Towards the Synthesis of Multifunctional Molecular Magnetic Materials Displaying Dual Physical Properties

分子磁学的跨学科领域中最热门的话题之一是寻找混合（多功能）磁体，即，以制备分子和/或分子种类的家族，其不仅具有感兴趣的磁性，例如铁磁性和/或单分子磁性（SMM），而且还将它们与例如光活性、催化、药用或导电性质相结合。SMM可以用于高密度信息存储，量子计算和基于自旋的分子电子学等潜在应用，而其他分子则有利于低温磁冷却，有可能取代目前使用的低温制冷剂氦-3，这既昂贵又非常罕见。所提出的研究的目标是：（i）开发用于合成具有荧光配体的SMM（发射SMM）的策略，（ii）合成光子可接近的SMM，其中将采用激光脉冲来改变晶体中SMM的性质，同时将固体簇保持在低温下，以及（iii）使用发射SMM作为用于活化的高级均相催化剂（即，氧化），例如在H2O到分子O2的光诱导氧化中。通过广泛的方法，并与美国，法国和加拿大的知名团体合作，我们的目标如下：（i）研究SMM在10 - 9至10 - 12秒的时间尺度上表现出的量子行为，这应该受到配体的发射状态和荧光寿命的显著影响，一个强制性要求的操作分子自旋作为真正的模型通用量子门;（ii）检测的SMM的一个分子的存在，通过存在的荧光配体，这是至关重要的，在分子电子学领域的辅助;和（iii）首次开发了作为负载型氧化催化剂的发射性SMM，提供了使用环境友好氧化剂的有效、耐用、低成本（不含贵金属）和可再循环的氧化催化剂。

One of the hottest topics in the interdisciplinary field of Molecular Magnetism is the search for hybrid (multifunctional) magnets, i.e., to make molecules and/or family of molecular species that not only possess interesting magnetic properties, such as ferromagnetism and/or single-molecule magnetism (SMM), but also combine them with photoactive, catalytic, medicinal, or conductive properties, for example. SMMs can find use in potential applications such as high-density information storage, quantum computing and spin-based molecular electronics, while other molecules are beneficial for low-temperature magnetic cooling with the potential for replacing the currently used low-temperature refrigerant, helium-3, which is both expensive and very rare. The goals of the proposed research are: (i) to develop strategies for the synthesis of SMMs with fluorescent ligands (emissive SMMs), (ii) to synthesize photon accessible SMMs, where a laser pulse will be employed to change the nature of a SMM in a crystal while the solid cluster is maintained at low temperature, and (iii) the use of emissive SMMs as advanced homogenous catalysts for the activation (i.e., oxidation) of various substrates, for example in the photo-induced oxidation of H2O to molecular O2. By means of a broad array of methods, and in collaboration with established groups in the USA, France and Canada, our goals are the following: (i) to study the quantum behaviour exhibited by SMMs on a time scale of 10-9 to 10-12 seconds, which should be dramatically affected by the ligands' emissive states and fluorescence lifetimes, a mandatory requirement for the operation of molecular spins as true models for universal quantum gates; (ii) to detect the presence of one molecule of a SMM, aided by the presence of fluorescence ligands, which is of vital importance in the field of molecular electronics; and (iii) to develop for the first time emissive SMMs as supported oxidation catalysts, providing effective, robust, low-cost (without noble metals), and recyclable oxidation catalysts using environmental friendly oxidants.