Nature Communications
·
2021
·Vol. 12
·期 1
·1-7
·
IF 14.919
Zhang Mingming,Zhao Lili,Xie Jiahao,Zhang Qian,Wang Xiaoyu,Yaqoob Najma,Yin Zhengmao,Kaghazchi Payam,Zhang San,Li Hua,Zhang Chunfeng,Wang Lei,Zhang Lijun,Xu Weigao,Xing Jun
Low-dimensional hybrid perovskites have demonstrated excellent performance as white-light emitters. The broadband white emission originates from self-trapped excitons (STEs). Since the mechanism of STEs formation in perovskites is still not clear, preparing new low-dimensional white perovskites relies mostly on screening lots of intercalated organic molecules rather than rational design. Here, we report an atom-substituting strategy to trigger STEs formation in layered perovskites. Halogen-substituted phenyl molecules are applied to synthesize perovskite crystals. The halogen-substituents will withdraw electrons from the branched chain (-R-NH 3 + ) of the phenyl molecule. This will result in positive charge accumulation on -R-NH 3 + , and thus stronger Coulomb force of bond (-R-NH 3 + )-(PbBr 4 2− ), which facilitates excitons self-trapping. Our designed white perovskites exhibit photoluminescence quantum yield of 32%, color-rendering index of near 90 and chromaticity coordinates close to standard white-light. Our joint experiment-theory study provides insights into the STEs formation in perovskites and will benefit tailoring white perovskites with boosting performance.
研究领域:
材料科学
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光学工程
·
化学
✓ 已验证
DOI
高影响因子
Materials Today Chemistry
·
2025
·
IF 6.7
Pengyu Zhang,Yiping Du,Chen Li,Lin Ma,Jiawen Xiao,Zhengguang Yan
Low-dimensional hybrid Cu(I)-based halide materials are a new class of materials with low toxicity and excellent photoluminescent properties. In this work, five novel single crystals of [1,4-BDA]Cu 2 X 4 (X = Cl, Br, I) (1,4-BDA: 1,4-butanediamine) and [1,3-PDA] 2 Cu 3 X 7 (X = Cl, Br) (1,3-propanediamine) were obtained using a solvent evaporation method. The [1,4-BDA]Cu 2 X 4 (X = Cl, Br, I) crystals all have 1D structures, while the [1,3-PDA] 2 Cu 3 X 7 (X = Cl, Br) crystals have 0D structures. All five single crystals exhibit broadband blue emissions under 254 nm UV excitation at room temperature. Interestingly, both crystals show a gradual blueshift of the emission peaks with increasing halogen atomic mass, realizing tunable emission from the dark blue to sky blue range. The energy transfer process of the [1,4-BDA]Cu 2 Br 4 single crystal was studied using temperature-dependent photoluminescence spectroscopy. Combined with density-functional theory calculations, the reason for the shift of the PL emission peaks is explained. Notably, by altering the chemical composition, different photoluminescent halide materials can be obtained. Providing insight into the discovery of new low-toxicity, low-cost Cu(I)-based halide materials.
研究领域:
材料科学
·
光学
✓ 已验证
产品关联
DOI
高影响因子
INORGANIC CHEMISTRY
·
2021
·
IF 5.165
Zhi-Kun Liu,Zi-Shuo Yao,Jun Tao
Halogen-substituted Fe(III) compounds, [Fe(HphsalpmX)2]PTFB (HphsalpmX = 5-X-(R,S)-((phenyl(2-pyridyl)methylimino)methyl)phenol, PTFB = phenyltrifluoroborate; X = F for 1, Cl for 2, Br for 3) and [Fe(HphsalpmX)2]PTFB·MeOH (X = I for 4·MeOH), were synthesized. Compounds 1, 4·MeOH, and its desolvated form 4 exhibited an invariant high-spin state in the whole temperature range, while 2 and 3 underwent gradual, nonhysteretic, and incomplete spin crossover (SCO) with transition temperatures (TC) of 153 and 220 K, respectively. Interestingly, the SCO-active compounds 2 and 3 showed light-induced excited spin-state trapping (LIESST) effects at 10 K, and light-induced reversible ON/OFF switching behaviors were realized by alternately using 880 and 1064 nm light, while the thermally inert compound 4·MeOH unexpectedly showed a reverse-LIESST effect. These results may help to design and synthesize new photoresponsive SCO Fe(III) compounds for the development of switchable materials.
