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Efficient and stable emission of warm-white light from lead-free halide double perovskites
摘要： 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 properties2,3; 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(Ag0.60Na0.40)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.
关键词： lead-free halide double perovskites,self-trapped excitons,white-light emission,photoluminescence efficiency,Jahn–Teller distortion
更新于2025-09-23 15:21:21
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Colloidal Synthesis of Ternary Copper Halides Nanocrystals for High-Efficiency Deep-Blue Light-Emitting Diodes with a Half-Lifetime Above 100 Hours
摘要： Currently, the blue perovskite light-emitting diodes (PeLEDs) suffer from a compromise in lead-toxicity and poor operation stability, and most previous studies have struggled to meet the crucial blue NTSC standard. In this study, electrically-driven deep-blue LEDs (~445 nm) based on zero-dimensional (0D) Cs3Cu2I5 nanocrystals (NCs) were demonstrated with the color coordinates of (0.16, 0.07) and a high external quantum efficiency of ~1.12%, comparable with the best-performing blue LEDs based on lead-halide perovskites. Encouraged by the remarkable stability of Cs3Cu2I5 NCs against heat and environmental oxygen/moisture, the proposed device was operated in a continuous current mode for 170 h, producing a record half-lifetime of ~108 h. The device stability was further verified by an aggressive thermal cycling test (300?360?300 K) and a 35-day storage test. Together with the eco-friendly features and facile colloidal synthesis technique, the 0D Cs3Cu2I5 NCs can be therefore regarded as a promising candidate for deep-blue LEDs applications.
关键词： self-trapped excitons,light-emitting diodes,stability,Cs3Cu2I5 nanocrystals,deep-blue
更新于2025-09-23 15:21:01
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Mn-doped 2D Sn-based perovskites with energy transfer from self-trapped excitons to dopants for warm white light-emitting diodes
摘要： Mn-doped 2D perovskite powders are promising phosphors for warm white light-emitting diodes (LEDs). However, it remains a challenge to solve the problem of lead toxicity and improve photoluminescence quantum yields (PLQYs). Here, we have successfully prepared Mn-doped 2D Sn-based perovskite materials ((C8H17NH2)2Sn1-xMnxBr4). The PLQYs of (C8H17NH2)2Sn1-xMnxBr4 (x = 0.26) powders reach up to 42%. The as-prepared (C8H17NH2)2Sn1-xMnxBr4 exhibit a single broad photoluminescence (PL) band, differing from the dual peaks of Mn-doped lead halide perovskite quantum dots. Theoretical conclusions and experimental results show the competitive relationship between self-trapped excitons (STEs) emission from the host crystal and dopant Mn d-d transition emission. With Mn dopant concentration increasing, the PL spectra exhibit red shifts and the full width at half-maximum (FWHM) turns larger, which is constructive for warm white LEDs. The fabricated warm white LEDs based on (C8H17NH2)2Sn1-xMnxBr4 show warm white light correlated color temperature (CCT, 3542 K) and high color-rendering index (Ra, 88.12). Our work provides new possibilities for optoelectronic devices based on lead-free perovskite materials.
关键词： self-trapped excitons,Mn-doped,photoluminescence quantum yields,2D Sn-based perovskites,warm white light-emitting diodes
更新于2025-09-23 15:21:01
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The role of self-trapped excitons in polaronic recombination processes in lithium niobate
摘要： Transient absorption and photoluminescence are experimentally investigated in the polaronic reference system lithium niobate, LiNbO3 (LN), with the aim to refine the microscopic model of small polaron dynamics in materials with strong electron-phonon coupling. As a unique feature, our study is performed by using two different spectroscopic methods, in crystals with dopants enhancing photorefraction or damage resistance, and over a broad temperature range from 15?400 K. Although being self-consistent for particular experimental conditions, the hitherto used microscopic polaronic models reveal inconsistencies when applied to this larger data set. We show that comprehensive modeling is unlocked by the inclusion of an additional type of polaronic state with the following characteristics: (i) strongly temperature- and dopant-dependent relaxation times, (ii) an absorption feature in the blue-green spectral range, and (iii) a Kohlrausch-Williams-Watts decay shape with a temperature-dependent stretching factor β(T ) showing a behavior contrary to that of small, strong-coupling polarons. The hypothesis of self-trapped excitons (STEs, i.e., bound electron-hole pairs strongly coupled to Nb5+ and O2? within a niobium-oxygen octahedron) and their pinning on defects as the microscopic origin of these characteristics is supported by a spectroscopic linkage of photoluminescence at low (15 K) and elevated (300 K) temperatures and explains the long-lifetime components in transient absorption as due to pinned STEs.
关键词： self-trapped excitons,lithium niobate,photoluminescence,transient absorption,polaronic recombination
更新于2025-09-23 15:19:57
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Bismuth doped lead-free two-dimensional tin based halide perovskite single crystals
摘要： Heterovalent-metal doping is an efficient tool to tune the optoelectronic properties of the famous halide perovskites. Previous studies have focused on the heterovalent-doping in three-dimensional (3D) halide perovskites. However, there is a lack of such doping in two-dimensional perovskites which possess unique optoelectronic properties and improved chemical stability as compared to 3D analogues. Here, we present successful doping of Bismuth into the lattice of lead-free, two-dimensional perovskite PEA2SnBr4 single crystals. Structural characterizations demonstrate that the doped crystals possess identical crystal structure and layered morphology with the pristine one. Intriguingly, we find the PL peak and spectral shape can be tailored by tuning the concentration of Bi dopants. Femtosecond transient absorption spectroscopy is performed to understand the underlying mechanism related to tunable PL behaviors, and a clear picture of the Bismuth-doping impact is provided.
关键词： Global analysis fit,Femtosecond transient absorption spectra,Self-trapped excitons,Photoluminescence,Heterovalent-metal doping
更新于2025-09-04 15:30:14