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OPTICS LETTERS · 2024 ·Vol. 49 ·期 3 ·478-481 · IF 3.1

Bright luminescence from nontoxic all-inorganic low-dimensional cesium halide

Ranran Fan,Junpeng Qiao,Jiaxin Xu,Sujuan Feng,Guangqiang Liu

Due to the superiority of low cost, easy manufacture, and tunable light emission owing to the diversity of compositions and dimensionalities, the metal halides have appeared as a promising class of semiconductors. Nevertheless, the toxicity problem along with inherent instability of Pb-based metal halides greatly limits their large-scale applications. Based on this situation, it is necessary to develop eco-friendly materials, which could simultaneously maintain the excellent optoelectronic properties of lead materials. In this Letter, the one-dimensional Cu + -alloyed Cs2AgI3 has been successfully synthesized. An intense blue emission located at 469 nm with a large Stokes shift was observed. Density functional theory calculation indicated that the Cu+ ions could effectively modulate the density of state population, which was the key factor drastically boosting the photoluminescence quantum yield (PLQY). This kind of highly efficient metal halide may overcome the bottlenecks of toxicity and poor efficiency issues of blue emission and will have a promising prospect in the optoelectronic fields.

研究领域: 材料科学 · 光学
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CHEMICAL ENGINEERING JOURNAL · 2024 · IF 13.3

Low-dimensional hybrid copper(I) halides single crystals: synthesis, structures, and tunable photoluminescence

Pengyu Zhang,Zhengguang Yan,Chen Li,Yiping Du,Lin Ma,Zhenzhong Wang,Taifeng Lin,Le Zhao,Jiawen Xiao

Low-dimensional organic–inorganic hybrid copper(I) compounds have attracted much attention due to their high luminescence efficiency and non-toxicity. In this study, we synthesized three novel centimeter-scale Cu(I)-based hybrid [1,2-PDA]CuX 3 (X=Cl, Br, I) single crystals using the solvent evaporation method. [1,2-PDA]CuCl 3 and [1,2-PDA]CuBr 3 exhibit zero-dimensional crystal structures composed of separated binary edge-sharing [CuX 4 ] 3- (X=Cl, Br) tetrahedra, while [1,2-PDA]CuI 3 exhibits a one-dimensional crystal structure composed of chains of corner-sharing [CuI 4 ] 3- tetrahedra. The photoluminescence emission of [1,2-PDA]CuX 3 (X=I, Cl, Br) ranges from cyan to purple light at room temperature, showing a tunable pattern with the halogen changes. The photoluminescence quantum yield of the [1,2-PDA]CuI 3 single crystal was measured to be 33.5 %. Density functional theory calculations demonstrate that all three single crystals have direct bandgaps. The emission mechanisms of [1,2-PDA]CuI 3 single crystals were investigated by temperature-dependent photoluminescence spectroscopy, and the broadband emissions were found to be typical of self-trapped exciton emission. It is worth mentioning that the discovery of low toxic, stable, and inexpensive copper(I) compounds paves the way for considering low-cost and environmentally friendly copper halides for practical applications.

CAS / MDL: 78-90-0 7647-01-0
研究领域: 材料科学 · 光学
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Solar RRL · 2022 ·Vol. 6 ·期 7 ·2200168 · IF 9.173

Amino Acid-Based Low-Dimensional Management for Enhanced Perovskite Solar Cells

Yingjie Hu,Lili Gao,Hang Su,Xinyi Du,Ningyi Yuan,Jianning Ding,Jing Zhang,Shengzhong (Frank) Liu

It has been reported that an overlayer of lower dimensional perovskite can effectively improve the properties of 3D perovskite solar cells. Here, 4-aminobutyric acid (C4I) and 6-aminocaproic acid iodides (C6I) are introduced onto the surface of the perovskite layer, forming a low-dimensional (LD) capping layer on the 3D perovskite films for high-performance devices. It is found that C4I forms a 2D perovskite layer, while C6I forms a 1D perovskite layer on the 3D perovskite surface. By using the LD capping layers, the integrated perovskite films show passivated surface traps, reduced defect density, improved carrier lifetimes, and altered band alignment, leading to improved fill factor and open-circuit voltage and, hence, significantly higher device efficiency. The devices with the C4I and C6I capping layers achieve solar cell efficiencies as high as 23.48% and 23.11%, respectively. In addition, bare devices with the C4I and C6I integration maintain 93.73% and 91.58%, respectively, of their initial efficiencies after exposure to the ambient atmosphere for 2000 h, demonstrating much better stability than the pristine 3D holding only 83.30% of its initial efficiency. It appears that this 2D capping is more suitable for enhancing 3D perovskite performance for general photoelectronic applications than the 1D capping.

