Xinyu Shen

Abstract:

Despite the enormous developments in perovskite light-emitting diodes (PeLEDs) recently, obtaining efficient blue PeLEDs is still considered a critical challenge due to the non-radiative recombination and unbalanced charge injection caused by the unmatched carrier mobility and the deep hole-injection barrier between the hole-transport layer (HTL) and the emissive layer (EML). Herein, we incorporate tris(4-trifluoromethylphenyl)phosphine oxide (TMFPPO), obtained through a facile oxidation synthesis process, into poly(9-vinylcarbazole) (PVK). TMFPPO incorporation modulated the energy level and hole mobility of the binary-blend HTLs to eliminate the hole-injection barrier and balance the charge injection within the EML. Consequently, the blue PeLEDs with blended HTL presented an external quantum efficiency (EQE) of 7.23% centred at 477 nm, which was much higher than the EQE of a PVK device (4.95%). Our results demonstrate that modulating the energy level and charge injection of the HTL in the device is a promising method for obtaining efficient blue PeLEDs.

Abstract:

The severely insufficient operational lifetime of perovskite light-emitting diodes (LEDs) is incompatible with the rapidly increasing external quantum efficiency, even as it approaches the theoretical limit, thereby significantly impeding the commercialization of perovskite LEDs. In addition, Joule heating induces ion migration and surface defects, degrades the photoluminescence quantum yield and other optoelectronic properties of perovskite films, and induces the crystallization of charge transport layers with low glass transition temperatures, resulting in LED degradation under continuous operation. Here, a novel thermally crosslinked hole transport material, poly(FCA₆₀ -co-BFCA₂₀ -co-VFCA₂₀ ) (poly-FBV), with temperature-dependent hole mobility is designed, which is advantageous for balancing the charge injection of the LEDs and limiting the generation of Joule heating. The optimised CsPbI₃ perovskite nanocrystal LEDs with poly-FBV realise approximately a 2-fold external quantum efficiency increase over the LED with commercial hole transport layer poly(4-butyl-phenyl-diphenyl-amine) (poly-TPD), owing to the balanced carrier injection and suppressed exciton quenching. Moreover, because of the Joule heating control provided by the novel crosslinked hole transport material, the LED utilising crosslinked poly-FBV has a 150-fold longer operating lifetime (490 min) than that utilizing poly-TPD (3.3 min). The study opens a new avenue for the use of PNC LEDs in commercial semiconductor optoelectronic devices.

Abstract:

Wide-coverage near infrared (NIR) phosphor-converted LEDs possess promising potential for practical applications, but little is developed towards the efficient and wide-coverage NIR phosphors. Here, we report the single-component lanthanide (Ln³⁺ ) ions doped Cs₂ M(In_0.95 Sb_0.05 )Cl₆ (M=alkali metal) nanocrystals (NCs), exhibiting emission from 850 to 1650 nm with high photoluminescence quantum yield of 20.3 %, which is accomplished by shaping the multiple metal halide octahedra of double perovskite via the simple alkali metal substitution. From Judd-Ofelt theoretical calculation and spectroscopic investigations, the shaping of metal halide octahedra in Cs₂ M(In_1-x Sb_x )Cl₆ NCs can break the forbidden of f-f transition of Ln³⁺ , thus increasing their radiative transition rates and simultaneously boosting the energy transfer efficiency from host to Ln³⁺ . Finally, the wide-coverage NIR LEDs based on Sm³⁺ , Nd³⁺ , Er³⁺ -tridoped Cs₂ K_0.5 Rb_0.5 (In_0.95 Sb_0.05 )Cl₆ NCs are fabricated and employed in the multiplex gas sensing and night-vision application.