Muons and magnets

Abstract:

Although muons are primarily regarded as a local spin probe, they can also access the charge state of an atom or molecule via quadrupolar level crossing resonance (QLCR) spectroscopy. We use Li+TCNQ– (TCNQ = 7,7,8,8-tetracyanoquinodimethane), a simple charge transfer salt, to test the potential of this technique in molecular systems by studying the interaction of a positive muon with the TCNQ nitrogen atoms. We show that both a positive muon and muonium are able to add to the nitrogen, leading to a singlet spin state for the addition molecule. This produces a characteristic three line QLCR spectrum, with the observed line positions and intensities determined by the principal values and orientation of the electric field gradient tensor at the nitrogen. Ab initio calculation of this field gradient and the resulting QLCR spectrum give good agreement with the experiment. A nonresonant background contribution to the relaxation rate also provides evidence for spin excitations rapidly diffusing along the TCNQ chains. These reflect mobile unpaired electrons introduced by muonium addition. It is thus shown that a single set of muon measurements can be sensitive to both spin and charge degrees of freedom in the same molecular material.

Abstract:

Combined resistance noise and muon-spin relaxation (μSR) measurements of the ferromagnetic semiconductor HgCr2Se4 suggest a degree of magnetoelectric coupling and provide evidence for the existence of isolated magnetic polarons. These form at elevated temperatures and undergo a percolation transition with a drastic enhancement of the low-frequency 1/f-type charge fluctuations at the insulator-to-metal transition at ∼95-98K in the vicinity of the magnetic ordering temperature TC∼105-107K. Upon approaching the percolation threshold from above, the strikingly unusual dynamics of a distinct two-level fluctuator superimposed on the 1/f noise can be described by a slowing down of the dynamics of a nanoscale magnetic cluster, a magnetic polaron, when taking into account an effective radius of the polaron depending on the spin correlation length. Coinciding temperature scales found in μSR and noise measurements suggest changes in the magnetic dynamics over a wide range of frequencies and are consistent with the existence of large polarized and domain-wall-like regions at low temperatures, that result from the freezing of spin dynamics at the magnetic polaron percolation transition.