2D Ruddlesden–Popper perovskites exhibit great potential in optoelectronic devices for superior stability compared with their 3D counterparts. However, to achieve a high level of device performance, it is crucial but challenging to regulate the phase distribution of 2D perovskites to facilitate charge carrier transfer. Herein, using a solvent additive method (adding a small amount of dimethyl sulfoxide (DMSO) in N,N‐dimethylformamide (DMF)) combined with a hot‐casting process, the phase distribution of (PEA)2MA3Pb4I13 (PEA+ = C6H5CH2CH2NH3+, MA+ = CH3NH3+) perovskite can be well controlled and the Fermi level of perovskites along the film thickness direction can achieve gradient distribution. The increased built‐in potential, oriented crystal, and improved crystal quality jointly contribute to the high photoresponse of devices in the entire response spectrum range. The optimum device exhibits a characteristic detection peak at 570 nm with large responsivity/detectivity (0.44 A W−1/3.38 × 1012 Jones), ultrafast response speed with a rise/fall time of 20.8/20.6 µs, and improved stability. This work suggests the possibility of manipulating the ordered phase distribution of 2D perovskites toward high‐performance and stable optoelectronic conversion devices.

It is crucial to retard the carrier recombination and minimize the energy loss at the transparent electrode/electron transport layer (ETL)/perovskite absorber interfaces to improve the performance of the perovskite solar cells (PSCs). Here, a bilayered TiO2/WO3 film is designed as ETL by combining atomic layer deposition (ALD) technology and spin‐coating process. The ALD‐TiO2 underlayer fills the fluorine‐doped tin oxide (FTO) valleys and makes the surface smoother, which effectively avoids the shunt pathways between perovskite layer and FTO substrate and thereby suppresses electron–hole recombination at the interface. Moreover, the presence of hydrophilic TiO2 underlayer is helpful in forming a uniform and compact WO3 layer which is beneficial for extracting electron from perovskite to ETL. Meanwhile, the lower valance band minimum level of TiO2 relative to WO3 can efficiently enhance the hole‐blocking ability. By employing the optimized TiO2 (7 nm)/WO3 bilayer as ETL, the resulting cell exhibits an obviously enhanced power conversion efficiency of up to 20.14%, which is much better than the single WO3 or TiO2 ETL based device. This work is expected to provide a viable path to design ultrathin and compact ETL for efficient PSCs.

where J ph and J d represent the photocurrent and dark current density, respectively. As shown in Figure 3e, the NIO device Adv.

There are significant applications for miniature on‐chip spectrometers in many fields. However, at present, on‐chip spectrometers have to utilize an integrated strategy to achieve spectral analysis, which undoubtedly squanders the photosensitive area and adds pressure to the miniaturization of the spectrometer. Here, a unique spectrometer design that adopts a single detection point with in situ modulation realized by the photogain control at various bias voltages is demonstrated. With micrometer‐level footprints, this single‐dot spectrometer processes a resolution of about 5 nm and a response time down to about 197 µs. This is the first in situ perovskite modulation strategy that breaks the footprint‐resolution restriction of spectrum analysis and demonstrates a new design direction for functional perovskite devices.

Transparent and flexible electronic devices are highly desired to meet the great demand for next-generation devices that are lightweight, flexible, and portable. Transparent conducting oxides (TCOs), such as indium-tin oxide, serve as fundamental components for the design of transparent and flexible electronic devices. However, indium is rare and expensive. Herein, we report the fabrication of low-cost perovskite SrVO3 TCO films on transparent and flexible mica substrates and further demonstrate their utilization as a TCO electrode for building a transparent, flexible, and self-powered perovskite photodetector. Superior stable optical transparency and electrical conductivity are retained in SrVO3 after bending up to 105 cycles. Without an external power source, the constructed all-perovskite photodetector exhibits a high responsivity (42.5 mA W–1), fast response time (3.09/1.23 ms), and an excellent flexibility and bending stability after dozens of cycles of bending at an extreme 90° bending angle. Our results demonstrate that low-cost and structure-compatible transition metal-based perovskite oxides, such as SrVO3, as TCO electrodes have huge potential for building high-performance transparent, flexible, and portable smart electronics.

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The ORCID identification number(s) for the author(s) of this article can be found under https://doi.org/10.1002/admi.202101766. Recently, organic-inorganic hybrid perovskite has gradually become the research focus in the photodetector field owing to the advantages of low cost, simple preparation process, and excellent photoelectric features, such as appropriate bandgap, high absorption coefficient, and long carrier diffusion