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1.
Perovskite single crystals and polycrystalline films have complementary merits and deficiencies in X-ray detection and imaging. Herein, we report preparation of dense and smooth perovskite microcrystalline films with both merits of single crystals and polycrystalline films through polycrystal-induced growth and hot-pressing treatment (HPT). Utilizing polycrystalline films as seeds, multi-inch-sized microcrystalline films can be in situ grown on diverse substrates with maximum grain size reaching 100 μm, which endows the microcrystalline films with comparable carrier mobility-lifetime (μτ) product as single crystals. As a result, self-powered X-ray detectors with impressive sensitivity of 6.1×104 μC Gyair−1 cm−2 and low detection limit of 1.5 nGyair s−1 are achieved, leading to high-contrast X-ray imaging at an ultra-low dose rate of 67 nGyair s−1. Combining with the fast response speed (186 μs), this work may contribute to the development of perovskite-based low-dose X-ray imaging.  相似文献   

2.
Two-dimensional (2D) AA′n−1MnX3n+1 type halide perovskites incorporating straight-chain symmetric diammonium cations define a new type of structure, but their optoelectronic properties are largely unexplored. Reported here is the synthesis of a centimeter-sized AA′n−1MnX3n+1 type perovskite, BDAPbI4 (BDA=NH3C4H8NH3), single crystal and its charge-transport properties under X-ray excitation. The crystal shows a staggered configuration of the [PbI6]4− layers, a band gap of 2.37 eV, and a low trap density of 3.1×109 cm−3. The single-crystal X-ray detector exhibits an excellent sensitivity of 242 μC Gyair−1 cm−2 under the 10 V bias (0.31 V μm−1), a detection limit as low as 430 nGyair s−1, ultrastable response current, a stable baseline with the lowest dark current drift of 6.06×10−9 nA cm−1 s−1 V−1, and rapid response time of τrise=7.3 ms and τfall=22.5 ms. These crystals are promising candidates for the next generation of optoelectronic devices.  相似文献   

3.
Inorganic Bi-based perovskites have shown great potential in X-ray detection for their large absorption to X-rays, diverse low-dimensional structures, and eco-friendliness without toxic metals. However, they suffer from poor carrier transport properties compared to Pb-based perovskites. Here, we propose a mixed-halogen strategy to tune the structural dimensions and optoelectronic properties of Cs3Bi2I9−nBrn (0≤n≤9). Ten centimeter-sized single crystals are successfully grown by the Bridgman technique. Upon doping bromine to zero-dimensional Cs3Bi2I9, the crystal transforms into a two-dimensional structure as the bromine content reaches Cs3Bi2I8Br. Correspondingly, the optoelectronic properties are adjusted. Among these crystals, Cs3Bi2I8Br exhibits negligible ion migration, moderate resistivity, and the best carrier transport capability. The sensitivities in 100 keV hard X-ray detection are 1.33×104 and 1.74×104 μC Gyair−1 cm−2 at room temperature and 75 °C, respectively, which are the highest among all reported bismuth perovskites. Moreover, the lowest detection limit of 28.6 nGyair s−1 and ultralow dark current drift of 9.12×10−9 nA cm−1 s−1 V−1 are obtained owing to the high ionic activation energy. Our work demonstrates that Br incorporation is an effective strategy to enhance the X-ray detection performance by tuning the dimensional and optoelectronic properties.  相似文献   

4.
Two‐dimensional (2D) layered hybrid perovskites have shown great potential in optoelectronics, owing to their unique physical attributes. However, 2D hybrid perovskite ferroelectrics remain rare. The first hybrid ferroelectric with unusual 2D multilayered perovskite framework, (C4H9NH3)2(CH3NH3)2Pb3Br10 ( 1 ), has been constructed by tailored alloying of the mixed organic cations into 3D prototype of CH3NH3PbBr3. Ferroelectricity is created through molecular reorientation and synergic ordering of organic moieties, which are unprecedented for the known 2D multilayered hybrid perovskites. Single‐crystal photodetectors of 1 exhibit fascinating performances, including extremely low dark currents (ca. 10−12 A), large on/off current ratios (ca. 2.5×103), and very fast response rate (ca. 150 μs). These merits are superior to integrated detectors of other 2D perovskites, and compete with the most active CH3NH3PbI3.  相似文献   

