Muons and magnets

Abstract:

Electron spin dynamics was studied down to 80 mK in the triangular-lattice quantum spin-liquid candidate YbZnGaO₄ using muon spin relaxation, finding no evidence for freezing or ordering of the Yb spins. The muon spin relaxation rate can be represented by the sum of two contributions, one dependent on longitudinal magnetic field and the other independent of field. The field-dependent term follows the form expected for two-dimensional diffusion of mobile spin excitations. The spin-diffusion rate obtained for these excitations in the high temperature paramagnetic regime is comparable with the exchange coupling frequency J/h, reducing significantly in the low temperature quantum regime. This slowdown is assigned to the effect of quantum entanglement. The exchange coupling J is estimated to be 2.0(2) K from the crossover between the two regimes. The field-independent term is only weakly dependent on temperature, and at 15 K its absolute value is consistent with dipolar coupling of the muon to the three Yb moments closest to the muon site, where the spin dynamics of these moments is determined by exchange fluctuations. The temperature-dependent properties in the quantum regime are compared against the three possible U(1) spin-liquid models that have been obtained for the strongly spin-orbit coupled triangular lattice by Y.-D. Li, Y.-M. Lu, and G. Chen [Phys. Rev. B 96, 054445 (2017)]. The comparison with theory takes published specific heat and thermal conductivity data into account, along with the spin-diffusion rate obtained from the muons. It is found that the nodal spin-liquid model U1A11 containing both linear and quadratic nodes provides better agreement with experiment than either the U1A00 spinon Fermi surface (FS) model or the U1A01 model that contains only linear nodes.

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.