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Molecular Magnetic Materials Based on Nanographenes: Controllable Synthesis and Characterization

Periodic Reporting for period 1 - MolecularMAGNET (Molecular Magnetic Materials Based on Nanographenes: Controllable Synthesis and Characterization)

Reporting period: 2020-08-01 to 2022-07-31

Spintronics based on molecular magnets, in which properties of bulk magnetic materials and molecular quantum effects coexist, has received a lot of attention, with potential applications in molecular spin detection and manipulation for information storage and the realization of spin qubits for quantum computing. One of the driving ideas in this research field has been the expected long spin-lifetime in organic semiconductors due to the presence of light atoms such as carbon or hydrogen, a key asset that spintronics had been missing for years. Nanographenes (NGs) consisting of hexagonal sp2 hybridized carbons is structurally confined nanoscale graphene segments. As a result of their relatively strong electron–phonon coupling and large spin coherence, π-conjugated organic semiconductors may offer a promising alternative approach to semiconductor spintronics. The main objective of this fellowship was to construct NGs with well-defined structure decorating by different spin centers, like organic radicals and rare-earth metals. This fellowship enabled the systematical investigation of the impact of different size and configuration on the behaviour of spin and revealed the intrinsic mechanism of spin-injection and interaction in molecular magnetic materials based on NGs.
During this fellowship, NGs with different spin centers have been synthesized via bottom-up strategy. The design and synthesis of these NGs is based on the consideration as following: structural configuration on the effect of communication between two spin centers; acquiring a strong spin injection to the backbone of NGs via covalent attaching of carbon radicals; solubility on the effect of decoherence of spin coupling. Electron paramagnetic resonance spectroscopy, EPR, was used to investigate couplings and spin dynamics in the materials that synthesized during the action. In collaboration with the Centre for Advanced Electron Spin Resonance in Oxford, EPR experiments were performed at X-band (9.5 GHz), Q-band (34 GHz) and W-band (94 GHz) frequencies. Preliminary results with great promising have been revealed, further characterization is continuing until the end of this action. The results are expecting to be published on one of the renowned peer-reviewed journals with open access. Dissemination of the findings took place through the annual Open Day of Oxford University an invited seminar for the Materials Department at the University of Oxford. Besides, the findings had been further communicated via face-to-face interactions or online approaches between visitors, researchers, and innovators.
The findings under the action, combining the recent results on transport on soluble molecular NGs in the host group, could lead to different attracting possibilities quantum nanoelectronic devices. This is especially true when it comes to the combination of structural precision and reproducibility of synthetic chemistry. By exploiting the atomic control inherent to synthetic chemistry, the properties of molecular magnets can be tailored on an as-needed basis. This fellowship developed reliable and economical synthetic strategies which can provide tremendous candidates for nanoelectronics, leading to practical application. Besides, this fellowship provided a deep understanding of fundamental mechanism of spin-injection and interaction in relation to NGs with different spin centers, offering solid guidance to practical applications. Personally, this prestigious fellowship provided me the great opportunity to direct my own research. The executing of this highly interdisciplinary project enabled me to interact with scientist from different background and equip with the skills of conduct research at the intersection of material science, device physics and nanoelectronic technology.
One of nanographenes synthesized