Jingwen Yao,Yuling Huang,Haifeng Sun,Zhiyu Wang,Jie Xue,Zhifeng Huang,Shou-Cheng Dong,Xihan Chen,Haipeng Lu
Spin light-emitting diodes (spin-LEDs) are important for spin-based electronic circuits as they convert the carrier spin information to optical polarization. Recently, chiral-induced spin selectivity (CISS) has emerged as a new paradigm to enable spin-LED as it does not require any magnetic components and operates at room temperature. However, CISS-enabled spin-LED with tunable wavelengths ranging from red to near-infrared (NIR) has yet to be demonstrated. Here, chiral quasi-2D perovskites are developed to fabricate efficient spin-LEDs with tunable wavelengths from red to NIR region by tuning the halide composition. The optimized chiral perovskite films exhibit efficient circularly polarized luminescence from 675 to 788 nm, with a photoluminescence quantum yield (PLQY) exceeding 86% and a dissymmetry factor ( g lum ) ranging from 8.5 × 10 −3 to 2.6 × 10 −2 . More importantly, direct circularly polarized electroluminescence (CPEL) is achieved at room temperature in spin-LEDs. This work demonstrated efficient red and NIR spin-LEDs with the highest external quantum efficiency (EQE) reaching 12.4% and the electroluminescence (EL) dissymmetry factors ( g EL ) ranging from 3.7 × 10 −3 to 1.48 × 10 −2 at room temperature. The composition-dependent CPEL performance is further attributed to the prolonged spin lifetime as revealed by ultrafast transient absorption spectroscopy.
Jingwen Yao,Zhiyu Wang,Yuling Huang,Jie Xue,Dengliang Zhang,Jiangshan Chen,Xihan Chen,Shou-Cheng Dong,Haipeng Lu
Introducing molecular chirality into perovskite crystal structures has enabled the control of carrier spin states, giving rise to circularly polarized luminescence (CPL) in thin films and circularly polarized electroluminescence (CPEL) in LEDs. Spin-LEDs can be fabricated either through a spin-filtering layer enabled by chiral-induced spin selectivity or a chiral emissive layer. The former requires a high degree of spin polarization and a compatible spinterface for efficient spin injection, which might not be easily integrated into LEDs. Alternatively, a chiral emissive layer can also generate circularly polarized electroluminescence, but the efficiency remains low and the fundamental mechanism is elusive. In this work, we report an efficient green LED based on quasi-two-dimensional (quasi-2D) chiral perovskites as the emitting layer (EML), where CPEL is directly produced without separate carrier spin injection. The optimized chiral perovskite thin films exhibited strong CPL at 535 nm with a photoluminescence quantum yield (PLQY) of 91% and a photoluminescence dissymmetry factor (glum) of 8.6 × 10–2. Efficient green spin-LEDs were successfully demonstrated, with a large EL dissymmetry factor (gEL) of 7.8 × 10–2 and a maximum external quantum efficiency (EQE) of 13.5% at room temperature. Ultrafast transient absorption (TA) spectroscopic study shows that the CPEL is generated from a rapid energy transfer accompanied by spin transfer from 2D to 3D perovskites. Our study not only demonstrates a reliable approach to achieve high performance spin-LEDs but also reveals the fundamental mechanism of CPEL with an emissive layer of chiral perovskites.
Spin-LEDs have been a central topic in semiconductor spintronics research and represent a promising avenue for advanced optoelectronic devices and applications. The future advancements of spin-LEDs will undoubtedly hinge on the generation and manipulation of spin-polarized population at room temperature. In this research, we elucidate the development of room-temperature spin-LEDs using quasi-2D perovskites, based on the chiral-induced spin selectivity (CISS) effect. During the carrier transfer from the chiral n2 phase to the randomly oriented high-n phase caused by the bandgap gradient distribution, CISS works to generate non-equilibrium spin population, leading to room-temperature spin-polarized fluorescence. A spin-polarization of ∼93% is observed for the films. Finally, we realize spin-LEDs at room temperature, exhibiting a |gCP-EL| value of 0.05 and an EQE of 3.8%. This work highlights the potential of integrating dual ligands to optimize the phase distribution and crystalline orientation in quasi-2D films to achieve efficient CISS for spin-LED applications.
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