Van der Waals heterostructures consisting of graphene and transition metal dichalcogenides have shown great promise for optoelectronic applications. However, an in-depth understanding of the critical processes for device operation, namely, interfacial charge transfer (CT) and recombination, has so far remained elusive. Here, we investigate these processes in graphene-WS2 heterostructures by complementarily probing the ultrafast terahertz photoconductivity in graphene and the transient absorption dynamics in WS2 following photoexcitation. We observe that separated charges in the heterostructure following CT live extremely long: beyond 1 ns, in contrast to ~1 ps charge separation reported in previous studies. This leads to efficient photogating of graphene. Furthermore, for the CT process across graphene-WS2 interfaces, we find that it occurs via photo-thermionic emission for sub-A-exciton excitations and direct hole transfer from WS2 to the valence band of graphene for above-A-exciton excitations. These findings provide insights to further optimize the performance of optoelectronic devices, in particular photodetection.

Graphitic carbon nitrides have appeared as a new type of photocatalyst for water splitting, but their broader and more practical applications are oftentimes hindered by the insolubility or difficult dispersion of the material in solvents. We herein prepared novel two-dimensional (2D) carbon nitride-type polymers doped by iron under a mild one-pot method through preorganizing formamide and citric acid precursors into supramolecular structures, which eventually polycondensed into a homogeneous organocatalyst for highly efficient visible light-driven hydrogen evolution with a rate of ∼16.2 mmol g(-1) h(-1) and a quantum efficiency of 0.8%. Laser photolysis and electrochemical impedance spectroscopic measurements suggested that iron-doping enabled strong electron coupling between the metal and the carbon nitride and formed unique electronic structures favoring electron mobilization along the 2D nanomaterial plane, which might facilitate the electron transfer process in the photocatalytic system and lead to efficient H2 evolution. In combination with electrochemical measurements, the electron transfer dynamics during water reduction were depicted, and the earth-abundant Fe-based catalyst may open a sustainable strategy for conversion of sunlight into hydrogen energy and cope with current challenging energy issues worldwide.

Ultrathin uniform BP nanosheets with lateral dimensions of up to several tens of micrometers were prepared via a small molecule-assisted liquid phase exfoliation method, which exhibited attractive electron accepting abilities from photosensitizers and was thus promising in diverse applications such as photocatalysis and photovoltaics.

Ultrathin 2D molybdenum disulfide (MoS2), which is the flagship of 2D transition‐metal dichalcogenide nanomaterials, has drawn much attention in the last few years. 2D MoS2 has been banked as an alternative to platinum for highly active hydrogen evolution reaction because of its low cost, high surface‐to‐volume ratio, and abundant active sites. However, when MoS2 is used directly as a photocatalyst, contrary to public expectation, it still performs poorly due to lateral size, high recombination ratio of excitons, and low optical cross section. Besides, simply compositing MoS2 as a cocatalyst with other semiconductors cannot satisfy the practical application, which stimulates the pursual of a comprehensive insight into recent advances in synthesis, properties, and enhanced hydrogen production of MoS2. Therefore, in this Review, emphasis is given to synthetic methods, phase transitions, tunable optical properties, and interfacial engineering of 2D MoS2. Abundant ways of band edge tuning, structural modification, and phase transition are addressed, which can generate the neoteric photocatalytic systems. Finally, the main challenges and opportunities with respect to MoS2 being a cocatalyst and coherent light–matter interaction of MoS2 in photocatalytic systems are proposed.

Ultrathin BP QDs with a uniform size of ∼3.4 nm were prepared via small molecule-assisted liquid phase exfoliation and they exhibited superior broadband nonlinear saturable absorption promising for nonlinear optical applications. Laser photolysis measurement implied that the nonlinear response origin was related to the long-lived electron-hole pairs delocalized within the BP QDs.

For decades, ultrafast time‐resolved spectroscopy has found its way into an increasing number of applications. It has become a vital technique to investigate energy conversion processes and charge transfer dynamics in optoelectronic systems such as solar cells and solar‐driven photocatalytic applications. The understanding of charge transfer and photochemical reactions can help optimize and improve the performance of relevant devices with solar energy conversion processes. Here, the fundamental principles of photochemical and photophysical processes in photoinduced reactions, in which the fundamental charge carrier dynamic processes include interfacial electron transfer, singlet excitons, triplet excitons, excitons fission, and recombination, are reviewed. Transient absorption (TA) spectroscopy techniques provide a good understanding of the energy/electron transfer processes. These processes, including excited state generation and interfacial energy/electron transfer, are dominate constituents of solar energy conversion applications, for example, dye‐sensitized solar cells and photocatalysis. An outlook for intrinsic electron/energy transfer dynamics via TA spectroscopic characterization is provided, establishing a foundation for the rational design of solar energy conversion devices.

Near-infrared-emitting CuGaS2/CdS QDs with enhanced visible light absorption were developed to achieve high efficiency photoelectrochemical cells.

To overcome the bottleneck of water splitting, the exploration of efficient, selective, and stable water oxidation catalysts (WOCs) is crucial. We report an all-inorganic, oxidatively and hydrolytically stable WOC based on a polyoxometalate [(A-α-SiW9 O34)2Co8(OH)6(H2O)2(CO3)3](16-) (Co8 POM). As a cobalt(II)-based cubane water oxidation catalyst, Co8POM embeds double Co(II)4O3 cores. The self-assembled catalyst is similar to the oxygen evolving complex (OEC) of photosystem II (PS II). Using [Ru(bpy)3](2+) as a photosensitizer and persulfate as a sacrificial electron acceptor, Co8POM exhibits excellent water oxidation activity with a turnover number (TON) of 1436, currently the highest among bioinspired catalysts with a cubical core, and a high initial turnover frequency (TOF). Investigation by several spectroscopy, spectrometry, and other techniques confirm that Co8POM is a stable and efficient catalyst for visible light-driven water oxidation. The results offer a useful insight into the design of water oxidation catalysts.