Combining Molecular Spintronics with Electron Paramagnetic Resonance: The Path Towards Single-Molecule Pulsed Spin Spectroscopy

Abstract

We provide a perspective on how single-molecule magnets can offer a platform to combine quantum transport and paramagnetic spectroscopy, so as to deliver time-resolved electron paramagnetic resonance at the single-molecule level. To this aim, we first review the main principles and recent developments of molecular spintronics, together with the possibilities and limitations offered by current approaches, where interactions between leads and single-molecule magnets are important. We then review progress on the electron quantum coherence on devices based on molecular magnets, and the pulse sequences and techniques necessary for their characterization, which might find implementation at the single-molecule level. Finally, we highlight how some of the concepts can also be implemented by including all elements into a single molecule and we propose an analogy between donor–acceptor triads, where a spin center is sandwiched between a donor and an acceptor, and quantum transport systems. We eventually discuss the possibility of probing spin coherence during or immediately after the passage of an electron transfer, based on examples of transient electron paramagnetic resonance spectroscopy on molecular materials.

Dynamic Magnetic Properties of Germole‐ligated Lanthanide Sandwich Complexes

“…Single‐molecule magnets (SMMs) containing highly anisotropic metal ions have generated considerable interest in recent years owing to their slow magnetic relaxation, magnetic bistability and other valuable properties [1] . Applications of SMMs in prototype molecular spintronic materials have also been reported [2] . In the case of monometallic lanthanide SMMs, single‐ion magnetic anisotropy, coordination symmetry and spin‐phonon interactions have been found to determine the overall SMM performance, in addition to specific features of the various relaxation pathways [3] .…”

“…[1] Applications of SMMs in prototype molecular spintronic materials have also been reported. [2] In the case of monometallic lanthanide SMMs, single‐ion magnetic anisotropy, coordination symmetry and spin‐phonon interactions have been found to determine the overall SMM performance, in addition to specific features of the various relaxation pathways. [3] Of the different subclasses, lanthanide organometallic sandwich and half‐sandwich SMMs have been known for over a decade.…”

Trapping integrated molecular devices via local transport circulation

“…8,44 On the other hand, the highly vulnerable character of electron spins threatens the ultimate goal of quantum device realization, where their deposition between conduction baths and/or on surfaces is deemed to introduce other interactions. 8,45 Therefore, in our present work, we neglect the nuclear spins, thus the above interactions are also neglected in our Hamiltonian, and we concentrate our attentions on the decoherence mechanisms induced by interactions between conduction bands and local molecular orbitals, and those residing in the devices.…”

Lanthanide Phosphonates and Phosphates in Molecular Magnetism

“…The spin populations in a SMM in a bistable ground state get populated in one of the m s states upon magnetization and remain so even after the magnetic field is removed below certain temperatures (Figure 2A). [10] This description is valid for transition metal complexes. On the other hand, for lanthanide complexes, the m j states would be the appropriate descriptors.…”