研究领域: 材料科学 · 能源技术
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Solar RRL · 2022 ·Vol. 6 ·期 11 ·2200672 · IF 9.173

Difluorine-Substituted Molecule-Based Low-Dimensional Structure for Highly Stable Tin Perovskite Solar Cells

Mingyuan Sun,Mingyu Ma,Yang Guo,Songyang Yuan,Hui Xiong,Ziyu Tan,Wenzhe Li,Jiandong Fan,Zhijun Ning

Despite tin perovskite showing excellent optoelectronic properties such as ideal bandgap and high carrier mobility, the intrinsic instability of tin perovskite due to the reaction with water and oxygen that significantly shadows its application. Herein, a molecule substituted with two fluorine atoms for the construction of low-dimensional tin perovskite is explored. Tin perovskite film based on this molecule shows much enhanced hydrophobicity, bringing much enhanced stability in atmosphere. The unencapsulated device can be kept over 200 h in atmospheric environment. In comparison to the instantaneous degradation of device performance for traditional 3D solar cells, no obvious degradation of device efficiency is observed under continuous operation in atmosphere without encapsulation over 10 h. Furthermore, the low-dimensional perovskite film exhibits a unique two-layer structure that can effectively passivate defects of the tin perovskite film. Accordingly, the power conversion efficiency (PCE) of Sn-perovskite solar cells realizes a remarkable enhancement by a factor of 45% and yields a PCE of 8.38%. This work indicates that molecular design of low-dimensional structure is a promising approach to improve the stability of tin perovskite.

研究领域: 材料科学 · 能源技术
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Journal of Materials Chemistry C · 2024 · IF 5.7

RbSb(SO4)(H2PO2)F: A Short-Wave UV Antimony(III) Oxysalt with Mixed-Anions Demonstrating Enhanced Birefringence

Jinwen Tan,Han Luo,Shiyi Wang,Ling Huang,Liling Cao,Xuehua Dong,Guohong Zou

A short-wave UV antimony(III) oxysalt, RbSb(SO4)(H2PO2)F, by incorporating three different anions (SO42-, H2PO2-, F-) with trivalent antimony cations that possess stereochemically active lone-pair electrons (SCALP), has been successfully synthesized. Significantly, the mixed anions and Sb3+ cations combine to form a low-dimensional 1D infinite anionic chain, denoted as [Sb(SO4)(H2PO2)F]∞-, where synergistic interactions among these units contribute to a substantial birefringence of 0.192 at 546 nm and achieve a short cutoff edge down to 276 nm. This research expands the family of UV birefringent optical materials and provides guidance for the further exploration of novel structural-functional materials.

研究领域: 材料科学 · 光学
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PHYSICAL CHEMISTRY CHEMICAL PHYSICS · 2020 ·Vol. 22 ·期 35 ·19697-19703 · IF 3.43

Enhanced optical anisotropy via dimensional control in alkali-metal chalcogenides

Jingmei Min,Ailijiang Abudurusuli,Junjie Li,Shilie Pan,Zhihua Yang

Crystals with both large birefringence and wide transparent range are suitable for broad applications in the areas of optical communications, the laser industry and modulation of the light polarization requirement. In this work, to assist the design of urgently needed crystals with large birefringence in the infrared (IR) region, typical alkali-metal chalcogenides, KPSe6, Na2Ge2Se5, and Li2In2GeSe6 have been studied. They exhibit a hierarchical characteristic in the calculated birefringence by about 0.21, 0.11, and 0.04, respectively. To explore the origin of the birefringence difference, the polarizability anisotropy and the effect of electron distribution anisotropy are analyzed. The alkali-metal chalcogenides KPSe6, Na2Ge2Se5, and Li2In2GeSe6 feature infinite one-dimensional (1D) chains of [PSe6], 2D anionic framework of [Ge2Se5] layers and 3D [In2GeSe9] networks, respectively. It is found that the anionic group with low-dimensional configuration could enhance polarizability anisotropy and render large birefringence for the macroscopic structure. This provides evidence that a low-dimensionality configuration in the structure would be beneficial for the enhancement of optical anisotropy, which can motivate the exploration and design of novel IR birefringent materials.

