Abstract2D transition metal dichalcogenide (2D‐TMD) materials and their van der Waals heterostructures (vdWHs) have inspired worldwide efforts in the fields of electronics and optoelectronics. However, photodetectors based on 2D/2D vdWHs suffer from performance limitations due to the weak optical absorption of their atomically thin nature. In this work, taking advantage of an excellent light absorption coefficient, low‐temperature solution‐processability, and long charge carrier diffusion length, all‐inorganic halides perovskite CsPbI3− xBrx quantum dots are integrated with monolayer MoS2 for high‐performance and low‐cost photodetectors. A favorable energy band alignment facilitating interfacial photocarrier separation and efficient carrier injection into the MoS2 layer inside the 0D–2D mixed‐dimensional vdWHs are confirmed by a series of optical characterizations. Owing to the synergistic effect of the photogating mechanism and the modulation of Schottky barriers, the corresponding phototransistor exhibits a high photoresponsivity of 7.7 × 104 A W−1, a specific detectivity of ≈5.6 × 1011 Jones, and an external quantum efficiency exceeding 107%. The demonstration of such 0D–2D mixed‐dimensional heterostructures proposed here would open up a wide realm of opportunities for designing low‐cost, flexible transparent, and high‐performance optoelectronics.

Fundamental understanding of charge behavior inside heterostructures is of vital importance for advancing high-performance optoelectronic applications. However, the charge behavior of 0D-2D mixed-dimensional van der Waals heterostructures (MvdWHs) in the photoexcited state remains elusive. In this work, an energy band alignment protocol is adopted to realize effective energy band structure engineering inside 0D-2D MvdWHs of perovskite quantum dots and MoS 2 monolayer with precisely designed typical type I and type II heterostructures, respectively. A profile and in-depth understanding of interfacial photoinduced charge behavior is determined from two opposite perspectives based on MvdWHs. Sufficient comparison of a series of optical characterization results, including Raman shift, quenched photoluminescence, visualized suppressed fluorescence intensity, and shortened fluorescence lifetime imaging, clearly verifies that interfacial charge behavior can be tailored by varying the band alignment in 0D-2D MvdWHs. Furthermore, the photoresponse performance and the relatively stronger and weaker photogating effects of such MvdWH-based phototransistors also demonstrate modulation of interfacial charge behavior in 0D-2D MvdWHs via energy band structure engineering, which is still feasible for optoelectronic performance optimization. These results are expected to shed light on designing novel functional devices and advancing the development process of 0D-2D MvdWHs in the foreseeable future.proposed stacked van der Waals heterostructures (vdWHs) have inspired worldwide efforts with rapid development of 2D materials. Such layer-by-layer assembled vdWHs could benefit from the high carrier mobilities, large surface-to-volume ratios, and especially flexible and semitransparent properties of atomically thin 2D materials. [4] However, the enhanced interlayer Coulombic interactions and Auger scattering processes in these 2D/2D vdWHs [5] as well as the inability to easily tune the energy band alignment for of the two given 2D layered materials has a great influence on the interfacial charge behavior, which is crucial to the performance of heterostructure-based functional devices. More recently, another type of vdWH was developed by integrating sizetunable semiconducting OD quantum dots (QDs) with 2D layered materials. This type of 0D-2D mixed-dimensional van der Waals heterostructure (MvdWH) has been demonstrated to possess various advantages, such as reduced Coulombic interactions, [6] easy preparation, and less constrained interfacial states. In addition, the interface in MvdWHs is more complex than that in conventional heterostructures, inducing interfacial disorder, synergistic effects, proximity effects, abrupt transitions of state density, and many other intriguing phenomena or properties. [4b,7] Hence, by combining the various remarkable optical properties of 0D-QDs with the unusual physical properties of 2D layered materials, 0D-2D MvdWHs may generate a fascinating interfacial charge behavior and exciting device performanc...

