We demonstrate CsPbBr3 perovskite nanocrystals with high photoluminescence quantum yield and fast down-transition lifetime as frequency down-converting material on matured silicon-based photodetectors. The hybrid photoreceiver demonstrates up to 25% increment in terms of photon-to-electron conversion and 34 megabit-per-second transmission for high-speed UVC communication link.

Hot carrier (HC) cooling is a critical photophysical process that significantly influences the optoelectronic performance of hybrid perovskite-based devices. The hot carrier extraction at the device interface is very challenging because of its ultrashort lifetime. Here, ultrafast transient reflectance spectroscopy measurements and time-domain ab initio calculations show how the dielectric constant of the organic spacers can control and slow the HC cooling dynamics in single-crystal 2D Ruddlesden–Popper hybrid perovskites. We find that (EA)2PbI4 (EA = HOC2H4NH3+) that correspond to a high dielectric constant organic spacer has a longer HC cooling time compared to that of (AP)2PbI4 (AP = HOC3H6NH3+) and (PEA)2PbI4 (PEA = C6H5C2H4NH3+). The slow HC relaxation process in the former case can be ascribed to a stronger screening of the Coulomb interactions, a small nonradiative internal conversion within the conduction bands, as well as a weak electron–phonon coupling. Our findings provide a strategy to prolong the hot carrier cooling time in low-dimensional hybrid perovskite materials by using organic spacers with reduced dielectric confinement.

We demonstrate enhancement of the photoluminescence (PL) properties of individual zero-dimensional (0D) Cs4PbBr6 perovskite nanocrystals (PNCs) upon encapsulation by alumina using an appropriately modified atomic layer deposition method. In addition to the increased PL intensity and improved long-term stability of encapsulated PNCs, our single-particle studies reveal substantial changes in the PL blinking statistics and the persistent appearance of the long-lived, “delayed” PL components. The blinking patterns exhibit a modification from the fast switching between fluorescent ON and OFF states found in bare PNCs to a behavior with longer ON states and more isolated OFF states in alumina-encapsulated PNCs. Controlled exposure of 0D nanocrystals to moisture suggests that the observed PL lifetime changes may be related to water-induced “reservoir” states that allow for longer-lived charge storage with subsequent back-feeding into the emissive states. Viable encapsulation of PNCs with metal oxides that can preserve and even enhance their PL properties can be utilized in the fabrication of extended structures on their basis for optoelectronic and photonic applications.

This review article presents and discusses the recent progress made in the stabilization, protection, improvement, and design of halide perovskite-based photocatalysts, photoelectrodes, and devices for solar-to-chemical fuel conversion. With the target of water splitting, hydrogen iodide splitting, and CO2 reduction reactions, the strategies established for halide perovskites used in photocatalytic particle-suspension systems, photoelectrode thin-film systems, and photovoltaic-(photo)electrocatalysis tandem systems are organized and introduced. Moreover, recent achievements in discovering new and stable halide perovskite materials, developing protective and functional shells and layers, designing proper reaction solution systems, and tandem device configurations are emphasized and discussed. Perspectives on the future design of halide perovskite materials and devices for solar-to-chemical fuel conversion are provided. This review may serve as a guide for researchers interested in utilizing halide perovskite materials for solar-to-chemical fuel conversion.

Optical wireless communication (OWC) using the ultra-broad spectrum of the visible-to-ultraviolet (UV) wavelength region remains a vital field of research for mitigating the saturated bandwidth of radio-frequency (RF) communication. However, the lack of an efficient UV photodetection methodology hinders the development of UV-based communication. The key technological impediment is related to the low UV-photon absorption in existing silicon photodetectors, which offer low-cost and mature platforms. To address this technology gap, we report a hybrid Si-based photodetection scheme by incorporating CsPbBr3 perovskite nanocrystals (NCs) with a high photoluminescence quantum yield (PLQY) and a fast photoluminescence (PL) decay time as a UV-to-visible colour-converting layer for high-speed solar-blind UV communication. The facile formation of drop-cast CsPbBr3 perovskite NCs leads to a high PLQY of up to ~73% and strong absorption in the UV region. With the addition of the NC layer, a nearly threefold improvement in the responsivity and an increase of ~25% in the external quantum efficiency (EQE) of the solar-blind region compared to a commercial silicon-based photodetector were observed. Moreover, time-resolved photoluminescence measurements demonstrated a decay time of 4.5 ns under a 372-nm UV excitation source, thus elucidating the potential of this layer as a fast colour-converting layer. A high data rate of up to 34 Mbps in solar-blind communication was achieved using the hybrid CsPbBr3–silicon photodetection scheme in conjunction with a 278-nm UVC light-emitting diode (LED). These findings demonstrate the feasibility of an integrated high-speed photoreceiver design of a composition-tuneable perovskite-based phosphor and a low-cost silicon-based photodetector for UV communication.