研究领域:
无机化学
·
材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CRYSTAL GROWTH & DESIGN
·
2025
·
IF 3.4
Zhonghua Li,Songgu Wu,Junbo Gong
The influence of halogen-atom substitution for a dimethyl isophthalate compound on the polymorphic behavior and isostructurality property was explored in this paper. Sublimation was demonstrated to exhibit remarkable advantages. Specifically, two polymorphs (Form I and Form II) of dimethyl 5-bromoisophthalate and two polymorphs (Form A and Form B) of dimethyl 5-iodoisophthalate were discovered for the first time. Moreover, the corresponding single crystals suitable for crystal structure determination were also successfully harvested within a few hours. More interestingly, the crystal packing similarities between the stable Form II and metastable Form A were established with the evaluation of quantitative analysis tools. The success in achieving the regulation of luminescence emission with the changes of crystal packing patterns, molecular conformations, and interactions via halogen substitution will provide some inspiration for the development of novel flexible optical solid-state systems in the future.
研究领域:
材料科学
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晶体学
✓ 已验证
DOI
高影响因子
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
·
2020
·Vol. 22
·期 30
·17299-17305
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IF 3.43
Chenyang Zhou,Ya Chu,Linlin Ma,Yingqian Zhong,Chao Wang,Yalan Liu,Haoyue Zhang,Beibei Wang,Xia Feng,Xi Yu,Xiaotao Zhang,Yan Sun,Xiaozeng Li,Guangjiu Zhao
In this work, we introduced halogen-substituted chiral molecules as A-site cations to synthesize a series of novel organic–inorganic hybrid two-dimensional (2D) chiral perovskite materials (R-X-p-mBZA)2PbBr4 (X = H, F, Cl, Br; p: para-position; mBZA = α-methylbenzylamine) for the first time. This halogen-substituted cation strategy collectively solved problems of narrow emission, weak chirality and low photoluminescence quantum yield (PLQY) for the emerged chiral perovskites. Photoluminescence (PL) spectra are significantly broadened due to the additional emission from self-trapped excitons (STEs) besides free excitons (FEs) states modulated by introducing significant disorder to the Pb–Br–Pb angle. The chirality of A-site chiral molecules is transferred and amplified to entire perovskite materials by fixing the chiral molecules at A-site via the interaction of halogen atoms. Furthermore, their PLQYs are improved with the reduction of energy gap and inhibition of the non-radiative transition from STEs to ground state. The halogen-substituted A-site cation strategy can be performed to develop organic–inorganic hybrid chiral perovskites with various optoelectronic applications.
研究领域:
材料科学
·
光学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF COORDINATION CHEMISTRY
·
2017
·
IF 1.795
Xiang-Lan Wang,Yuan-Xia Li,Shuai-Liang Yang,Chen-Xi Zhang,Qing-Lun Wang
Complexes based on different halogen-substituted nitronyl nitroxide radicals and Cu(II), Cu3(hfac)6(NIT-Ph-F)2 (1) and Cu3(hfac)6(NIT-Ph-Cl)2 (2) (hfac = hexafluoroacetylacetonate; NIT-Ph-F = 2-(4′-fluorophenyl)-4,4,5,5-tetramethyl-imidazoline-1-oxyl-3-oxide; NIT-Ph-Cl = 2-(4′-chlorphenyl)-4,4,5,5-tetramethylimidazoline-1-oxyl-3-oxide), were synthesized and characterized structurally and magnetically. X-ray crystal structure analyses show that 1 and 2 have similar centrosymmetric five-spin structures consisting of three Cu(II) ions bridged by two nitroxide ligands. The Cu(II) is coordinated by six oxygens to form an octahedron, while the five coordination of the terminal Cu(II) ion is square pyramidal. Magnetic measurements reveal strong antiferromagnetic interactions between Cu(II) ions and radicals in 1 (J = −38.9 cm−1) and weak antiferromagnetic interactions between Cu(II) ions and radicals in 2 (J = −1.23 cm−1), which may be explained by the bond length of the Cu–Orad (2.468(2) Å) in 1, which is shorter than that (2.514(2) Å) in 2, and the dihedral angle (73.17(1)°) of the plane O7–O8–Cu(2)–O7A–O8A with the moiety O5–N1–C11–N2–O6 in 1 is smaller than (77.82(1)°) in 2.
