Sb3+-Doping in Cesium Zinc Halides Single Crystals Enabling High-Efficiency Near-Infrared Emission

As an effective method to improve the optical properties and stability of perovskite matrix, doped halide perovskites have attracted extensive attention in the field of optoelectronic applications. Herein, a series of all inorganic lead-free Te4+-doped Cs2ZrCl6 vacancy-ordered perovskites were successfully synthesized with different Te-doping concentrations by a solvothermal method, and deliberate Te4+-doping results in green-yellow triplet self-trapped exciton (STE) emission with a high photoluminescence quantum yield (PLQY) of 49.0%. The efficient energy transfer was observed from singlet to triplet emission. Further, the effects of A-site Rb alloying on the optical properties and stability were investigated. We found that A-site Rb alloying and C-site cohalogenation did not change the luminescence properties of Te4+, but the addition of a small amount of Rb+ can improve the PL intensity and moisture stability. Our results provide physical insights into the nS2 Te4+-ion-doping-induced emissive mechanism and shed light on improving the environmental stability for further applications.

Efficient Energy Transfer in Te4+-Doped Cs2ZrCl6 Vacancy-Ordered Perovskites and Ultrahigh Moisture Stability via A-Site Rb-Alloying Strategy.

Lead-free lower-dimensional organic-inorganic metal halide materials have recently triggered intense research because of their excellent photophysical properties and chemical stability. Herein, we report a novel zero-dimensional (0D) organic-inorganic hybrid single crystal (TMA)2SbCl5·DMF (TMA = N(CH3)3, DMF= HCON(CH3)2), which exhibits typical self-trapped exciton (STE) emission with an efficient yellow emission at 630 nm and high photoluminescence quantum yield (PLQY) of 67.2%. The dual STE emission is attributed to the singlet and triplet STEs in inorganic [SbCl5]2-, respectively. Further, an ab initio molecular dynamics simulation was performed to estimate the stability of crystal structure at room temperature. The calculated excited-state structure indicates that the deformation parameter (Δd) of the excited-state structure is larger than that of the ground state, illustrating the origin of a large Stokes shift. These results indicate that these new 0D lead-free organic-inorganic hybrid metal halides are promising luminescent materials for optoelectronic applications.

Self-Trapped Exciton Emission in a Zero-Dimensional (TMA)2SbCl5·DMF Single Crystal and Molecular Dynamics Simulation of Structural Stability.

0D hybrid metal halides (0D HMHs) are considered to be promising luminescent emitters. 0D HMHs commonly exhibit self‐trapped exciton (STE) emissions originating from the inorganic metal halide anion units. Exploring and utilizing the emission features of the organic cation units in 0D HMHs is highly desired to enrich their optical properties as multifunctional luminescent materials. Here, tunable emissions from organic and inorganic units are successfully achieved in triphenylsulfonium (Ph3S+)‐based 0D HMHs. Notably, integrated afterglow and STE emissions with adjustable intensities are obtained in (Ph3S)2Sn1−xTexCl6 (x = 0–1) via the delicate combination of [SnCl6]2− and [TeCl6]2−. Moreover, such a strategy can be readily extended to develop other HMH materials with intriguing optical properties. As a demonstration, 0D (Ph3S)2Zn1−xMnxCl4 (x = 0–1) are constructed to achieve integrated afterglow and Mn2+ d–d emissions with high efficiency. Consequently, these novel 0D HMHs with colorful afterglow and STE emissions are applied in multiple anti‐counterfeiting applications.

Integrated Afterglow and Self‐Trapped Exciton Emissions in Hybrid Metal Halides for Anti‐Counterfeiting Applications

Luminescent metal halides have attracted considerable attention in next-generation solid-state lighting because of their superior optical properties and easy solution processibility. Herein, we report a new class of highly efficient and dual-band tunable white-light emitters based on Bi3+/Te4+ co-doped perovskite derivative Cs2SnCl6 microcrystals. Owing to the strong electron-phonon coupling and efficient energy transfer from Bi3+ to Te4+, the microcrystals exhibited broad dual-band white-light emission originating from the inter-configurational 3P0,1 → 1S0 transitions of Bi3+ and Te4+, with good stability and a high photoluminescence (PL) quantum yield up to 68.3%. Specifically, a remarkable transition in Bi3+-PL lifetime from milliseconds at 10 K to microseconds at 300 K was observed, as a solid evidence for the isolated Bi3+ emission. These findings provide not only new insights into the excited-state dynamics of Bi3+ and Te4+ in Cs2SnCl6, but also a general approach to achieve single-composition white-light emitters based on lead-free metal halides through ns2-metal ion co-doping.