The matching of charge transport layer and photoactive layer is critical in solar energy conversion devices, especially for planar perovskite solar cells based on the SnO2 electron‐transfer layer (ETL) owing to its unmatched photogenerated electron and hole extraction rates. Graphdiyne (GDY) with multi‐roles has been incorporated to maximize the matching between SnO2 and perovskite regarding electron extraction rate optimization and interface engineering towards both perovskite crystallization process and subsequent photovoltaic service duration. The GDY doped SnO2 layer has fourfold improved electron mobility due to freshly formed C−O σ bond and more facilitated band alignment. The enhanced hydrophobicity inhibits heterogeneous perovskite nucleation, contributing to a high‐quality film with diminished grain boundaries and lower defect density. Also, the interfacial passivation of Pb−I anti‐site defects has been demonstrated via GDY introduction.

The simultaneous and efficient evolution of hydrogen and oxygen with earth-abundant, highly active, and robust bifunctional electrocatalysts is a significant concern in water splitting. Herein, non-noble metalbased Ni-Co-S bifunctional catalysts with tunable stoichiometry and morphology are realized. The engineering of electronic structure and subsequent morphological design synergistically contributes to significantly elevated electrocatalytic performance. Stable overpotentials (η 10 ) of 243 mV (vs reversible hydrogen electrode) for oxygen evolution reaction (OER) and 80 mV for hydrogen evolution reaction (HER), as well as Tafel slopes of 54.9 mV dec −1 for OER and 58.5 mV dec −1 for HER, are demonstrated. In addition, density functional theory calculations are performed to determine the optimal electronic structure via the electron density differences to verify the enhanced OER activity is related to the Co top site on the (110) surface. Moreover, the tandem bifunctional NiCo 2 S 4 exhibit a required voltage of 1.58 V (J = 10 mA cm −2 ) for simultaneous OER and HER, and no obvious performance decay is observed after 72 h. When integrated with a GaAs solar cell, the resulting photoassisted water splitting electrolyzer shows a certified solar-to-hydrogen efficiency of up to 18.01%, further demonstrating the feasibility of engineering protocols and the promising potential of bifunctional NiCo 2 S 4 for large-scale overall water splitting.

The Lewis acid–base adduct approach has been widely used to form high‐crystalline perovskite films, but the complicated crystallization pathway and underlying film formation mechanism are still ambiguous. Here, the detailed crystallization process of perovskites manipulated by Lewis base additives has been revealed by in situ X‐ray scattering measurements. Through monitoring the film formation process, two distinct crystal growth stages have been definitely recognized: i) an intermediate phase‐dominated stage; and ii) a phase transformation stage from intermediates to crystalline perovskite phase. Incorporating Lewis base additives significantly prolongs the duration of stage 1 and induces a postponed phase transformation pathway, which could be responsible for retardant crystallization kinetics. Based on a series of experimental results and theoretical calculations, it is indicated that the manipulation of perovskite crystallization pathway is a result of the modulated molecular interactions between Lewis base additives and solution precursors. Owing to the retardant crystallization kinetics, enhanced‐quality perovskite films with reduced defect density and improved optoelectronic properties, as well as optimized photovoltaic performance have been demonstrated. This work provides in‐depth understanding with respect to perovskite crystallization pathway modulated by Lewis base additives and perceptive guidelines for precise regulation of crystallization kinetics of perovskite film toward high performance.

Metal–halide hybrid perovskites have prompted the prosperity of the sustainable energy field and simultaneously demonstrated their great potential in meeting both the growing consumption of energy and the increasing social development requirements.

Photoelectrochemical water splitting via consumption of solar energy is considered an alternative approach to address both fossil resource and global warming issues. On the basis of the bottom‐up technique, major strategies have been developed to enrich the complexity of nanostructures by incorporating various functional components to realize outstanding photoelectrochemical (PEC) performance for hydrogen evolution, such as high solar‐to‐hydrogen efficiency and long‐term stability. In such a PEC system, each nanomaterial component individually, and more importantly, together with the formed interfaces, contributes to PEC performance elevation. Specifically, the two types of interfaces that have emerged, i.e., the interfaces between photoelectrodes and electrolytes (solid–liquid contact) and the interfaces inside photoelectrodes (solid–solid contact), have both been effectively engineered to facilitate charge separation and transportation and even enhance the antiphotocorrosion properties. A comprehensive understanding, summary, and review of such interface engineering protocols may provide novel and effective approaches for PEC system designing.

We report a universal phase reconfiguration phenomenon and a doping strategy to enhance the activity of multivalent nickel sulfides in hydrogen evolution. Based on these, a life-time dynamic structure-activity correlation has been established.