Interface engineering in two-dimensional heterostructures towards novel emitters

Two-dimensional(2D) semiconductors have captured broad interest as light emitters, due to their unique excitonic effects. These layer-blocks can be integrated through van der Waals assembly, i.e., fabricating homo-or heterojunctions, which show novel emission properties caused by interface engineering. In this review, we will first give an overview of the basic strategies that have been employed in interface engineering, including changing components, adjusting interlayer gap, and tuning twist angle. By modifying the interfacial factors, novel emission properties of emerging excitons are unveiled and discussed. Generally, well-tailored interfacial energy transfer and charge transfer within a 2D heterostructure cause static modulation of the brightness of intralayer excitons. As a special case, dynamically correlated dual-color emission in weakly-coupled bilayers will be introduced, which originates from intermittent interlayer charge transfer. For homobilayers and type Ⅱ heterobilayers, interlayer excitons with electrons and holes residing in neighboring layers are another important topic in this review. Moreover, the overlap of two crystal lattices forms moiré patterns with a relatively large period, taking effect on intralayer and interlayer excitons. Particularly, theoretical and experimental progresses on spatially modulated moiré excitons with ultra-sharp linewidth and quantum emission properties will be highlighted. Moiré quantum emitter provides uniform and integratable arrays of single photon emitters that are previously inaccessible, which is essential in quantum many-body simulation and quantum information processing. Benefiting from the optically addressable spin and valley indices, 2D heterostructures have become an indispensable platform for investigating exciton physics, designing and integrating novel concept emitters.

二维材料最新研究进展

Research on two-dimensional(2D) materials has been explosively increasing in last seventeen years in varying subjects including condensed matter physics, electronic engineering, materials science, and chemistry since the mechanical exfoliation of graphene in 2004. Starting from graphene, 2D materials now have become a big family with numerous members and diverse categories. The unique structural features and physicochemical properties of 2D materials make them one class of the most appealing candidates for a wide range of potential applications. In particular, we have seen some major breakthroughs made in the field of 2D materials in last five years not only in developing novel synthetic methods and exploring new structures/properties but also in identifying innovative applications and pushing forward commercialisation. In this review, we provide a critical summary on the recent progress made in the field of 2D materials with a particular focus on last five years. After a brief backgroundintroduction, we first discuss the major synthetic methods for 2D materials, including the mechanical exfoliation, liquid exfoliation, vapor phase deposition, and wet-chemical synthesis as well as phase engineering of 2D materials belonging to the field of phase engineering of nanomaterials(PEN). We then introduce the superconducting/optical/magnetic properties and chirality of 2D materials along with newly emerging magic angle 2D superlattices. Following that, the promising applications of 2D materials in electronics, optoelectronics, catalysis, energy storage, solar cells, biomedicine, sensors, environments, etc. are described sequentially. Thereafter, we present the theoretic calculations and simulations of 2D materials. Finally, after concluding the current progress, we provide some personal discussions on the existing challenges and future outlooks in this rapidly developing field.

Predictably synthesizing a library of white-light-emitting perovskites

The low-dimensional organic-inorganic halide perovskites with self-trapped exciton emission have promising prospects for single-phase white-light emitters. However, so far, these broadband white-light-emitting(BWLE) perovskites were synthesized by trial-and-error testing spacing molecules. Here, we developed a steric hindrance regulation strategy to predictably synthesize BWLE perovskites. The molecules containing C–C(–NH_(2))–C groups were introduced into low-dimensional perovskites, which brings a large steric hindrance in-plane orientation. The bigger C–C(–NH_(2))–C bond angle would induce larger structural distortion in perovskites, which leads to the higher rate of self-trapping of excitons and the deeper self-trapping depth. The photoluminescence spectra of the synthesized perovskites can cover the cool-to-warm white light region. Overall, we fabricated a material library consisting of 40 kinds of BWLE compounds according to this strategy. Our findings develop a general strategy to synthesize BWLE perovskites and offer a material platform for optoelectronic applications.

