We address the cause of the unusual muon spin relaxation (muSR) results on molecular nanomagnets (MNMs). Through measurements on protonated and deuterated samples of the MNMs Cr7Mn (S=1) and Cr8 (S=0), we show that the muon spin for $S eq 0$ MNMs is relaxed via dynamic fluctuations of the electronic spins. A freezing out of dynamic processes occurs on cooling and at low temperatures the muon spins are relaxed by the electronic spins which themselves are dephased by incoherent nuclear field fluctuations.We observe a transition to a state of static magnetic order of the MNM electronic spins in Cr7Mn below 2 K.
Coherent control of individual molecular spins in nano-devices is a pivotal prerequisite for fulfilling the potential promised by molecular spintronics. By applying electric field pulses during time-resolved electron spin resonance measurements, we measure the sensitivity of the spin in several antiferromagnetic molecular nanomagnets to external electric fields. We find a linear electric field dependence of the spin states in Cr$_7$Mn, an antiferromagnetic ring with a ground-state spin of $S=1$, and in a frustrated Cu$_3$ triangle, both with coefficients of about $2~mathrm{rad}, mathrm{s}^{-1} / mathrm{V} mathrm{m}^{-1}$. Conversely, the antiferromagnetic ring Cr$_7$Ni, isomorphic with Cr$_7$Mn but with $S=1/2$, does not exhibit a detectable effect. We propose that the spin-electric field coupling may be used for selectively controlling individual molecules embedded in nanodevices.
The information accessible from a muon-spin relaxation experiment is often limited since we lack knowledge of the precise muon stopping site. We demonstrate here the possibility of localizing a spin polarized muon in a known stopping state in a molecular material containing fluorine. The muon-spin precession that results from the entangled nature of the muon-spin and surrounding nuclear spins is sensitive to the nature of the stopping site and we use this property to identify three classes of site. We are also able to describe the extent to which the muon distorts its surroundings.
Impressive advances in the field of molecular spintronics allow one to study electron transport through individual magnetic molecules embedded between metallic leads in the purely quantum regime of single electron tunneling. Besides fundamental interest, this experimental setup, in which a single molecule is manipulated by electronic means, provides the elementary units of possible forthcoming technological applications, ranging from spin valves to transistors and qubits for quantum information processing. Theoretically, while for weakly correlated molecular junctions established first-principles techniques do enable the system-specific description of transport phenomena, methods of similar power and flexibility are still lacking for junctions involving strongly correlated molecular nanomagnets. Here we propose an efficient scheme based on the ab initio construction of material-specific Hubbard models and on the master-equation formalism. We apply this approach to a representative case, the Ni$_2$ molecular spin dimer, in the regime of weak molecule-electrode coupling, the one relevant for quantum-information applications. Our approach allows us to study in a realistic setting many-body effects such as current suppression and negative differential conductance. We think that this method has the potential for becoming a very useful tool for describing transport phenomena in strongly correlated molecules.
The magnetization of the prototypical molecular magnet Mn12-acetate exhibits a series of sharp steps at low temperatures due to quantum tunneling at specific resonant values of magnetic field applied along the easy c-axis. An abrupt reversal of the magnetic moment of such a crystal can also occur as an avalanche, where the spin reversal proceeds along a deflagration front that travels through the sample at subsonic speed. In this article we review experimental results that have been obtained for the ignition temperature and the speed of propagation of magnetic avalanches in molecular nanomagnets. Fits of the data with the theory of magnetic deflagration yield overall qualitative agreement. However, numerical discrepancies indicate that our understanding of these avalanches is incomplete.
This mini-review presents a simple and accessible summary on the fascinating physics of quantum nanomagnets coupled to a nuclear spin bath. These chemically synthesized systems are an ideal test ground for the theories of decoherence in mesoscopic quantum degrees of freedom, when the coupling to the environment is local and not small. We shall focus here on the most striking quantum phenomenon that occurs in such nanomagnets, namely the tunneling of their giant spin through a high anisotropy barrier. It will be shown that perturbative treatments must be discarded, and replaced by a more sophisticated formalism where the dynamics of the nanomagnet and the nuclei that couple to it are treated together from the beginning. After a critical review of the theoretical predictions and their experimental verification, we continue with a set of experimental results that challenge our present understanding, and outline the importance of filling also this last gap in the theory.