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1.
Inorg Chem ; 63(27): 12445-12456, 2024 Jul 08.
Artigo em Inglês | MEDLINE | ID: mdl-38820063

RESUMO

MgMn3(OH)6Cl2 serves readily as the classical Heisenberg kagome antiferromagnet lattice spin frustration material, due to its similarity to herbertsmithite in composition and crystal structure. In this work, nanosheets of MgMn3(OH)6Cl2 are synthesized through a solid-phase reaction. Low-temperature magnetic measurements revealed two antiferromagnetic transitions, occurring at ∼8 and 55 K, respectively. Utilizing high-pressure synchrotron radiation X-ray diffraction techniques, the topological structural evolution of MgMn3(OH)6Cl2 under pressures up to 24.8 GPa was investigated. The sample undergoes a second-order structural phase transition from the rhombohedral phase to the monoclinic phase at pressures exceeding 7.8 GPa. Accompanying the disappearance of the Fano-like line shape in the high-pressure Raman spectra were the emergence of new Raman active modes and discontinuities in the variations of Raman shifts in the high-frequency region. The phase transition to a structure with lower symmetry was attributed to the pressure-induced enhancement of cooperative Jahn-Teller distortion, which is caused by the mutual substitution of Mn2+ ions from the kagome layer and Mg2+ ions from the triangular interlayer. High-pressure ultraviolet-visible absorption measurements support the structural evolution. This research provides a robust experimental approach and physical insights for further exploration of classical geometrical frustration materials with kagome lattice.

2.
Chem Sci ; 14(6): 1479-1484, 2023 Feb 08.
Artigo em Inglês | MEDLINE | ID: mdl-36794196

RESUMO

A novel piezo-activated luminescent material with wide range modulation of the luminescence wavelength and a giant intensity enhancement upon compression was prepared using a strategy of molecular doping. The doping of THT molecules into TCNB-perylene cocrystals results in the formation of a weak but pressure-enhanced emission center in the material at ambient pressure. Upon compression, the emissive band from the undoped component TCNB-perylene undergoes a normal red shift and emission quenching, while the weak emission center shows an anomalous blue shift from 615 nm to 574 nm and a giant luminescence enhancement up to 16 GPa. Further theoretical calculations show that doping by THT could modify intermolecular interactions, promote molecular deformation, and importantly, inject electrons into the host TCNB-perylene upon compression, which contributes to the novel piezochromic luminescence behavior. Based on this finding, we further propose a universal approach to design and regulate the piezo-activated luminescence of materials by using other similar dopants.

3.
Chem Sci ; 14(42): 11629-11637, 2023 Nov 01.
Artigo em Inglês | MEDLINE | ID: mdl-37920334

RESUMO

Unlike the known aggregation-caused quenching (ACQ) that the enhancement of π-π interactions in rigid organic molecules usually decreases the luminescent emission, here we show that an intermolecular "head-to-head" π-π interaction in the phenanthrene crystal, forming the so-called "transannular effect", could result in a higher degree of electron delocalization and thus photoluminescent emission enhancement. Such a transannular effect is molecular configuration and stacking dependent, which is absent in the isomers of phenanthrene but can be realized again in the designed phenanthrene-based cocrystals. The transannular effect becomes more significant upon compression and causes anomalous piezoluminescent enhancement in the crystals. Our findings thus provide new insights into the effects of π-π interactions on luminescence emission and also offer new pathways for designing efficient aggregation-induced emission (AIE) materials to advance their applications.

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