研究领域:
无机化学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
Journal of Materials Chemistry C
·
2022
·Vol. 10
·期 31
·11371-11378
·
IF 8.067
Meng-Meng Lun,Fo-Ling Zhou,Da-Wei Fu,Qiong Ye
Multi-functional switching materials, possessing a high transition temperature, can work in a relatively wide temperature range, particularly for practical applications under extreme thermal conditions such as automotive, aerospace and power generating industries. The halogen substitution strategy, known as an effective molecular modification method, can introduce halogen atoms into cations to increase the energy barrier of cationic motion for obtaining compounds with high transition temperature. Herein, by halogenating organic cations of the prototype (N,N-dimethylmorpholinium)PbBr3 (compound 1), we report two triple-channel dielectric/SHG/PL switching materials (N-ClCH2-N-methylmorpholinium)PbBr3 and (N-BrCH2-N-methylmorpholinium) PbBr3 (2 and 3). These compounds adopt a one-dimensional perovskite structure constituted by face-sharing octahedral [PbBr6]− chains and organic cations, and could emit orange-red light under ultraviolet light excitation. The phase transition temperatures of 2 and 3 achieve a very high value: ca. 380 K. Meanwhile, good nonlinear optical properties (SHG) and optimized PL properties were obtained. Thus, multi-functional hybrid perovskites simultaneously with triple-channel switches and optical properties were successfully fabricated. This work might provide a new impetus for designing new organic hybrid perovskites with multi-channel switching behavior and prominent optical properties.
研究领域:
材料科学
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光学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF MOLECULAR STRUCTURE
·
2024
·
IF 4
Liang Jiao,Meifen Huang,Jiajun Xu,Qiuling Yang,Qiong Wu
The manipulation of intermolecular interaction intensities significantly influences a wide range of domains in material science, attracting widespread attention from researchers. In this study, we used a strategy distinct from the adjustment of molecular skeletons, through the introduction of different halogenated ligands, two new coplanar halogenated Schiff base complexes with large conjugate structure [Cu II (3,5-Cl-Salphmen)]·DMF( CuL 3,5-Cl ) and [Cu II (3Br-5Cl-Salphmen)]·DMF( CuL 3Br5Cl ), where 3,5-Cl-Salphmen( H 2 L 3,5-Cl ) = N,N′ -bis(3,5-dichlorosalicylidene)- diamine, 3Br-5Cl-Salphmen( H 2 L 3,5-Br ) = N,N′ -bis(3‑bromo-5-chlorosalicylidene)- diamine were obtained. The effects of different substituted atoms on molecular orbitals, energy levels, intermolecular interstrength are analyzed in detail by DFT theory calculations, and compared with Cu II -3,5-Br-Salphmen( CuL 3,5-Br ) and non-halogenated analogues Cu II -Salphmen( CuL H ). Analysis results show that the strategy of increasing molecular conjugation by the substitution of different halogen atoms can not only effectively modulate the charge distribution on the benzene ring but also can precisely control the binding energy as well as strength of intermolecular interactions .
研究领域:
材料科学
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理论化学
✓ 已验证
产品关联
DOI
高影响因子
ADVANCED FUNCTIONAL MATERIALS
·
2020
·Vol. 31
·期 5
·2008404
·
IF 16.836
Ze Wang,Qi Wei,Xiaodong Liu,Li Liu,Xinyu Tang,Jia Guo,Shengqiang Ren,Guichuan Xing,Dewei Zhao,Yonghao Zheng
Halide substitution in phenethylammonium spacer cations (X-PEA + , X = F, Cl, Br) is a facile strategy to improve the performance of PEA based perovskite solar cells (PSCs). However, the power conversion efficiency (PCE) of X-PEA based quasi-2D (Q-2D) PSCs is still unsatisfactory and the underlying mechanisms are in debate. Here, the in-depth study on the impact of halide substitution on the crystal orientation and multi-phase distribution in PEA based perovskite films are reported. The halide substitution eliminates n = 1 2D perovskite and thus leads to the perpendicular crystal orientation. Furthermore, nucleation competition exists between small- n and large- n phases in PEA and X-PEA based perovskites. This gives rise to the orderly distribution of different n -phases in the PEA and F-PEA based films, and random distribution in Cl-PEA and Br-PEA based films. As a result, (F-PEA) 2 MA 3 Pb 4 I 12 (MA = CH 3 NH 3 + , n = 4) based PSCs achieve a PCE of 18.10%, significantly higher than those of PEA (12.23%), Cl-PEA (7.93%) and Br-PEA (6.08%) based PSCs. Moreover, the F-PEA based devices exhibit remarkably improved stability compared to their 3D counterparts.
