Halogen-Dependent Thermochromic Properties in Three Methyl-Viologen/Haloargentate Charge Transfer (CT) Salts

Zhu, Yachen; Yu, Tanlai; Hao, Pengfei; Shen, Junju; Fu, Yongqi

doi:10.1007/s10876-016-0999-6

Cited by 21 publications

(9 citation statements)

References 68 publications

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“…The structural unit of 3 contains five crystallographically independent Ag (4e sites), eight Cl (4e sites) atoms, and three [HDABCO] + cations. All the silver atoms connect with four chlorine atoms in [AgCl 4 ] tetrahedral coordination configurations with Ag–Cl bond distances of 2.5185(16)–2.7420(18) Å, which are close to those of [MV]Ag 2 Cl 4 . Each [Ag(1)Cl 4 ], [Ag(4)Cl 4 ], and [Ag(5)Cl 4 ] tetrahedra first interconnect through sharing one edge to form a trimer [Ag 3 Cl 8 ] unit, and [Ag(2)Cl 4 ] and [Ag(3)Cl 4 ] tetrahedrons are condensed into a [Ag 2 Cl 6 ] unit via edge-sharing.…”

Section: Resultsmentioning

confidence: 98%

Broadband White-Light Emission in One-Dimensional Organic–Inorganic Hybrid Silver Halide

et al. 2020

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In the past few decades, organic–inorganic hybrid metal halides acting as single-component white light emission diodes (LEDs) have attracted extensive attentions, but most of the studies concentrate on the low-dimensional lead perovskites. Here, by using the nontoxic silver as optically active metal center, a series of hybrid silver halides based on one-dimensional structures were constructed and realized broadband white light emission. Compounds [H2DABCO][Ag2X4(DABCO)] (X = Br (1), I (2)) feature one-dimensional [Ag2X4(DABCO)]2– structures charged balanced by [H2DABCO]2+ cations. Compound 1 exhibits an efficient broadband white-light emission with photoluminescence quantum efficiency (PLQE) of about 2.1% and excellent photochemical stability, while compound 2 gives a broadband yellow-white emission centered at 556 nm. [HDABCO]3Ag5Cl8 (3) gives a strong broadband yellow emission (585 nm) with high PLQE of 6.7%, which can be easily fabricated as a white light emitting device. Based on the temperature-dependent, particle-size-dependent, and time-resolved PL measurements as well as other detailed studies, the broadband white-light emissions are ascribed to the synergetic effects of the organic and inorganic components. Our work provides a unique structural assembly method to explore lead-free single-component white-light illuminants from molecular level.

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Section: Resultsmentioning

confidence: 98%

Broadband White-Light Emission in One-Dimensional Organic–Inorganic Hybrid Silver Halide

et al. 2020

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“…The results demonstrate the formation of the desired compounds, showing experimental data in concordance with the theoretical ones. Elemental composition calculated for C 18 H 28 Thermogravimetric Analyses (TGA). Thermogravimetric analyses of the obtained polycrystalline powders were performed in TGA-DTA thermal analysis SDT2960 equipment.…”

Section: ■ Experimental Sectionmentioning

confidence: 99%

“…In this context, a large variety of organic cations were combined with bismuth halides to obtain different structures and physical properties. However, most of these studies focused on viologen cations (N-alkylated derivatives of 4,4′-bipyridine), which allow us to obtain materials with interesting optical properties, such as photochromism, thermochromism, luminescence, and solvochromism. − …”

Section: Introductionmentioning

confidence: 99%

Diimidazolium Halobismuthates [Dim]₂[Bi₂X₁₀] (X = Cl^–, Br^–, or I^–): A New Class of Thermochromic and Photoluminescent Materials

et al. 2018

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We present a novel family of polyhalide salts of Bi(III) with the general formula [Dim][BiX], where Dim is the diimidazolium cation (CHN) and X is Cl, Br, or I. Single-phase materials are easily obtained by means of a mild solution chemistry method performed at room temperature. This [Dim][BiX] family exhibits a crystal structure based on halobismuthate [BiX] dimers, built by distorted {BiX} octahedra interconnected by edge sharing, and sandwiched between two diimidazolium cations. The optical band gaps displayed by these materials (1.9-3.2 eV) allow their classification as semiconductors. Additionally, the three halides display photoluminescence with emission in the visible range. The behavior of [Dim][BiI] is particularly interesting, as it shows an optical band gap of 1.9 eV, a broad band photoluminescence emission, and a relatively long emission lifetime of 190 ns. Moreover, the iodide and bromide compounds also exhibit a reversible solid state thermochromism, being the first example of a bromobismuthate with this property. The diimidazolium cations play an important structural role by stabilizing the crystal structure and balancing the charges of the [BiX] dimers. Furthermore, density functional theory calculations suggest that they play a key role in the thermochromic behavior. Therefore, compounds [Dim][BiX] (X = Cl, Br, or I) represent a very versatile family in which the optical band gap can be tuned by changing the halide or temperature. This makes them promising new materials for different optoelectronic applications, in particular for obtaining new solar absorbers.

