Slow hot carrier (HC) cooling resulting from hot phonon bottleneck has been widely demonstrated in metal halide perovskites. Although manipulating HC kinetics in these materials is of both fundamental and technological importance, this task remains a daunting challenge. Here, via interfacial engineering, i.e., epitaxial growth of Cs 4 PbBr 6 on CsPbBr 3 nanocrystals (NCs), we have revealed an obvious shortening of HC cooling times, evidenced by transient absorption and ultrafast PL spectra. Collaborated with the longitudinal optical (LO) phonon model, theoretical calculations verify the breaking of the hot phonon bottleneck in CsPbBr 3 @Cs 4 PbBr 6 and identify the interfacial electron-LO phonon coupling as the leading mechanism for the observed large tuning of HC cooling times. Especially, the participation of LO phonons from Cs 4 PbBr 6 enables the efficient Klemens channel for hot phonon decay. Our findings establish an effective method to tailor HC dynamics in perovskite NCs, which could be conducive to improving the performance of optoelectronic applications.
Bi2O2Se, a high‐mobility and air‐stable 2D material, has attracted substantial attention for application in integrated logic electronics and optoelectronics. However, achieving an overall high performance over a wide spectral range for Bi2O2Se‐based devices remains a challenge. A broadband phototransistor with high photoresponsivity (R) is reported that comprises high‐quality large‐area (≈180 µm) Bi2O2Se nanosheets synthesized via a modified chemical vapor deposition method with a face‐down configuration. The device covers the ultraviolet (UV), visible (Vis), and near‐infrared (NIR) wavelength ranges (360–1800 nm) at room temperature, exhibiting a maximum R of 108 696 A W−1 at 360 nm. Upon illumination at 405 nm, the external quantum efficiency, R, and detectivity (D*) of the device reach up to 1.5 × 107%, 50055 A W−1, and 8.2 × 1012 Jones, respectively, which is attributable to a combination of the photogating, photovoltaic, and photothermal effects. The devices reach a −3 dB bandwidth of 5.4 kHz, accounting for a fast rise time (τrise) of 32 µs. The high sensitivity, fast response time, and environmental stability achieved simultaneously in these 2D Bi2O2Se phototransistors are promising for high‐quality UV and IR imaging applications.
Graphene has been widely investigated for use in high-performance photodetectors due to its broad absorption band and high carrier mobility. While exhibiting remarkably strong absorption in the ultraviolet range, the fabrication of a large-scale integrable, graphene-based ultraviolet photodetector with long-term stability has proven to be a challenge. Here, using graphene as a template for C assembly, we synthesized a large-scale all-carbon hybrid film with inherently strong and tunable UV aborption. Efficient exciton dissociation at the heterointerface and enhanced optical absorption enables extremely high photoconductive gain, resulting in UV photoresponsivity of ∼10 A/W. Interestingly, due to the electron-hole recombination process at the heterointerface, the response time can be modulated by the gate voltage. More importantly, the use of all-carbon hybrid materials ensures robust operation and further allows the demonstration of an exemplary 5 × 5 (2-dimensional) photodetector array. The devices exhibit negligible degradation in figures of merit even after 2 month of operation, indicating excellent environmental robustness. The combination of high responsivity, reliability, and scalable processability makes this new all-carbon film a promising candidate for future integrable optoelectronics.
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