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Abstract The transition from planar to three-dimensional (3D) magnetic nanostructures represents a significant advancement in both fundamental research and practical applications, offering vast potential for next-generation technologies like ultrahigh-density storage, memory, logic, and neuromorphic computing. Despite being a relatively new field, the emergence of 3D nanomagnetism presents numerous opportunities for innovation, prompting the creation of a comprehensive roadmap by leading international researchers. This roadmap aims to facilitate collaboration and interdisciplinary dialogue to address challenges in materials science, physics, engineering, and computing. The roadmap comprises eighteen sections, roughly divided into three blocks. The first block explores the fundamentals of 3D nanomagnetism, focusing on recent trends in fabrication techniques and imaging methods crucial for understanding complex spin textures, curved surfaces, and small-scale interactions. Techniques such as two-photon lithography and focused electron beam-induced deposition enable the creation of intricate 3D architectures, while advanced imaging methods like electron holography and synchrotron x-ray tomography provide nanoscale spatial resolution for studying magnetization dynamics in three dimensions. Various 3D magnetic systems, including coupled multilayer systems, artificial spin-ice, magneto-plasmonic systems, topological spin textures, and molecular magnets are discussed. The second block introduces analytical and numerical methods for investigating 3D nanomagnetic structures and curvilinear systems, highlighting geometrically curved architectures, interconnected nanowire systems, and other complex geometries. Finite element methods are emphasized for capturing complex geometries, along with direct frequency domain solutions for addressing magnonic problems. The final block focuses on 3D magnonic crystals and networks, exploring their fundamental properties and potential applications in magnonic circuits, memory, and spintronics. Computational approaches using 3D nanomagnetic systems and complex topological textures in 3D spintronics are highlighted for their potential to enable faster and more energy-efficient computing. 

The synthesis of a novel family of homoleptic COT-based heterotrimetallic self-assemblies bearing the formula [LnKCa(COT) 3 (THF) 3 ] (Ln( iii ) = Gd, Tb, Dy, Ho, Er, Tm, and Yb) is reported followed by their X-ray crystallographic and magnetic characterization. All crystals conform to the monoclinic P 2 1 / c space group with a slight compression of the unit cell from 3396.4(2) Å 3 to 3373.2(4) Å 3 along the series. All complexes exhibit a triple-decker structure having the Ln( iii ) and K( i ) ions sandwiched by three COT 2− ligands with an end-bound {Ca 2+ (THF) 3 } moiety to form a non-linear (153.5°) arrangement of three different metals. The COT 2− ligands act in a η 8 -mode with respect to all metal centers. A detailed structural comparison of this unique set of heterotrimetallic complexes has revealed consistent trends along the series. From Gd to Yb, the Ln to ring-centroid distance decreases from 1.961(3) Å to 1.827(2) Å. In contrast, the separation of K( i ) and Ca( ii ) ions from the COT-centroid (2.443(3) and 1.914(3) Å, respectively) is not affected by the change of Ln( iii ) ions. The magnetic property investigation of the [LnKCa(COT) 3 (THF) 3 ] series (Ln( iii ) = Gd, Tb, Dy, Ho, Er, and Tm) reveals that the Dy, Er, and Tm complexes display slow relaxation of their magnetization, in other words, single-molecule magnet (SMM) properties. This behaviour is dominated by thermally activated (Orbach-like) and quantum tunneling processes for [DyKCa(COT) 3 (THF) 3 ] in contrast to [ErKCa(COT) 3 (THF) 3 ], in which the thermally activated and Raman processes appear to be relevant. Details of the electronic structures and magnetic properties of these complexes are further clarified with the help of DFT and ab initio theoretical calculations.