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

分子磁学交叉学科领域中最热门的话题之一是寻找杂化(多功能)磁体，即制造分子和/或分子物种家族，这些分子和/或分子物种不仅具有有趣的磁性，例如铁磁性和/或单分子磁性(SMM)，而且还结合了光活性、催化、医疗或导电性能。SMM可用于高密度信息存储、量子计算和自旋分子电子等潜在应用，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，后者既昂贵又非常稀有。拟议研究的目标是：(I)开发合成带有荧光配体的SMM(发光SMM)的策略，(Ii)合成光子可达SMM，其中将使用激光脉冲来改变晶体中SMM的性质，同时保持固体团簇的低温，以及(Iii)使用发射SMM作为先进的均相催化剂来活化(即氧化)各种底物，例如在光诱导H2O氧化为分子O2的过程中。通过广泛的方法，并与美国、法国和加拿大的现有研究小组合作，我们的目标如下：(I)在10-9到10-12秒的时间尺度上研究SMM表现出的量子行为，这应该受到配体的发射态和荧光寿命的显著影响，这是作为通用量子门的真实模型的分子自旋操作的强制性要求；(Ii)在荧光配体的存在的帮助下，检测SMM的一个分子的存在，这在分子电子学领域是至关重要的；以及(Iii)首次开发发射SMM作为负载型氧化催化剂，提供有效、坚固、低成本(不含贵金属)和可回收的使用环境友好氧化剂的氧化催化剂。

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.