研究领域: 材料科学 · 光学
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ADVANCED MATERIALS · 2019 ·Vol. 31 ·期 37 ·1901673 · IF 25.809

Fluorinated Low-Dimensional Ruddlesden–Popper Perovskite Solar Cells with over 17% Power Conversion Efficiency and Improved Stability

Jishan Shi,Yerun Gao,Xiang Gao,Yun Zhang,Junjie Zhang,Xin Jing,Ming Shao

Low-dimensional Ruddlesden–Popper perovskites (RPPs) exhibit excellent stability in comparison with 3D perovskites; however, the relatively low power conversion efficiency (PCE) limits their future application. In this work, a new fluorine-substituted phenylethlammonium (PEA) cation is developed as a spacer to fabricate quasi-2D (4FPEA) 2 (MA) 4 Pb 5 I 16 ( n = 5) perovskite solar cells. The champion device exhibits a remarkable PCE of 17.3% with a J sc of 19.00 mA cm −2 , a V oc of 1.16 V, and a fill factor (FF) of 79%, which are among the best results for low-dimensional RPP solar cells ( n ≤ 5). The enhanced device performance can be attributed as follows: first, the strong dipole field induced by the 4-fluoro-phenethylammonium (4FPEA) organic spacer facilitates charge dissociation. Second, fluorinated RPP crystals preferentially grow along the vertical direction, and form a phase distribution with the increasing n number from bottom to the top surface, resulting in efficient charge transport. Third, 4FPEA-based RPP films exhibit higher film crystallinity, enlarged grain size, and reduced trap-state density. Lastly, the unsealed fluorinated RPP devices demonstrate superior humidity and thermal stability. Therefore, the fluorination of the long-chain organic cations provides a feasible approach for simultaneously improving the efficiency and stability of low-dimensional RPP solar cells.

CAS / MDL: 13078-79-0 10034-85-2
研究领域: 材料科学 · 能源科学
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Advanced Energy Materials · 2021 ·Vol. 12 ·期 1 ·2102820 · IF 29.368

Improved Performance and Stability of Perovskite Solar Modules by Regulating Interfacial Ion Diffusion with Nonionic Cross-Linked 1D Lead-Iodide

Haipeng Zeng,Lin Li,Fengxiang Liu,Min Li,Shujing Zhang,Xin Zheng,Long Luo,Shuai You,Yang Zhao,Rui Guo,Zhongmiao Gong,Rong Huang,Zhe Li,Ti Wang,Yi Cui,Yaoguang Rong,Xiong Li

Long-term stability has become the major obstacle for the successful large-scale application of perovskites devices. Owing to the ionic nature of metal-halide perovskites, the interfacial ion diffusion can induce irreversible degradation under operational conditions, which presents a great challenge to realize stable perovskite solar modules. Here, a diphenylphosphine oxide compound, ethane-1,2-diylbis(diphenylphosphine oxide) (DPPO) is introduced to coordinate with lead iodide and form a cross-linked 1D Pb 3 I 6 -DPPO (1D-PbI 2 ) complex. These judiciously designed cross-linked nonionic low-dimensional lead halide/organic adducts can passivate the defects of perovskite while acting as a robust ion diffusion barrier, thus significantly improving the electronic quality and intrinsic stability of perovskite films. As a result, high-performance inverted (p-i-n) solar modules with a champion efficiency approaching 19% (a certified stabilized efficiency of 17.8%) for active device areas above 17 cm 2 without the use of antisolvents, accompanied by outstanding operational stability under heat stress and continuous illumination are achieved.

研究领域: 材料科学 · 能源技术 · 化学工程
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CHEMISTRY OF MATERIALS · 2022 · IF 10.508

Chiral Ligand-Induced Structural Transformation of Low-Dimensional Hybrid Perovskite for Circularly Polarized Photodetection

Maoxin Li,Feier Fang,Xiao Huang,Guangyou Liu,Zheng Lai,Zhihao Chen,Jiahao Hong,Yu Chen,Rong-jia Wei,Guo-Hong Ning,Kai Leng,Yumeng Shi,Bingbing Tian

Chiral organic–inorganic hybrid perovskites (OIHPs) are inversion-asymmetric and have many remarkable properties, including circular dichroism, optical rotation, nonlinear optics, and second-harmonic generation (SHG). Although chiral molecules are responsible for chiroptical properties, they are generally not expected to influence the crystallization of OIHPs. Here, we find that OIHPs synthesized with pristine S- and R-molecules crystallize as 1D perovskites, whereas those synthesized with the racemic molecule crystallized as 2D perovskites. Single crystal X-ray diffraction reveals that the structure change is related to the differing packing of chiral molecules versus racemic ones in OIHPs. Furthermore, we demonstrate that chiral OIHPs containing the S- or R-ligands could be applied in circularly polarized light detectors.

