Executive Summary : | Two-dimensional (2D) magnetic materials, comprising a few layers of atomically thin crystalline sheets, can potentially act as building blocks for futuristic electronic devices due to their unique magnetic properties. Although it may at times be tractable to manipulate spins using external electric fields, the real challenge remains in designing such kind of 2D materials with tailored magnetic properties that can remain stable even at room temperature so as to eventually make way for facilitating low-energy data storage and information processing. It is believed that, with incorporation of new functionalities, low-dimensional molecular magnets (LDMMs), especially in the form of 2D coordination polymers, can turn out to be quite gainful for faster development of quantum computers. LDMMs usually consist of organic ligands around paramagnetic metal centers (either transition metals or lanthanides) as building blocks. Electron distribution in 4f orbitals of lanthanide ions can play an important role in designing a LDMM for retaining magnetization even in the absence of an external magnetic field. Such kind of designer materials, being lighter in weight, easier to synthesize, and lower in preparation cost (unlike their metal counterparts) are expected to speed up the development of quantum technologies in coming years. An important aspect of LDMMs lies in its ability to enhance the barrier height (Ueff) for magnetization reversal, which could be exploited in high-density information storage devices. It is therefore imperative to understand and control the electron-phonon coupling for designing LDMMs with larger thermal energy barriers to magnetic reversal. Furthermore, spin-orbit coupling with time-reversal symmetry can freeze the spin directions and also, the electron momentum along the metallic edge states of 2D topological insulators, rendering the quantum spin Hall effect (QSHE). If such 2D topological insulators can be made somehow magnetic, the associated time-reversal symmetry breaking may lead to the quantum anomalous Hall effect (QAHE). Even though such defect-tolerant materials with minimal power consumption can be potential candidates for spintronic devices, low operating temperatures often plague their practical efficacies. Development of organic topological materials (OTMs) with well-designed metal-organic coordination may be promising in this regard, not just for its mechanical flexibility, facile fabrication, and low cost, but even from the perspective of possible room-temperature magnetic ordering at molecular scale. We therefore propose here to study the phenomena of electron tunneling and anisotropic magnetoresistance at varying temperatures (10-300 K) in low-dimensional ligand-functionalized molecular magnets interfaced with half- or semi-metallic substrates, utilizing a combination of first-principles analysis and low-temperature magneto-transport measurements, to identify a few potential OTMs for quantum device applications. |