Addressing individual bistable magnetic molecules, known as Single Molecule Magnets (SMMs), is a fascinating goal at the borderline between molecular magnetism and spin electronics. This tutorial review focuses on the first step towards single-molecule experiments, namely the organization of SMMs on surfaces. Both preparation and characterization of surface-supported SMMs prove to be quite demanding and a multidisciplinary approach is necessary, which is described here using selected examples. We first illustrate the chemical strategies devised to assemble SMMs and to control their orientation on surfaces. Then, we present characterization tools, which have been selected on the basis of their relevance to address specific points, i.e. the chemical composition of the deposited SMM films, the organization of the molecules on the surface, the intramolecular arrangement of the spins, the magnetic anisotropy of SMMs, and eventually the dynamics of their magnetization on surfaces. Particular attention is devoted to techniques exploiting synchrotron light.

Magneto-chiral dichroism is a non-reciprocal—that is, directional—effect observed in magnetized chiral systems, featuring an unbalanced absorption of unpolarized light depending on the direction of the magnetization. Despite the fundamental interest in a phenomenon breaking both parity and time-reversal symmetries, magneto-chiral dichroism is one of the least investigated aspects of light–matter interaction most likely because of the weakness of the effect in most reported experiments. Here we have exploited the element selectivity of hard X-ray radiation to investigate the magneto-chiral properties of enantiopure crystals of two isostructural molecular helicoidal chains comprising either cobalt(II) or manganese(II) ions. A strong magneto-chiral dichroism, with Kuhn asymmetry of the order of a few per cent, has been observed in the cobalt chains system, whereas it is practically absent for the manganese derivative. The spectral features of the X-ray magneto-chiral dichroism signal differ significantly from the natural and magnetic dichroic contributions and have been rationalized here using the multipolar expansion of matter–radiation interaction.

The square antiprismatic Na[Dy(DOTA)(H₂O)]·4H₂O complex was characterised by single crystal X-ray diffraction and ac magnetic susceptometry. Two competing mechanisms for magnetic relaxation as well as the remarkable increase of six orders of magnitude in the relaxation time upon application of a static magnetic field were detected.

Electronic spins in different environments are currently investigated as potential qubits, i.e. the logic units of quantum computers. These have to retain memory of their quantum state for a sufficiently long time (phase memory time, T_m) allowing quantum operations to be performed. For molecular based spin qubits, strategies to increase phase coherence by removing nuclear spins are rather well developed, but it is now crucial to address the problem of the rapid increase of the spin–lattice relaxation rate, T₁ ⁻¹, with increasing temperature that hampers their use at room-temperature. Herein, thanks to the combination of pulsed EPR spectroscopy and AC susceptometry we evidence that an evaporable vanadyl complex of formula VO(dpm)₂, where dpm⁻ is the anion of dipivaloylmethane, presents a combination of very promising features for potential application as molecular spin-qubit. The spin–lattice relaxation time, T₁, studied in detail through AC susceptometry, decreases slowly with increasing temperature and, more surprisingly, it is not accelerated by the application of an external field up to several Teslas. State-of-the art phase memory times for molecular spin systems in protiated environment are detected by pulsed EPR also in moderate dilution, with values of 2.7 μs at 5 K and 2.1 μs at 80 K. Low temperature scanning tunnel microscopy and X-ray photoelectron spectroscopy in situ investigations reveal that intact molecules sublimated in ultra-high vacuum spontaneously form an ordered monolayer on Au(111), opening the perspective of electric access to the quantum memory of ensembles of spin qubits that can be scaled down to the single molecule.