CAS / MDL: 10034-85-2
研究领域: 材料科学 · 光学
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Advanced Powder Materials · 2023 · IF 0

Anisotropic solution growth of 1D/2D N-rich carbon

Zongge Li,Chenwei Wang,Anuj Kumar,Hongrui Jia,Yin Jia,Huifang Li,Lu Bai,Guoxin Zhang,Xiaoming Sun

Despite the fact that low-dimensional carbons (LDCs, 1D/2D) materials are very interesting due to their intriguing electrical properties, we still attempt to enrich them by high N-content in order to enjoy their electro-applications. We here report a template-free synthesis of 1D/2D LDC with high N content (>40 ​at%) and tunable aspect ratios from molecular formamide (FA). The 1D/2D LDC is in polyaminoimidazole as confirmed by pair distribution function analysis, and 1D growth mode can be altered to 2D by simply adding a 2D-guiding molecule of melamine. Electrochemical properties of the LDC can be finely tuned by adjusting the solvothermal temperature and melamine dosage. It is revealed that the optimal 2D LDC delivers superior O 2 -to-H 2 O 2 yield (687.2 ​mmol·g −1 ⋅h −1 ) and Faradic efficiency (87.5%). Considering the heavy N content and high adjustability of aspect ratio, the FA-derived LDCs potentially open new synthesis routes for structural carbon materials for broad electrochemical applications.

研究领域: 材料科学 · 电化学
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ADVANCED FUNCTIONAL MATERIALS · 2024 · IF 18.5

Low-Dose and Stable X-Ray Imaging Enabled by Low-Dimensional Dion-Jacobson Perovskites

Deyu Xin,Min Zhang,Zhenghui Fan,Yujie Yang,Siyin Dong,Lin Lei,Wei Zhao,Qianqian Lin,Xiaojia Zheng

Metal halide perovskites have emerged as highly promising candidates for next-generation X-ray detectors due to their facile and low-cost processability, high attenuation coefficient, and tunable optoelectrical properties. In this work, quasi-2D Dion-Jacobson (DJ) perovskites are introduced in a flat panel X-ray imager (FPXI) for X-ray imaging. This study demonstrates that the diammonium interlayers in DJ perovskites play a key role in enhancing structural stability, suppressing ion migration, and improving charge transport. As a result, DJ perovskite-based X-ray FPXIs achieve a sensitivity of 18000 µC Gy air −1 cm −2 , a low detection limit of 5.7 nGy air s −1 , representing performance comparable to that of state-of-the-art 3D perovskite FPXIs. Thanks to the decrease in the signal crosstalk effect of the FPXIs, a high spatial resolution of 0.54 line-pair-per-pixel is achieved, which is higher than that of 3D perovskite FPXIs. Remarkably, high-quality X-ray imaging is achieved at a total dose of 20 µGy air , which is only 1/5 of the dose typically used in commercial equipment. This work not only provides valuable insights and guidance for the fabrication of 2D DJ perovskite X-ray detectors but also lays the groundwork for the adoption of high-performance, stable DJ perovskite imagers as novel flat-panel X-ray detectors.

研究领域: 材料科学 · 医学影像 · 电子工程
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JOURNAL OF ELECTRONIC MATERIALS · 2024 ·Vol. 53 ·期 8 ·4613-4621 · IF 2.2

Facile Synthesis and Characterization of Low-Dimensional Layered Y2O3 Nanosheets by a Rapid Heating Route

Wang Hongjun,Yang Shuning,Zeng Xiong,Chen Mengyao,Guo Zicong,Mi Pengtao,Zhou Jing,Zhu Yuanyuan

Low-dimensional yttrium oxide (Y 2 O 3 ) nanostructures have garnered significant research interest due to their intriguing properties arising from the dimensional effect and the modulation of the band structure. However, the simple preparation of Y 2 O 3 nanosheets is rarely investigated due to the inherent limitations posed by the counterpart bulk cubic or monoclinic crystal structure. Herein, the low-dimensional layered Y 2 O 3 nanosheets are prepared by a facile route of rapid heating followed by centrifugation, in which its corresponding hydrous-chloride compound is used as the sole reagent. The formation stages of layered Y 2 O 3 nanosheets and corresponding mechanisms are elucidated in detail. The x-ray diffraction results confirm that the intermediate product after rapid heating is yttrium oxychloride (YOCl), which converts to the single-phase Y 2 O 3 with a 2D layered phase after centrifugation. In addition, the obtained Y 2 O 3 nanosheets possess a direct optical bandgap of 5.49 eV, and thus may hold promise for use in electronic applications. This research provides a facile and low-cost method for the preparation of other low-dimensional nanosheets with similar structures. Graphical Abstract

CAS / MDL: 10025-94-2
研究领域: 材料科学 · 纳米技术
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