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1.
Adv Mater ; 36(24): e2310831, 2024 Jun.
Article in English | MEDLINE | ID: mdl-38553988

ABSTRACT

0D Bi-based 329-type halide perovskite is demonstrated as a promising semiconductor for X-ray detection due to its strong X-ray absorption, superior stability, availability of large single crystals (SCs) and solution processibility at low temperature. However, its low mobility-lifetime product (µτ) limits its further improvement in detection sensitivity. Based on the first-principles calculations, this work designs a new 2D Bi-based 329-type halide perovskite using a mixed-halide-induced structural dimension regulation strategy. By using a continuous supply of a precursor solution, this work successfully grows inch-sized high-quality SCs. These SCs exhibit large µτ product, high resistivity, and low ion migration. The detectors fabricated using the SCs show X-ray detection sensitivity as high as 24,509 µC Gyair -1 cm-2, short response time of 315 µs, low detection limit of 4.3 nGy s-1, and superior stability. These properties are the best among all lead-free perovskite detectors and are comparable to those of the best lead-based perovskite detectors. The linear array detector assembled on the SCs for the first time also shows a high spatial resolution of 10.6 lp mm-1 during X-ray imaging. The high performance combined with superior stability of these new 329-type lead-free halide perovskite SCs is expected to promote a new generation of X-ray detection technologies.

2.
Adv Mater ; 36(3): e2305513, 2024 Jan.
Article in English | MEDLINE | ID: mdl-37878999

ABSTRACT

Metal halide perovskite single crystals (MHP-SCs) are known for their facile fabrication into large sizes using inexpensive solution methods. Owing to their combination of large mobility-lifetime products and strong X-ray absorption, they are considered promising materials for efficient X-ray detection. However, they suffer from large dark currents and severe ion migration, which limit their sensitivity and stability in critical X-ray detection applications. Herein, a heterointerface design is proposed to reduce both the dark current and ion migration by forming a heterojunction. In addition, the carrier transport performance is significantly improved using heterointerface engineering by designing a gradient band structure in the SCs. The SC heterojunction detectors exhibit a high sensitivity of 3.98 × 105 µC Gyair -1 cm-2 with a low detection limit of 12.2 nGyair s-1 and a high spatial resolution of 10.2 lp mm-1 during imaging. These values are among the highest reported for state-of-the-art MHP X-ray detectors. Moreover, the detectors show excellent stability under continuous X-ray irradiation and maintainclear X-ray imaging after 240 d. This study provides novel insights into the design and fabrication of X-ray detectors with high detection efficiency and stability, which are beneficial for developing inexpensive, high-resolution X-ray imaging equipment.

3.
ACS Appl Mater Interfaces ; 15(33): 39550-39558, 2023 Aug 23.
Article in English | MEDLINE | ID: mdl-37614000

ABSTRACT

Near-infrared phosphor-converted light-emitting diodes (NIR pc-LEDs) offer numerous advantages, including compact size, tunable emission spectra, energy efficiency, and high integration potential. These features make them highly promising for various applications, such as night vision monitoring, food safety inspection, biomedical imaging, and theragnostics. All-inorganic halide double-perovskite materials, known for their large absorption cross section, excellent defect tolerance, and long carrier diffusion radius, serve as unique matrices for constructing near-infrared fluorescent materials. In this study, we successfully prepared the all-inorganic metal halide double-perovskite Cs2NaYCl6:Cr3+ using a grinding-sintering method. A small fraction of the [YCl6] octahedra within the host material's lattice was substituted with Cr3+ ions, resulting in the creation of the Cs2NaYCl6:Cr3+ phosphor. When excited with λ = 310 nm UV light, the phosphor exhibited a broad emission range spanning from 800 to 1400 nm, covering the NIR-I and NIR-II regions. It had a broad bandwidth emission of 185 nm and achieved a fluorescence quantum yield of 20.2%. The unique broadband emission of the phosphor originates from the weak crystal field environment provided by the Cs2NaYCl6 host matrix, which enhances the luminescence properties of the Cr3+ ions. To create NIR pc-LEDs, the phosphor was encapsulated onto a commercially available UV LED chip operating at 310 nm. The potential application of these NIR pc-LEDs in night vision imaging was successfully validated.

4.
Sci Adv ; 9(35): eadh2255, 2023 Sep.
Article in English | MEDLINE | ID: mdl-37647409

ABSTRACT

Preliminary theoretical analyses indicate that lattice relaxation may be used to release lattice strain in the FAPbI3 perovskite to warrant both high x-ray detection performance and improved stability. Herein, we demonstrate stable black α-phase FAPbI3 single crystals (SCs) realized by lattice engineering via annealing in the ambient atmosphere. The engineered α-FAPbI3 SC detector shows almost all the best figures of merit including a high sensitivity of 4.15 × 105 µC Gyair-1 cm-2, a low detection limit of 1.1 nGyair s-1, a high resolution of 15.9 lp mm-1, and a short response time of 214 µs. We further demonstrate high-definition x-ray imaging at a dose rate below 10 nGyair s-1 on the FAPbI3 SC, indicating a minimal dose-area product of 0.048 mGyair cm2 to the patient for one-time posteroanterior chest diagnosis, which is more than 3000 times lower than the international reference level of 150 mGyair cm2. In addition, the robust long-term stability enables the FAPbI3 SC x-ray detector to work steadily for more than 40 years.

5.
J Phys Chem Lett ; 13(22): 4981-4987, 2022 Jun 09.
Article in English | MEDLINE | ID: mdl-35647795

ABSTRACT

Halide perovskite materials have been used in the field of lithium-ion batteries because of their excellent ion migration characteristics and defect tolerance. However, the current lead-based perovskites used for lithium-ion batteries are highly toxic, which may hinder the pace of further commercialization. Therefore, it is still necessary to develop a new type of stable and pollution-free perovskite anode material. Herein, we for the first time use a high-concentration lithium-ion doped rare-earth-based double perovskite Cs2NaErCl6:Li+ as the negative electrode material for a lithium-ion battery. Thanks to its excellent structure stability, the assembled battery also has high cycle stability, with a specific capacity of 120 mAh g-1 at 300 mA g-1 after 500 cycles with a Coulomb efficiency of nearly 100%. The introduction of a rare earth element in a lead-free double perovskite paves a new way for the development of novel promising anode materials in the field of lithium storage applications.

6.
J Phys Chem Lett ; 12(17): 4125-4129, 2021 May 06.
Article in English | MEDLINE | ID: mdl-33886336

ABSTRACT

Perovskite materials, as a multifunctional material, have been widely applied in the field of electrochemistry due to its ion migration properties. Although the lead based halide perovskite has been applied in the anode of the lithium battery, it is necessary to develop new lead-free perovskite anode materials because of its the instability and environmental unfriendliness. Herein, we develop a facile grinding method to prepare ultrahigh Li+ concentration doping Cs2NaBiCl6 powders, which are used as the anode material of the lithium battery. The assembled battery possesses a stable specific capacity of about 300 mA h g-1 with over 99% Coulombic efficiency. Owing to their particular crystal structure with high adjustability, the double perovskite materials have promising potentials in lithium storage applications.

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