A mononuclear complex with long alkyl chains, [Fe(HBpz)(Cbpy)] (1; HBpz = dihydrobis(1-pyrazolyl)borate, Cbpy = 4,4'-dinonyl-2,2'-bipyridine), was synthesized. Single-crystal X-ray crystallographic studies revealed that the Δ- and Λ-forms of the complex co-crystallized in the lattice asymmetric unit, while magnetic measurements unveiled that this complex underwent incomplete one-step spin crossover (SCO) with the transition completeness and temperature depending on the measurement velocity because of slow spin equilibrium. Multivariable approaches such as varying scan rate, annealing the sample, light irradiation and pressure have been adopted to effectively overcome the slow spin equilibrium and thus improve the SCO completeness.
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Angew Chem Int Ed Engl
January 2025
University of Science and Technology of China, Chemistry and Material Science, No.96, JinZhai Road Baohe District, 230026, Hefei, CHINA.
Multi-resonance thermally activated delayed fluorescence (MR-TADF) materials have great potential for applications in ultrahigh-definition (UHD) organic light-emitting diode (OLED) displays, that benefit from their narrowband emission characteristic. However, key challenges such as aggregation-caused quenching (ACQ) effect and slow triplet-to-singlet spin-flip process, especially for blue MR-TADF materials, continue to impede their development due to planar skeletons and relatively large ΔESTs. Here, an effective strategy that incorporates multiple carbazole donors into the parent MR moieties is proposed, synergistically engineering their excited states and steric hindrances to enhance both the spin-flip process and quenching resistance.
View Article and Find Full Text PDFChem Sci
December 2024
State Key Laboratory of Catalysis, Dalian National Laboratory for Clean Energy, Dalian Institute of Chemical Physics, Chinese Academy of Sciences Zhongshan Road 457 Dalian 116023 China
In solid-state NMR, dipolar-based heteronuclear polarization transfer has been extensively used for sensitivity enhancement and multidimensional correlations, but its efficiency often suffers from undesired spin interactions and hardware limitations. Herein, we propose a novel dipolar-echo edited R-symmetry (DEER) sequence, which is further incorporated into the INEPT-type scheme, dubbed DEER-INEPT, for achieving highly efficient heteronuclear polarization transfer. Numerical simulations and NMR experiments demonstrate that DEER-INEPT offers significantly improved robustness, enabling efficient polarization transfer under a wide range of MAS conditions, from slow to ultrafast rates, outperforming existing methods.
View Article and Find Full Text PDFPhys Rev Lett
December 2024
Harish-Chandra Research Institute, A CI of Homi Bhabha National Institute, Chhatnag Road, Jhusi, Allahabad 211019, India.
Pump-probe response of the spin-orbit coupled Mott insulator Sr_{2}IrO_{4} reveals a rapid creation of low-energy optical weight and suppression of three-dimensional magnetic order on laser pumping. Postpump there is a quick reduction of the optical weight but a very slow recovery of the magnetic order-the difference is attributed to weak interlayer exchange in Sr_{2}IrO_{4} delaying the recovery of three-dimensional magnetic order. We suggest that the effect has a very different and more fundamental origin.
View Article and Find Full Text PDFJ Phys Condens Matter
December 2024
Departmet of Physics(MMV), Banaras Hindu University, Varanasi, Varanasi, Uttar Pradesh, 221005, INDIA.
We report a detailed experimental study of the structural, magnetic and electrical properties of La and Ru doped (Sr1-x Lax)2Ir1-xRuxO4 (x= 0.05, 0.15).
View Article and Find Full Text PDFSmall
December 2024
College of Material Science and Engineering, Zhejiang University of Technology, Hangzhou, 310014, P. R. China.
Lithium-sulfur batteries (LSBs) face challenges from the shuttle effect of lithium polysulfides (LiPSs) and slow redox kinetics. In this study, a NiCo-Doped 3D Ordered Mesoporous Carbon (NiCo-3DOMC) composite material is synthesized using a gel-crystalline template and sol-gel method to modify polypropylene separators in LSBs. Density Functional Theory calculations and experiment results demonstrate that under a magnetic field, the NiCo-3DOMC enhances adsorption and catalyzes the conversion of LiPSs, effectively mitigating the shuttle effect and boosting redox kinetics.
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