5.
Metal-free perovskites (MFPs) with flexible and degradable properties have been adopted in flexible X-ray detection. For now, figuring out the key factors between structure and device performance are critical to guide the design of MFPs. Herein, MPAZE-NH4I3 ⋅ H2O was first designed and synthesized with improved structural stability and device performance. Through theoretical calculations, the introducing methyl group benefits modulating tolerance factor, increases dipole moment and strengthens hydrogen bonds. Meanwhile, H2O increases the hydrogen bond formation sites and synergistically realizes the band nature modulation, ionic migration inhibition and structural stiffness optimization. Spectra analysis also proves that the improved electron-phonon coupling and carrier recombination lifetime contribute to enhanced performance. Finally, a flexible and degradable X-ray detector was fabricated with the highest sensitivity of 740.8 μC Gyair−1 cm−2 and low detection limit (0.14 nGyair s−1).  相似文献   

6.
The unique optoelectronic properties and promising photovoltaic applications of organolead halide perovskites have driven the exploration of facile strategies to synthesize organometal halide perovskites and corresponding hybrid materials and devices. Currently, the preparation of CH3NH3PbBr3 perovskite nanowires, especially those with porous features, is still a great challenge. An efficient self‐template‐directed synthesis of high‐quality porous CH3NH3PbBr3 perovskite nanowires in solution at room temperature using the Pb‐containing precursor nanowires as both the sacrificial template and the Pb2+ source in the presence of CH3NH3Br and HBr is now presented. The initial formation of CH3NH3PbBr3 perovskite layers on the surface of the precursor nanowires and the following dissolution of the organic component of the latter led to the formation of mesopores and the preservation of the 1D morphology. Furthermore, the perovskite nanowires are potential materials for visible‐light photodetectors with high sensitivity and stability.  相似文献   

7.
A 3D supramolecular compound [NH3CH2CH2NH3]3H4[H2W12O42] · 2.5H2O (I) was synthesized hydrothermally and characterized by elemental analyses, IR, UV, TG analyses, and X-ray single-crystal diffraction. The X-ray diffraction experiment indicates that compound I exhibits a 3D network through electrostatic interactions and hydrogen bonding interactions between protonated ethylenediamine molecules, [H2W12O40]10− polyanions, and water molecules.  相似文献   

8.
Wang  Shutao  Wang  Enbo  Hou  Yu  Li  Yangguang  Wang  Li  Yuan  Mei  Hu  Changwen 《Transition Metal Chemistry》2003,28(6):616-620
A novel organic/inorganic hybrid molybdenum phosphate, [NH3(CH2CH2)2NH3]3[NH3(CH2CH2)2NH2]Na5-[Mo6O12(OH)3(PO4)(HPO4)3]2·4H2O (1), involving molybdenum presented in V oxidation, has been hydrothermally prepared and characterized by elemental analysis, i.r., u.v.–vis., x.p.s., t.g. and single crystal X-ray diffraction. The structure of the title compound (1) may be considered to consist of two [Mo6O12(OH)3(PO4)(HPO4)3] units bonded together with NaO6 octahedra, forming dimers. Further, these dimers connect with each other through four Na+ cations as bridges, giving rise to novel one-dimensional chain-like skeleton. Piperazines exist among inorganic chains acting as charge balancing cations.  相似文献   

9.
Abstract  The compound [NH4][(CH3)2NH2]2[Ta(C2O4)4]·2H2O has been synthesized and characterized by elemental and TG/DTA analyses, IR spectroscopy and by the single-crystal X-ray diffraction study. The structure comprises the [Ta(C2O4)4]3− anion, NH4 + and [(CH3)2NH2]+ cations and crystallization water molecules. The Ta atom is octacoordinated by oxygen atoms from four bidentate oxalate groups forming a coordination polyhedron close to the triangular dodecahedron. The charge-assisted hydrogen bonds from both cations connect the [Ta(C2O4)4]3− anions into a three-dimensional framework. Graphical Abstract  The synthesis and properties of [NH4][(CH3)2NH2]2[Ta(C2O4)4]·2H2O, the first structurally characterized compound with the tetra(oxalato)tantalate(V) anion, is reported.   相似文献   

