Dr Shunran Li

Abstract:

Recently, Bi-doped Cs₂ Ag_0.6 Na_0.4 InCl₆ lead-free double perovskites demonstrating efficient warm-white emission have been reported. To enable the solution processing and enrich the application fields of this promising material, here a colloidal synthesis of Cs₂ Ag_{1- x} Na_x In_{1- y} Bi_y Cl₆ nanocrystals is further developed. Different from its bulk states, the emission color temperatures of the nanocrystal can be tuned from 9759.7 to 4429.2 K by Na⁺ and Bi³⁺ incorporation. Furthermore, the newly developed nanocrystals can break the wavefunction symmetry of the self-trapped excitons by partial replacement of Ag⁺ ions with Na⁺ ions and consequently allow radiative recombination. Assisted with Bi³⁺ ions doping and ligand passivation, the photoluminescence quantum yield of the Cs₂ Ag_0.17 Na_0.83 In_0.88 Bi_0.12 Cl₆ nanocrystals is further promoted to 64%, which is the highest value for lead-free perovskite nanocrystals at present. The new colloidal nanocrystals with tunable color temperature and efficient photoluminescence are expected to greatly advance the research progress of lead-free perovskites in single-emitter-based white emitting materials and devices.

Abstract:

Photoluminescence is a radiative recombination process of electron-hole pairs. Self-trapped excitons (STEs), occurring in a material with soft lattice and strong electron-phonon coupling, emit photons with broad spectrum and large Stokes shift. Recently, series halide perovskites with efficient STE emission have been reported and showed promise for solid-state lighting. In this Perspective, we present an overview of various photoluminescence phenomena with the emphasis on the mechanism and characteristics of emission derived from STEs. This is followed by the introduction of STE emission in hybrid halide perovskites. We then introduce all-inorganic STE emitters and focus in particular on the mechanism of STEs in double-perovskite Cs₂AgInCl₆ and strategies for efficiency improvement. Finally, we summarize the current photoluminescence and electroluminescence applications of STE emitters as well as the potential in luminescent solar concentrators and provide an overview of future research opportunities.

Abstract:

Lighting accounts for one-fifth of global electricity consumption¹. Single materials with efficient and stable white-light emission are ideal for lighting applications, but photon emission covering the entire visible spectrum is difficult to achieve using a single material. Metal halide perovskites have outstanding emission properties^2,3; however, the best-performing materials of this type contain lead and have unsatisfactory stability. Here we report a lead-free double perovskite that exhibits efficient and stable white-light emission via self-trapped excitons that originate from the Jahn-Teller distortion of the AgCl₆ octahedron in the excited state. By alloying sodium cations into Cs₂AgInCl₆, we break the dark transition (the inversion-symmetry-induced parity-forbidden transition) by manipulating the parity of the wavefunction of the self-trapped exciton and reduce the electronic dimensionality of the semiconductor⁴. This leads to an increase in photoluminescence efficiency by three orders of magnitude compared to pure Cs₂AgInCl₆. The optimally alloyed Cs₂(Ag_0.60Na_0.40)InCl₆ with 0.04 per cent bismuth doping emits warm-white light with 86 ± 5 per cent quantum efficiency and works for over 1,000 hours. We anticipate that these results will stimulate research on single-emitter-based white-light-emitting phosphors and diodes for next-generation lighting and display technologies.