Dual-Band-Tunable White-Light Emission from Bi3+/Te4+ Emitters in Perovskite-Derivative Cs2SnCl6 Microcrystals.

Perovskite variants have attracted wide interest because of the lead-free nature and strong self-trapped exciton (STE) emission. Divalent Sn(II) in CsSnX3 perovskites is easily oxidized to tetravalent Sn(IV), and the resulted Cs2SnCl6 vacancy-ordered perovskite variant exhibits poor photoluminescence property although it has a direct band gap. Controllable doping is an effective strategy to regulate the optical properties of Cs2SnX6. Herein, combining the first principles calculation and spectral analysis, we attempted to understand the luminescence mechanism of Te4+-doped Cs2SnCl6 lead-free perovskite variants. The chemical potential and defect formation energy are calculated to confirm theoretically the feasible substitutability of tetravalent Te4+ ions in Cs2SnCl6 lattices for the Sn-site. Through analysis of the absorption, emission/excitation, and time-resolved photoluminescence (PL) spectroscopy, the intense green-yellow emission in Te4+:Cs2SnCl6 was considered to originate from the triplet Te(IV) ion 3P1→1S0 STE recombination. Temperature-dependent PL spectra demonstrated the strong electron-phonon coupling that inducing an evident lattice distortion to produce STEs. We further calculated the electronic band structure and molecular orbital levels to reveal the underlying photophysical process. These results will shed light on the doping modulated luminescence properties in stable lead-free Cs2MX6 vacancy-ordered perovskite variants and be helpful to understand the optical properties and physical processes of doped perovskite variants.

Boosting triplet self-trapped exciton emission in Te(IV)-doped Cs 2 SnCl 6 perovskite variants

Lead halide perovskites have demonstrated promising emission tunability achieved by composition engineering, which makes them viable in several potential applications. Determining how to effectively control the crystalline structural transformation and composition in lead‐free halide perovskites is of great importance. Herein, a controllable synthetic method is reported to obtain the 0D metal halide perovskite derivatives (Cs1−xRbx)2InCl5∙H2O and (Cs1−xRbx)3InCl6, through synergistic regulation of the Cs/Rb feed ratios and the reaction solvent. When hydrochloric acid (HCl) is used as the reaction solvent, (Cs1−xRbx)2InCl5∙H2O is obtained at a high Cs/Rb feed ratio greater than 2:1, while (Cs1−xRbx)3InCl6 is obtained at a low Cs/Rb feed ratio of less than 2:5. However, when anhydrous methanol (MeOH) is used as the reaction solvent, only the (Cs1−xRbx)3InCl6 structure is obtained at all Cs/Rb feed ratios. In addition, a reversible crystalline structural transformation is demonstrated between (Cs0.67Rb0.33)2InCl5∙H2O and (Cs0.67Rb0.33)3InCl6 by immersing the as‐prepared products into MeOH and HCl sequentially, which generates a novel green/yellow reversible emission switch. The Sb3+ ion self‐trapped exciton emission and stability of the synthesized (Cs1−xRbx)2InCl5∙H2O and (Cs1−xRbx)3InCl6 are systematically investigated. The results are helpful for promoting the diverse photonics and optoelectronics applications of these environmentally stable perovskite derivatives.

Controlled Structural Transformation in Sb-Doped Indium Halides A3InCl6 and A2InCl5∙H2O Yields Reversible Green-to-Yellow Emission Switch

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Boosting triplet self-trapped exciton emission in Te(IV)-doped Cs 2 SnCl 6 perovskite variants

Controlled Structural Transformation in Sb-Doped Indium Halides A3InCl6 and A2InCl5∙H2O Yields Reversible Green-to-Yellow Emission Switch