10.
《Polyhedron》2001,20(15-16):2033-2036
The complex [(HL)Cu(SCN)Cr(NCS)3(NH3)2]·DMF [H2L=3,3′-trimethylenedinitrilobis(2-butanoneoxime), DMF=N,N′-dimethylformamide] has been synthesized and the structure determined by single-crystal X-ray diffraction. The structure consists of a dinuclear thiocyanato-bridged Cr(III)Cu(II) unit and a DMF molecule as crystal solvate. The chromium ion is six-coordinated with two NH3 molecules in axial positions and four nitrogen atoms, from four NCS, in equatorial positions. One of the NCS bridges the Cr and Cu ions, the S atom of which occupies the apex of the square-pyramidal coordination at Cu with the tetradentate HL ligand in the basal site. Cryomagnetic measurement revealed a weak antiferromagnetic coupling between the heterometal ions with J=−0.63 cm−1 based on the spin Hamiltonian H=−2JS1S2.  相似文献   

11.
Two new chain like B-Anderson type polyoxomolybdates based hybrids {Na[(CH3)3N(CH2)2OH]2}[Al(OH)6Mo6O18]·2(NH2CONH2)·6H2O (1) and {Na[(CH3)3N(CH2)2OH]2}[Cr(OH)6Mo6O18]·2(NH2CONH2)·6H2O (2) were synthesized in choline chloride/urea eutectic mixture and characterized by element analysis, IR, UV–vis, TG, single-crystal X-ray analysis, and power X-ray diffraction. Through the linkage [Na(H2O)2(NH2CONH2)2]+, the [X(OH)6Mo6O18]3− (X = Al, Cr) units are arranged into a chain. Considering hydrogen bonding interactions between the chains, compound 1 and 2 are all well-arranged into 3-D supermolecular assembly. The structure is first obtained in the choline chloride/urea eutectic mixture.  相似文献   

12.
A new organic-inorganic hybrid Strandberg-type polyoxomolybdate derivative [(n-C4H9)4N]2[(NH2CH2PO3)2Mo5O15] · (CH3NHCH3)2 · H2O (I) has been synthesized and structurally characterized by elemental analysis, IR spectrum, UV spectrum, TG analysis, cyclic voltammetry, and single-crystal X-ray diffraction. The hybrid polyoxoanion [(NH2CH2PO3)2Mo5O15]2− consists of a ring-shaped {Mo5O21} cluster with two [NH2CH2PO3] groups incorporating into the opposite sides of the ring. The UV spectrum studied at different times reveals that I remains stable in CH3CN-H2O solvents (volume ratio = 1 : 2) for one day, and the electrochemical measurement indicates that I can exist in a pH range of 4.12–4.72.  相似文献   

13.
Methylammonium lead tribromide (CH3NH3PbBr3) perovskite as a photovoltaic material has attracted a great deal of recent interest. Factors that are important in their application in optoelectronic devices include their fractional contribution of the composition of the materials as well as their microscopic arrangement that is responsible for the formation of well-defined macroscopic structures. CH3NH3PbBr3 assumes different polymorphs (orthorhombic, tetragonal and cubic) depending on the evolution temperature of the bulk material. An understanding of the structure of these compounds will assist in rationalizing how halogen-centered non-covalent interactions play an important role in the rational design of these materials. Density functional theory (DFT) calculations have been performed on polymorphs of CH3NH3PbBr3 to demonstrate that the H atoms on C of the methyl group in CH3NH3+ entrapped within a PbBr64? perovskite cage are not electronically innocent, as is often contended. We show here that these H atoms are involved in attractive interactions with the surrounding bromides of corner-sharing PbBr64? octahedra of the CH3NH3PbBr3 cage to form Br?H(C) hydrogen bonding interactions. This is analogous to the way the H atoms on N of the NH3+ group in CH3NH3+ form Br?H(N) hydrogen bonding interactions to stabilize the structure of CH3NH3PbBr3. Both these hydrogen bonding interactions are shown to persist regardless of the nature of the three polymorphic forms of CH3NH3PbBr3. These, together with the Br?C(N) carbon bonding, the Br?N(C) pnictogen bonding, and the Br?Br lump-hole type intermolecular non-covalent interactions identified for the first time in this study, are shown to be collectively responsible for the eventual emergence of the orthorhombic geometry of the CH3NH3PbBr3 system. These conclusions are arrived at from a systematic analysis of the results obtained from combined DFT, Quantum Theory of Atoms in Molecules (QTAIM), and Reduced Density Gradient Non-Covalent Interaction (RDG-NCI) calculations carried out on the three temperature-dependent polymorphic geometries of CH3NH3PbBr3.  相似文献   

