Muon spin spectroscopy, also known as µSR, is an experimental technique based on the implantation of spin-polarized muons in matter and on the detection of the influence of the atomic, molecular or crystalline surroundings on their spin motion. The motion of the muon spin is due to the magnetic field experienced by the particle and may provide information on its local environment in a very similar way to other magnetic resonance techniques, such as electron spin resonance (ESR or EPR) and, more closely, nuclear magnetic resonance (NMR). Introduction Muon spin spectroscopy is an atomic, molecular and condensed matter experimental technique that exploits nuclear detection methods. In analogy with the acronyms for the previously established spectroscopies NMR and ESR, muon spin spectroscopy is also known as µSR. The acronym stands for muon spin rotation, relaxation, or resonance, depending respectively on whether the muon spin motion is predominantly a rotation (more precisely a precession around a still magnetic field), a relaxation towards an equilibrium direction, or a more complex dynamic dictated by the addition of short radio frequency pulses. µSR does not require any radio-frequency technique to align the probing spin. More generally speaking, muon spin spectroscopy includes any study of the interactions of the muon's magnetic moment with its surroundings when implanted into any kind of matter. Its two most notable features are its ability to study local environments, due to the short effective range of muon interactions with matter, and the characteristic time-window (10−13 – 10−5 s) of the dynamical processes in atomic, molecular and condensed media. The closest parallel to µSR is "pulsed NMR", in which one observes time-dependent transverse nuclear polarization or the so-called "free induction decay" of the nuclear polarization. However, a key difference is that in µSR one uses a specifically implanted spin (the muon's) and does not rely on internal nuclear spins. Although particles are used as a probe, µSR is not a diffraction technique. A clear distinction between the µSR technique and those involving neutrons or X-rays is that scattering is not involved. Neutron diffraction techniques, for example, use the change in energy and/or momentum of a scattered neutron to deduce the sample properties. In contrast, the implanted muons are not diffracted but remain in a sample until they decay. Only a careful analysis of the decay product (i.e. a positron) provides information about the interaction between the implanted muon and its environment in