研究领域:
材料科学
·
能源科学
✓ 已验证
产品关联
DOI
高影响因子
Advanced Optical Materials
·
2020
·Vol. 8
·期 16
·2000418
·
IF 8.286
Mingze Li,Yawen Li,Maxim S. Molokeev,Jing Zhao,Guangren Na,Lijun Zhang,Zhiguo Xia
Zero-dimensional (0D) organic−inorganic hybrid metal halides haveunprecedented degrees of freedom for structural tunability and photoluminescence modulation. Here, the 0D isomorphic hybrid metal mixed halides (C 9 NH 20 ) 9 Pb 3 Zn 2 Br 19(1− x ) Cl 19 x ( x = 0–1) with continuous halogen contents control, exhibiting tunable emission and enhancement of photoluminescence quantum yield (PLQY) are reported. The competitive bromine to chlorine substitution process in (C 9 NH 20 ) 9 Pb 3 Zn 2 Br 19(1− x ) Cl 19 x occurs first in [ZnBr 4− x Cl x ] 2− tetrahedron before the [Pb 3 Br 11− x Cl x ] 5− trimer. The increasing Cl content in samples from x = 0 to 1 results in an expected blue shift of emission peak from 565 to 516 nm, and meanwhile a strikingly room temperature PL quantum yield increase from 8% to 91%. Combined experimental characterizations and theoretical calculations indicate that the blue shift of interband transition energy is responsible for the emission peak shift. Moreover, with the increasing Cl content, the enhanced electron−phonon interaction and the weakened thermal-assisted nonradiative recombination result in more efficient radiative transition channels and ultimately enhanced PLQY. The impact of halogen substitution on electronic structures and optical properties in 0D hybrid metal halides is emphasized in this work as a new strategy to promote the future development of new luminescent materials.
研究领域:
材料科学
·
光学
✓ 已验证
DOI
高影响因子
BIOMACROMOLECULES
·
2025
·
IF 5.4
Jiahui Yang,Zhiyuan Wang,Zepeng Li,Haoyang Xu,Bin Xue,Yi Cao,Zhaojie Li,Yiran Li
3,4-Dihydroxyphenylalanine (DOPA) has inspired the development of artificial adhesives, but efforts to enhance its adhesion strength and durability continue to evolve. However, it is tough work to improve DOPA wet adhesion by chemically decorating DOPA itself, despite the potential benefit of a concise and high-quality adhesion unit. Here, we synthesized a series of DOPA substituents by introducing different electron-withdrawing groups at the ortho position of the phenyl ring. This modification allowed us to effectively control the adhesion and antioxidation properties of DOPA. Combining atomic force microscopy (AFM)-based single-molecule force spectroscopy (SFMS) and cyclic voltammetry, we comprehensively investigated DOPA’s antioxidation and adhesion capabilities. We found that adding a chlorine or bromine atom to the catechol ring significantly increases the DOPA wet adhesion strength. Additionally, halogen-substituted DOPA exhibited greater stability than dopamine in liquid solutions. Notably, chlorine-substituted DOPA maintained a strong adhesion ability even in salt water, offering potential benefits for bioadhesive applications.
研究领域:
材料科学
·
化学
·
生物黏合剂
·
表面科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Small
·
2023
·Vol. 19
·期 49
·2303127
·
IF 13.3
Meng-Meng Lun,Chang-Yuan Su,Jie Li,Qiang-Qiang Jia,Hai-Feng Lu,Da-Wei Fu,Yi Zhang,Zhi-Xu Zhang
Organic–inorganic hybrid lead halide perovskites (OLHPs), represented by (CH 3 NH 3 )PbI 3 , are one of the research focus due to their exceptional performance in optoelectronic applications, and ferroelastic domain walls are benign to their charge carrier transport that is confirmed recently. Among them, the 1D OLHPs feature better stability against desorption and moisture, but related 1D ones possessing ferroelasticity are rarely investigated and reported so far. In this work, the 1D ferroelastic semiconductor ( N -iodomethyl- N -methyl-morpholinium)PbI 3 ((IDMML)PbI 3 ) is prepared successfully by introducing successively halogenate atoms from Cl, Br to I into the organic cation of the prototype ( N,N -dimethylmorpholinium)PbI 3 ((DMML)PbI 3 ). Notably, (IDMML)PbI 3 shows the narrow bandgap energy (≈2.34 eV) according to the ultraviolet-visible absorption spectrum and the theoretical calculation, and possesses the evident photoconductive characteristic with the on/off ratio of current of ≈50 under the 405 nm light irradiation. This work provides a new case for the ferroelastic OLHPs and will inspire intriguing research in the field of optoelectronic.
研究领域:
材料科学
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光学
·
半导体物理
✓ 已验证
产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）