Novel quantum-dot light-emitting diodes based on all-inorganic perovskite CsPbX3 (X = Cl, Br, I) nanocrystals are reported. The well-dispersed, single-crystal quantum dots (QDs) exhibit high quantum yields, and tunable light emission wavelength. The demonstration of these novel perovskite QDs opens a new avenue toward designing optoelectronic devices, such as displays, photodetectors, solar cells, and lasers.

Solution-processed CsPbBr quantum-dot light-emitting diodes with a 50-fold external quantum efficiency improvement (up to 6.27%) are achieved through balancing surface passivation and carrier injection via ligand density control (treating with hexane/ethyl acetate mixed solvent), which induces the coexistence of high levels of ink stability, photoluminescence quantum yields, thin-film uniformity, and carrier-injection efficiency.

Printed flexible photodetectors based on 2D inorganic perovskites with atomic thickness show excellent photosensing with fast rise and decay response times. As-synthesized nanosheets can easily be dispersed in various solvents, leading to large-area, crack-free, low-roughness, flexible films after printing. This study demonstrates that all-inorganic perovskite CsPbX3 nanosheets as a new class of 2D semiconductors have huge potential for flexible optoelectronic applications.

All-inorganic perovskites have high carrier mobility, long carrier diffusion length, excellent visible light absorption, and well overlapping with localized surface plasmon resonance (LSPR) of noble metal nanocrystals (NCs). The high-performance photodetectors can be constructed by means of the intrinsic outstanding photoelectric properties, especially plasma coupling. Here, for the first time, inorganic perovskite photodetectors are demonstrated with synergetic effect of preferred-orientation film and plasmonic with both high performance and solution process virtues, evidenced by 238% plasmonic enhancement factor and 10 on/off ratio. The CsPbBr and Au NC inks are assembled into high-quality films by centrifugal-casting and spin-coating, respectively, which lead to the low cost and solution-processed photodetectors. The remarkable near-field enhancement effect induced by the coupling between Au LSPR and CsPbBr photogenerated carriers is revealed by finite-difference time-domain simulations. The photodetector exhibits a light on/off ratio of more than 10 under 532 nm laser illumination of 4.65 mW cm . The photocurrent increases from 0.67 to 2.77 μA with centrifugal-casting. Moreover, the photocurrent rises from 245.6 to 831.1 μA with Au NCs plasma enhancement, leading to an enhancement factor of 238%, which is the most optimal report among the LSPR-enhanced photodetectors, to the best of our knowledge. The results of this study suggest that all-inorganic perovskites are promising semiconductors for high-performance solution-processed photodetectors, which can be further enhanced by Au plasmonic effect, and hence have huge potentials in optical communication, safety monitoring, and biological sensing.

Visible‐infrared dual‐modal light harvesting is crucial for various optoelectronic devices, particularly for solar cells and photodetectors. For the first time, this study reports on large 25 cm3‐volume all‐inorganic perovskite CsPbBr3 single crystal (SC) with an emphasis on the observed visible‐infrared dual‐modal light harvesting and sensing as demonstrated by the high‐performance visible‐infrared dual‐modal photodetectors. First, ultralarge 25 cm3‐volume CsPbBr3 SC ingots with trapping state density as low as of 1 × 109 cm−3 have been achieved by a modified Bridgman growth method. The volume reported here is the largest CsPbX3 (X = Cl, Br, I) all‐inorganic perovskite system up to now, and the SC can be facilely cut into SC wafers with a diameter of 25 mm for various optoelectronic devices. Furthermore, these CsPbBr3 SCs exhibit a visible absorbance coefficient, a near‐infrared (IR) two‐phonon absorption coefficient, a carrier diffusion length, and a mobility as high as of 105 cm−1, 3.7 cm per Goeppert‐Mayer (GM), 10 µm and 2000 cm2 V−1 s−1, respectively. These merits match well to the requirements of high‐performance Vis‐IR dual‐modal light harvesting optoelectronic devices, which has been demonstrated by the CsPbBr3 SC photodetectors operated under the irradiation of both visible and IR light sources with light on/off ratio higher than 103. These results demonstrate the CsPbBr3 SCs with high visible‐infrared dual‐modal light harvesting capability and excellent electrical transporting properties have a huge potential in various optoelectronic devices, such as solar cells, photodetectors, and lasers.