐Organized Nanopatterned Substrates

Manipulating the anisotropy in 2D nanosheets is a promising way to tune or trigger functional properties at the nanoscale. Here, a novel approach is presented to introduce a one‐directional anisotropy in MoS₂ nanosheets via chemical vapor deposition (CVD) onto rippled patterns prepared on ion‐sputtered SiO₂/Si substrates. The optoelectronic properties of MoS₂ are dramatically affected by the rippled MoS₂ morphology both at the macro‐ and the nanoscale. In particular, strongly anisotropic phonon modes are observed depending on the polarization orientation with respect to the ripple axis. Moreover, the rippled morphology induces localization of strain and charge doping at the nanoscale, thus causing substantial redshifts of the phonon mode frequencies and a topography‐dependent modulation of the MoS₂ workfunction, respectively. This study paves the way to a controllable tuning of the anisotropy via substrate pattern engineering in CVD‐grown 2D nanosheets.     

Synergetic Behavior in 2D Layered Material/Complex Oxide Heterostructures

The marriage between a 2D layered material (2DLM) and a complex transition metal oxide (TMO) results in a variety of physical and chemical phenomena that cannot be achieved in either material alone. Interesting recent discoveries in systems such as graphene/SrTiO₃, graphene/LaAlO₃/SrTiO₃, graphene/ferroelectric oxide, MoS₂/SrTiO₃, and FeSe/SrTiO₃ heterostructures include voltage scaling in field‐effect transistors, charge state coupling across an interface, quantum conductance probing of the electrochemical activity, novel memory functions based on charge traps, and greatly enhanced superconductivity. In this context, various properties and functionalities appearing in numerous different 2DLM/TMO heterostructure systems are reviewed. The results imply that the multidimensional heterostructure approach based on the disparate material systems leads to an entirely new platform for the study of condensed matter physics and materials science. The heterostructures are also highly relevant technologically as each constituent material is a promising candidate for next‐generation optoelectronic devices.     

二维层状WS2/MoS2异质结中镧系近红外光子发射与能量转移（英文）

镧系离子由于其独特的光子特性而备受关注.二维层状范德华异质结的光电特性和器件性能受到界面耦合的极大影响,该异质结通常是由两层或多层过渡金属二硫化物(TMD)堆叠而成.本文通过两步合成构建了镧系离子掺杂的层状WS2/MoS2异质结.所制备的掺杂薄膜是在晶圆衬底上生长的高度织构纳米片.更重要的是,由于两个TMD层中镧系离子之间的能量转移,层状异质结的结构减少了因均匀掺杂或浓度猝灭而引起的无益交叉松弛,所制备的堆叠异质结能够在近红外通讯窗口产生高效的光子发射.镧系掺杂和能量转移的研究结果表明,镧系离子可以有效地扩展TMD薄膜的发射波段及其异质结构.本工作所发展的镧系掺杂TMD异质结有助于进一步研究原子级超薄近红外光子器件.     

Microlandscaping of Au Nanoparticles on Few‐Layer MoS2 Films for Chemical Sensing

Surface modification or decoration of ultrathin MoS₂ films with chemical moieties is appealing since nanointerfacing can functionalize MoS₂ films with bonus potentials. In this work, a facile and effective method for microlandscaping of Au nanoparticles (NPs) on few‐layer MoS₂ films is developed. This approach first employs a focused laser beam to premodify the MoS₂ films to achieve active surface domains with unbound sulfur. When the activated surface is subsequently immersed in AuCl₃ solution, Au NPs are found to preferentially decorate onto the modified regions. As a result, Au NPs can be selectively and locally anchored onto designated regions on the MoS₂ surface. With a scanning laser beam, microlandscapes comprising of Au NPs decorated on laser‐defined micropatterns are constructed. By varying the laser power, reaction time and thickness of the MoS₂ films, the size and density of the NPs can be controlled. The resulting hybrid materials are demonstrated as efficient Raman active surfaces for the detection of aromatic molecules with high sensitivity.     

Many‐Body Complexes in 2D Semiconductors

2D semiconductors such as transition metal dichalcogenides (TMDs) and black phosphorus (BP) are currently attracting great attention due to their intrinsic bandgaps and strong excitonic emissions, making them potential candidates for novel optoelectronic applications. Optoelectronic devices fabricated from 2D semiconductors exhibit many‐body complexes (exciton, trion, biexciton, etc.) which determine the materials optical and electrical properties. Characterization and manipulation of these complexes have become a reality due to their enhanced binding energies as a direct result from reduced dielectric screening and enhanced Coulomb interactions in the 2D regime. Furthermore, the atomic thickness and extremely large surface‐to‐volume ratio of 2D semiconductors allow the possibility of modulating their inherent optical, electrical, and optoelectronic properties using a variety of different environmental stimuli. To fully realize the potential functionalities of these many‐body complexes in optoelectronics, a comprehensive understanding of their formation mechanism is essential. A topical and concise summary of the recent frontier research progress related to many‐body complexes in 2D semiconductors is provided here. Moreover, detailed discussions covering the aspects of fundamental theory, experimental investigations, modulation of properties, and optoelectronic applications are given. Lastly, personal insights into the current challenges and future outlook of many‐body complexes in 2D semiconducting materials are presented.     

A Universal Strategy for Constructing Seamless Graphdiyne on Metal Oxides to Stabilize the Electrochemical Structure and Interface

The structural and interfacial stabilities of metal oxides (MOs) are key issues while facing the volumetric variation and intensive interfacial polarization in electrochemical applications, including lithium‐ion batteries (LIBs), supercapacitors, and catalysts. The growth of a seamless all‐carbon interfacial layer on MOs with complex dimensions is not only a scientific problem, but also a practical challenge in these fields. Here, the growth of graphdiyne under ultramild condition is successfully implemented in situ for coating MOs of complex dimensions. The seamless all‐carbon interface and conductive network are formed at the same time. This method cleverly avoids the structural degradation of MOs at a high temperature in the presence of traditional carbon materials. Under the protection of the high‐quality graphdiyne layer, the samples as LIB anodes deliver high performances in terms of Coulomb efficiency, capacity, long‐term retention, and structural and interfacial stabilities. Both experimental achievements and theoretical calculations demonstrate that the graphdiyne is a particular protection layer for MOs and plays a crucial role for preventing the structural and interfacial degradation of the electrode. Furthermore, the universality of this method will promote the potential applications of many promising MOs in other electrochemical fields.