14.
Novel polyoxometalate-based organic-inorganic hybrid [NH3-CH(CH3)COOH][H3O]8[PMo12O40]3.4NH3CH(CH3)COO was synthesized and characterized by 31P, 1H, 13C NMR and IR spectroscopies, elemental analysis and single crystal X-ray determination. Two of the PMo12O40 3? anions in the title hybrid are symmetrically equivalent. They are crystallographically independent from the third PMo12O40 3? polyoxoanion, in the case of various interactions with neighboring components in the crystal network (i.e. +NH3-CH(CH3)-COOH and H3O+ cations, +NH3CH(CH3)COO? zwitterions and polyoxoanions). The compound crystallizes in an orthorhombic C222 space group with a = 16.0392(16) Å, b = 34.480(4) Å, c = 12.8968(13) Å and Z = 2.  相似文献   

15.
A comprehensive study unveiling the impact of heterovalent doping with Bi3+ on the structural, semiconductive, and photoluminescent properties of a single crystal of lead halide perovskites (CH3NH3PbBr3) is presented. As indicated by single-crystal XRD, a perfect cubic structure in Bi3+-doped CH3NH3PbBr3 crystals is maintained in association with a slight lattice contraction. Time-resolved and power-dependent photoluminescence (PL) spectroscopy illustrates a progressively quenched PL of visible emission, alongside the appearance of a new PL signal in the near-infrared (NIR) regime, which is likely to be due to energy transfer to the Bi sites. These optical characteristics indicate the role of Bi3+ dopants as nonradiative recombination centers, which explains the observed transition from bimolecular recombination in pristine CH3NH3PbBr3 to a dominant trap-assisted monomolecular recombination with Bi3+ doping. Electrically, it is found that the mobility in pristine perovskite crystals can be boosted with a low Bi3+ concentration, which may be related to a trap-filling mechanism. Aided by temperature (T)-dependent measurements, two temperature regimes are observed in association with different activation energies (Ea) for electrical conductivity. The reduction of Ea at lower T may be ascribed to suppression of ionic conduction induced by doping. The modified electrical properties and NIR emission with the control of Bi3+ concentration shed light on the opportunity to apply heterovalent doping of perovskite single crystals for NIR optoelectronic applications.  相似文献   

16.
A new heterometallic compound, [CoCl(NH3)5][KCr(C2O4)3]·0.5H2O (1), has been synthesized and characterized by elemental analysis, IR and electronic spectra, thermal analysis, variable temperature magnetic susceptibility measurements, and single crystal X-ray diffraction. Compound 1 consists of two-dimensional [{KCr(C2O4)3}n]2n? layers, [CoCl(NH3)5]2+ ions and water molecules. Within the 2-D layer, three different types of oxalate coordination modes are present. Each K cation is coordinated by eight oxygen atoms from oxalate groups and also weakly interacts with the ninth oxygen atom. The extensive network of hydrogen bond is formed between the [KCr(C2O4)3]2? layer and the [CoCl(NH3)5]2+ ions. These interactions involve all hydrogen atoms of ammonia ligads and water molecule.  相似文献   

