Tailoring plasmonic interfaces for efficient hot-electron injection in perovskite-based photodetectors
摘要
A plasmonic–perovskite hybrid platform for high-sensitivity, light-assisted environmental sensing was studied. For the formation of nanoscale Schottky junctions, halide-alloyed CsPbBr₃₋ₓIₓ thin films with tunable optical bandgaps were interfaced with gold nanocubes (AuNCs). Uniform grain formation and effective AuNC anchoring within grain boundaries, forming effective plasmonic coupling sites, were ensured by structural and morphological studies. Localised surface plasmon resonance (LSPR) and interfacial hot-electron injection contributed to the hybrid’s increased broadband absorption and photoluminescence suppression, as revealed by optical characterisation. Delayed recombination and greater charge separation were established by transient absorption spectroscopy through a longer carrier lifetime (τ2 = 6.8 ps) compared to pristine films (τ2 ≈ 3.1 ps). The AuNC edges were visualized to display strong near-field enhancement that directly overlapped with the perovskite’s absorption spectrum through finite-difference time-domain (FDTD) simulation. The Au–perovskite hybrid showed enhanced photoelectrochemical sensing performance in stability, reversibility, and selectivity. It recorded a limit of detection of about 120 ppb for NO₂ and a rapid response to Pb²⁺ ions. These result evidence that the system is capable of monitoring the environment at low bias and reliability. The research offers a potential route for scalable, high-efficiency optoelectronic sensors by explicitly establishing the link between plasmon-amplified hot-carrier dynamics and sensing performance. With surface functionalisation and LSPR tunability, subsequent studies can extend this approach to multiplexed chemical and biosensing applications.
Graphical abstractThe plasmonic–perovskite hybrid structure for enhanced environmental sensing is illustrated in this graphical abstract. Under light stimulation, a gold nanocube (Au) placed on top of a CsPbBr₃₋ₓIₓ thin film forms a Schottky junction, allowing efficient hot-electron transport. Contact-induced localised surface plasmon resonance (LSPR) causes greater broadband optical absorption and extended carrier lifetimes. Photoelectrochemical (PEC) sensitivity towards environmental pollutants such as NO₂ and Pb²⁺ is significantly enhanced by these phenomena. The illustration illustrates the capability of the platform for low-detection-limit, high-selectivity air pollution monitoring by showing both the physical mechanism and the useful sensing advantage.