碳酸物种和氯离子对生物磷灰石磷酸钙成核的影响

磷灰石是骨骼和牙齿等生物硬组织的主要无机成分,对脊椎动物至关重要.生物系统的体液中普遍存在碳酸物种和Cl^(-)离子,了解这些阴离子对生物磷灰石成核过程的影响有助于解释生物矿化的控制作用.理论研究表明,Ca-O配位数在CaP成核和CaP与添加剂的界面相互作用中是一个重要描述符.CaP团簇最外层的Ca^(2+)离子能够通过静电作用吸引碳酸物种和Cl^(-)离子,从而促进CaP相的形成.在碳酸物种和Cl^(-)离子存在的情况下,钙磷石(DCPD)可以转化为羟基磷灰石(HA).平衡氧同位素分馏和振动光谱分析结果表明,Cl^(-)离子掺杂的B型HA是最有可能的生物磷灰石.上述结果可以指导阴离子掺杂的具有生物功能的磷灰石材料的合成.

Temperature-driven reversible structural transformation and conductivity switching in ultrathin Cu_(9)S_(5)crystals

Two-dimensional(2D)materials with reversible phase transformation are appealing for their rich physics and potential applications in information storage.However,up to now,reversible phase transitions in 2D materials that can be driven by facile nondestructive methods,such as temperature,are still rare.Here,we introduce ultrathin Cu_(9)S_(5)crystals grown by chemical vapor deposition(CVD)as an exemplary case.For the first time,their basic electrical properties were investigated based on Hall measurements,showing a record high hole carrier density of~1022 cm^(-3) among 2D semiconductors.Besides,an unusual and repeatable conductivity switching behavior at~250 K were readily observed in a wide thickness range of CVD-grown Cu_(9)S_(5)(down to 2 unit-cells).Confirmed by in-situ selected area electron diffraction,this unusual behavior can be ascribed to the reversible structural phase transition between the room-temperature hexagonalβphase and low-temperatureβ’phase with a superstructure.Our work provides new insights to understand the physical properties of ultrathin Cu_(9)S_(5)crystals,and brings new blood to the 2D materials family with reversible phase transitions.

Interfacial charge and energy transfer in van der Waals heterojunctions

Van der Waals heterojunctions are fast-emerging quantum structures fabricated by the controlled stacking of two-dimensional(2D)materials.Owing to the atomically thin thickness,their carrier properties are not only determined by the host material itself,but also defined by the interlayer interactions,including dielectric environment,charge trapping centers,and stacking angles.The abundant constituents without the limitation of lattice constant matching enable fascinating electrical,optical,and magnetic properties in van der Waals heterojunctions toward next-generation devices in photonics,optoelectronics,and information sciences.This review focuses on the charge and energy transfer processes and their dynamics in transition metal dichalcogenides(TMDCs),a family of quantum materials with strong excitonic effects and unique valley properties,and other related 2D materials such as graphene and hexagonalboron nitride.In the first part,we summarize the ultrafast charge transfer processes in van der Waals heterojunctions,including its experimental evidence and theoretical understanding,the interlayer excitons at the TMDC interfaces,and the hot carrier injection at the graphene/TMDCs interface.In the second part,the energy transfer,including both Förster and Dexter types,are reviewed from both experimental and theoretical perspectives.Finally,we highlight the typical charge and energy transfer applications in photodetectors and summarize the challenges and opportunities for future development in this field.

Controlled growth of two-dimensional InAs single crystals via van der Waals epitaxy

Two-dimensional(2D)indium arsenide(InAs)is promising for future electronic and optoelectronic applications such as highperformance nanoscale transistors,flexible and wearable devices,and high-sensitivity broadband photodetectors,and is advantageous for its heterogeneous integration with Si-based electronics.However,the synthesis of 2D InAs single crystals is challenging because of the nonlayered structure.Here we report the van der Waals epitaxy of 2D InAs single crystals,with their thickness down to 4.8 nm,and their lateral sizes up to~37μm.The as-grown InAs flakes have high crystalline quality and are homogenous.The thickness can be tuned by growth time and temperature.Moreover,we explore the thickness-dependent optical properties of InAs flakes.Transports measurement reveals that 2D InAs possesses high conductivity and high carrier mobility.Our work introduces InAs to 2D materials family and paves the way for applying 2D InAs in high-performance electronics and optoelectronics.