Perovskite single crystals (PSCs) are considered the next breakthrough in optoelectronics research due to their free-grain boundary and much lower density of trap states compared to those of their polycrystalline counterparts. However, the inevitable formation of triiodide-based intrinsic defects during high-temperature crystal growth is one of the major challenges impeding the further development of optoelectronic devices based on PSCs. Here, we not only identified the existence of these triiodide ions as hole-trapping centers and their tremendous negative impact on the performance of PSCs, but more importantly, we used a reduction treatment to prevent their formation during crystal growth. The removal of such defect centers resulted in much higher charge carrier mobility and longer carrier lifetime than the untreated counterparts, leading to enhanced photodetection properties. The I3–-free MAPbI3 single crystal (MSC) devices consistently generated a more than 100 times higher photocurrent than that generated by I3–-rich devices under the same light intensity.

The application of liquid-exfoliated 2D transition metal disulfides (TMDs) as the hole transport layers (HTLs) in nonfullerene-based organic solar cells is reported. It is shown that solution processing of few-layer WS2 or MoS2 suspensions directly onto transparent indium tin oxide (ITO) electrodes changes their work function without the need for any further treatment. HTLs comprising WS2 are found to exhibit higher uniformity on ITO than those of MoS2 and consistently yield solar cells with superior power conversion efficiency (PCE), improved fill factor (FF), enhanced short-circuit current (JSC), and lower series resistance than devices based on poly(3,4-ethylenedioxythiophene):poly(styrenesulfonate) and MoS2. Cells based on the ternary bulk-heterojunction PBDB-T-2F:Y6:PC71BM with WS2 as the HTL exhibit the highest PCE of 17%, with an FF of 78%, open-circuit voltage of 0.84 V, and a JSC of 26 mA cm−2. Analysis of the cells' optical and carrier recombination characteristics indicates that the enhanced performance is most likely attributed to a combination of favorable photonic structure and reduced bimolecular recombination losses in WS2-based cells. The achieved PCE is the highest reported to date for organic solar cells comprised of 2D charge transport interlayers and highlights the potential of TMDs as inexpensive HTLs for high-efficiency organic photovoltaics.

Interest has been growing in defects of halide perovskites in view of their intimate connection with key material optoelectronic properties. In perovskite quantum dots (PQDs), the influence of defects is even more apparent than in their bulk counterparts. By combining experiment and theory, we report herein a halide-vacancy-driven, ligand-directed self-assembly process of CsPbBr3 PQDs. With the assistance of oleic acid and didodecyldimethylammonium sulfide, surface-Br-vacancy-rich CsPbBr3 PQDs self-assemble into nanowires (NWs) that are 20-60 nm in width and several millimeters in length. The NWs exhibit a sharp photoluminescence profile (≈18 nm full-width at-half-maximum) that peaks at 525 nm. Our findings provide insight into the defect-correlated dynamics of PQDs and defect-assisted fabrication of perovskite materials and devices.

By combining femtosecond transient reflectance (TR) spectroscopy and density functional theory (DFT) calculations, we reveal the impact of the length of the organic linkers (HOC2H4NH3+ and C6H5C2H4NH3+) and the number of inorganic layers (n = 1–3) on the hot carrier relaxation dynamics and coherent acoustic phonons in 2D Ruddlesden–Popper (RP) perovskites. We find that the interplay between the hot carriers and the coherent longitudinal acoustic phonons (CLAPs) can extend the oscillation of the TR kinetics to nanoseconds, which could lead to the higher thermal conductivities of 2D RP perovskites. Moreover, we find that the frequency of the acoustic phonon oscillation and phonon velocity decreases with the increasing number of layers due to the increased mass of the inorganic layers and reduced electron–phonon coupling. This finding provides new physical insights into how the organic spacers and number of inorganic layers control the overall carrier dynamics of 2D perovskite materials.

Halide perovskites are known to be photoconductive for more than half a century, and their efficient photocarrier generation gives rise to positive photoconductivity (PPC). In this work, the discovery of negative photoconductivity (NPC) in hybrid perovskite CH3NH3PbBr3 after Bi doping is reported. Transient photoconductivity measurements reveal a surprising bipolar behavior with a fast positive response followed by exponential negative photocurrent decay, resulting in an equilibrium photocurrent even below the dark level. The NPC effect in Bi-doped CH3NH3PbBr3 is among the largest ones reported so far for semiconductors. It is proposed that the transition to negative photoconductance is related to the presence of DX-like centers in Bi-doped halide perovskites, similar to doped III–V and chalcopyrite semiconductors. Such photogenerated DX-like centers in the Bi-doped CH3NH3PbBr3 can trap mobile band electrons and enhance charge recombination, thus reducing the conductivity. This mechanism is consistent with the observations of crossover from PPC to NPC as functions of temperature, composition, and illumination. The results underscore the importance of defect engineering for tuning the optoelectronic properties of halide perovskites.