17.
An organic–inorganic hybrid compound [(CH3)2NH2]2ZnBr4 has been prepared at room temperature under the slow evaporation method. Its structure was solved at 150 K using the single-crystal X-ray diffraction method. [(CH3)2NH2]2ZnBr4 crystallizes in the monoclinic system – a = 8.5512 (12) Å, b = 11.825 (2) Å, c = 13.499 (2) Å, β = 90.358 (6)°, V = 1365 (4) Å3, and Z = 4, space group P21/n. In the structure of [(CH3)2NH2]2ZnBr4, tetrabromozincate anions are connected to organic cations through N–H⋯ Br hydrogen bonds. Differential scanning calorimetry (DSC) measurements indicate that [(CH3)2NH2]2ZnBr4 undergoes four phase transitions at T1 = 281 K, T2 = 340 K, T3 = 377 K, and T4 = 408 K. Meanwhile, several studies including DSC measurements and variable-temperature structural analyses were performed to reveal the structural phase transition at T = 281 K in [(CH3)2NH2]2ZnBr4. Conductivity and dielectric study as a function of temperature (378 < T [K] < 423) and frequency (10−1 < f [Hz] < 106) were investigated. Analysis of equivalent circuit, alternating current conductivity, and dielectric studies confirmed the phase transition at T4. Conduction takes place by correlated barrier hopping in each phase.  相似文献   

18.
The title compound, {[Cu(NH3)4][Cu(CN)3]2}n, features a CuI–CuII mixed‐valence CuCN framework based on {[Cu2(CN)3]}n anionic layers and [Cu(NH3)4]2+ cations. The asymmetric unit contains two different CuI ions and one CuII ion which lies on a centre of inversion. Each CuI ion is coordinated to three cyanide ligands with a distorted trigonal–planar geometry, while the CuII ion is ligated by four ammine ligands, with a distorted square‐planar coordination geometry. The interlinkage between CuI ions and cyanide bridges produces a honeycomb‐like {[Cu2(CN)3]}n anionic layer containing 18‐membered planar [Cu(CN)]6 metallocycles. A [Cu(NH3)4]2+ cation fills each metallocyclic cavity within pairs of exactly superimposed {[Cu2(CN)3]}n anionic layers, but there are no cations between the layers of adjacent pairs, which are offset. Pairs of N—H...N hydrogen‐bonding interactions link the N—H groups of the ammine ligands to the N atoms of cyanide ligands.  相似文献   

19.
Abstract

The complexes [Cu(TAABNH(CH2)2NH2)](NO3) · 2H2O, (1) [Cu(TAABNH(CH2)4NH2)] (NO3)·4H2O, (2), [Cu(TAABNH(CH2)12NH2](NO3)·4H2O,(3) and [Cu(TAAB(C14H10 N2O2)2]·4H2O, (4) have been synthesized and characterized by IR, mass spectroscopy, electronic spectroscopy, thermogravimetric analysis and elemental analysis. Electrical conductivity and activation energy evaluation were obtained from study of the temperature dependence of the electrical current (in tablet and thin film). Refraction and reflectance indices, absorption coefficient and optical activation energy were established through ellipsometry and UV-Vis spectroscopy. The electrical conductivity values at room temperature were within the range of semiconducting molecular solids (10?6?101Ω?1cm?1).  相似文献   

20.
We report a combined experimental and theoretical study of the synthesis of CH3NH3PbBr3 nanoplatelets through self‐organization. Shape transformation from spherical nanodots to square or rectangular nanoplatelets can be achieved by keeping the preformed colloidal nanocrystals at a high concentration (3.5 mg mL−1) for 3 days, or combining the synthesis of nanodots with self‐organization. The average thickness of the resulting CH3NH3PbBr3 nanoplatelets is similar to the size of the original nanoparticles, and we also noticed several nanoplatelets with circular or square holes, suggesting that the shape transformation experienced a self‐organization process through dipole–dipole interactions along with a realignment of dipolar vectors. Additionally, the CH3NH3PbBr3 nanoplatelets exhibit excellent polarized emissions for stretched CH3NH3PbBr3 nanoplatelets embedded in a polymer composite film, showing advantageous photoluminescence properties for display backlights.  相似文献   

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