(411g) Molecular Design of Chiral Naphthalenediimides Cations for 1D Perovskites with Excellent Carrier Mobility and Strong Chirality

Chiral hybrid organic-inorganic perovskites (CHOIPs) have emerged as promising materials for optoelectronics and chiro-spintronics. By incorporating relatively large chiral organic cations, CHOIPs can be extended to low-dimensional crystalline phases, bringing unique electronic structures that arise from quantum confinement effects and structural distortions. Compared with 2D CHOIPs, 1D CHOIPs have stronger octahedral bond length distortion, less orbital overlap, and larger quantum confinement, resulting in higher chirality, larger band gap, but lower electrical conductivity. Therefore, the design of chiral cations with excellent charge transport ability and amplified chirality are highly desired for 1D CHOIPs. Here, we demonstrate a molecular design strategy to utilize the n-type semiconducting material naphthalenediimide (NDI) as the core of the chiral cation to achieve superior chirality and carrier mobility in the corresponding 1D perovskites. We have synthesized chiral NDI-based cations, namely (R)/(S)-NDIEPAI, by introducing (R)/(S)-propane-1,2-diamine, ethylamine, and iodide ion to the NDI core. The (R)/(S)-NDIEPAI thin film annealed at 200°C exhibited crystallization with strong chirality of 3000 medg, superior g-factor of 4 × 10^-2, and a unique 30° tilted edge-on lamellar orientation. These features suggest that the designed (R)/(S)-NDIEPAI are highly promising as chiral cations for perovskites. The corresponding 1D (R)/(S)-NDIEPAPbI₃ perovskite thin film at 200 °C showed chirality larger than 100 medg with g-factor over 2 × 10^-3, indicating the successful chirality transfer from the chiral cations to the inorganic frameworks. The strong emission quenching of (R)/(S)-NDIEPAPbI₃ was observed, suggesting the efficient charge separation in 1D (R)/(S)-NDIEPAPbI₃. The carrier mobility of 1D (R)/(S)-NDIEPAPbI₃ will be studied through the space charge-limited current measurement of hole-only and electron-only devices, and the direct detection of circular polarized light will be realized through (R)/(S)-NDIEPAPbI₃-based photodiodes.