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“…Given these considerations mentioned above and as a continuing work of our studies on the metal halide derived from tpt derivatives, , we attempted to explore the copper(I)/lead(II)/halide/tpt system, taking into account the following considerations. (a) Paralleling the well-explored homometallic halide mentioned above, the heterometallic halides have also received focus because the integration of distinct metal ions in one framework may give novel molecular materials. − (b) The utilization of dipyridine motifs to construct novel metal halides with optoelectronic properties has been broadly explored. − In comparison to the metal/halide/dipyridine materials, the assembly of tritopic pyridyl motifs with metal halides is still undeveloped and exciting results may be expected. (c) Considering the distinct coordination modes between Cu(I) and Pb(II) ions and the great achievements in the corresponding homometallic halide system, together with the intrinsic advantage of the tritopic pyridyl motif tpt, it is feasible to synthesize tpt-based heterometallic halides with captivating structures and potential structure-related properties.…”

Section: Introductionmentioning

confidence: 99%

In Situ Ligand Modification Strategy for the Construction of One-, Two-, and Three-Dimensional Heterometallic Iodides

et al. 2017

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Three heterometallic iodides featuring the novel in situ modified ligands N,N',N″-trimethyl-2,4,6-tris(4-pyridyl)-1,3,5-triazine (Metpt), N,N'-dimethyl-2,4,6-tris(4-pyridyl)-1,3,5-triazine (Metpt), and N-monomethyl-2,4,6-tris(4-pyridyl)-1,3,5-triazine (Metpt), [PbCuI(Metpt)] (1), [PbCuI(Metpt)] (2), and [PbCuI(Metpt)] (3), were synthesized. Compound 1 exhibits a chain structure, in which the PbI units are connected by the CuI units. The negative charge of the resulting chain is balanced by the cationic Metpt groups. 2 features a layer structure, in which the Pb-I chains are connected by the dimeric Cu units. The anionic layer is decorated by the Metpt motifs via coordinating to the intralayer Cu(I) ions. 3 displays a 3D framework structure, in which the inorganic layer with an 18-membered ring is composed of the strictly alternating arrangements of trimeric Pb units and hexameric Cu units. The adjacent inorganic layer is further connected by a Metpt linker to form the final 3D hybrid framework. It is notable that the in situ N-methylation reaction for tpt has taken place and the resultant motif (Metpt for 1, Metpt for 2, and Metpt for 3) is captured within the corresponding structure. More importantly, the structural diversities from low-dimensional chain and layer to high-dimensional framework is accomplished via the (partial) N-methylation of tripyridine motifs in the heterometallic iodide systems. Our studies offer a new coordination mode of tripyridine motif (N-coordination together with N-methylation) and provide a general strategy to integrate the polypyridine motifs and heterometallic halide systems to generate intriguing hybrid structure and investigate the potential structure-related properties. The UV-vis spectra show that the band gaps for 1-3 are 1.48, 1.35, and 1.34 eV, respectively. Their thermal stabilities have also been studied.

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Halogen-Dependent Thermochromic Properties in Three Methyl-Viologen/Haloargentate Charge Transfer (CT) Salts

Cited by 21 publications

References 68 publications

Broadband White-Light Emission in One-Dimensional Organic–Inorganic Hybrid Silver Halide

Broadband White-Light Emission in One-Dimensional Organic–Inorganic Hybrid Silver Halide

Diimidazolium Halobismuthates [Dim]₂[Bi₂X₁₀] (X = Cl^–, Br^–, or I^–): A New Class of Thermochromic and Photoluminescent Materials

In Situ Ligand Modification Strategy for the Construction of One-, Two-, and Three-Dimensional Heterometallic Iodides

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Halogen-Dependent Thermochromic Properties in Three Methyl-Viologen/Haloargentate Charge Transfer (CT) Salts

Cited by 21 publications

References 68 publications

Broadband White-Light Emission in One-Dimensional Organic–Inorganic Hybrid Silver Halide

Broadband White-Light Emission in One-Dimensional Organic–Inorganic Hybrid Silver Halide

Diimidazolium Halobismuthates [Dim]2[Bi2X10] (X = Cl–, Br–, or I–): A New Class of Thermochromic and Photoluminescent Materials

In Situ Ligand Modification Strategy for the Construction of One-, Two-, and Three-Dimensional Heterometallic Iodides

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Diimidazolium Halobismuthates [Dim]₂[Bi₂X₁₀] (X = Cl^–, Br^–, or I^–): A New Class of Thermochromic and Photoluminescent Materials