A number of studies have suggested that molecular materials could offer similar performance as, or even potentially supersede, those of inorganic materials in spintronics devices. Radically new spintronics functionalities, unavailable with conventional inorganic materials, could stem from the interface between ferromagnetic (FM) and molecular materials, giving rise to the so-called “spinterface” field. In this article, we review the fundamental concepts, recent experiments, and perspectives in this fast rising field, where the functionality is brought from the bulk to the ultimate downscaled device: the interface. The article shows how spin-dependent hybridization at the FM metal/molecule interface can lead to induced spin polarization in the molecular orbitals thanks to spin-dependent broadening and energy shifting of the molecular levels. Interfacial spin polarization can then be tailored thanks to chemical interactions. Examples of enhancement and reversal are given, and we highlight how this spin-dependent hybridization opens a new door for the spintronics crafting of multifunctionality through chemical designing and tuning on the molecular scale.

Organic materials provide a unique platform for exploiting the spin of the electron—a field dubbed organic spintronics. Originally, this was mostly motivated by the notion that because of weak spin-orbit coupling, due to the small mass elements in organics and small hyperfine field coupling, organic matter typically displays a very long electron spin coherence time. More recently, however, it was found that organics provide a special class of spintronic materials for many other reasons—several of which are discussed throughout this issue. Over the past decade, there has been a growing interest in utilizing the molecular spin state as a quantum of information, aiming to develop multifunctional molecular spintronics for memory, sensing, and logic applications. The aim of this issue is to stimulate the interest of researchers by bringing to their attention the vast possibilities not only for unexpected science but also for the enormous potential for developing new functionalities and applications. The six articles in this issue deal with some of the breakthrough work that has been ongoing in this field in recent years.

Organic molecules adsorbed on magnetic surfaces offer the possibility to merge the concepts of molecular electronics with spintronics to build future nanoscale data storage, sensing, and computing multifunctional devices. In order to engineer the functionalities of such hybrid spintronic devices, an understanding of the electronic and magnetic properties of the interface between carbon-based aromatic materials and magnetic surfaces is essential. In this article, we discuss recent progress in the study of spin-dependent chemistry and physics associated with the above molecule-ferromagnet interface by combining state-of-the-art experiments and theoretical calculations. The magnetic properties such as molecular magnetic moment, electronic interface spin-polarization, magnetic anisotropy, and magnetic exchange coupling can be specifically tuned by an appropriate choice of the organic material and the magnetic substrate. These reports suggest a gradual shift in research toward an emerging subfield of interface-assisted molecular spintronics.

Magnetic metal-organic complexes and coordination polymer frameworks can exhibit a transition between two different spin states of the integrated transition-metal ion, an attribute known as a spin-crossover (SCO) transition. This is a spectacular phenomenon that provides magnetic bi-stability and reversible spin-switchability to the material. Consequently, the magnetic state of the metal-organic center can be externally steered by temperature, pressure, or light irradiation. SCO molecules therefore are promising materials for various technological applications, such as spintronics devices, photo-switches, color displays, and information storage units. In spite of the importance of SCO materials in spintronics and other applications, the materials-specific understanding of the SCO phenomenon has remained a challenge. Here we survey recent developments in first-principles computational design of SCO metal-organic materials. A major outcome of recent state-of-the-art investigations is that an accurate quantitative description and even computational design of SCO materials can be provided by density functional theory-based electronic structure calculations combined with ab initio molecular dynamics simulations.