ABSTRACT
The mutual coupling of spin and lattice degrees of freedom is ubiquitous in magnetic materials and potentially creates exotic magnetic states in response to the external magnetic field. Particularly, geometrically frustrated magnets serve as a fertile playground for realizing magnetic superstructure phases. Here, we observe an unconventional two-step magnetostructural transition prior to a half-magnetization plateau in a breathing pyrochlore chromium spinel by means of state-of-the-art magnetization and magnetostriction measurements in ultrahigh magnetic fields available up to 600 T. Considering a microscopic magnetoelastic theory, the intermediate-field phase can be assigned to a magnetic superstructure with a three-dimensional periodic array of 3-up-1-down and canted 2-up-2-down spin molecules. We attribute the emergence of the magnetic superstructure to a unique combination of the strong spin-lattice coupling and large breathing anisotropy.
ABSTRACT
Bose-Einstein condensation of electron-hole pairs, exciton condensation, has been effortfully investigated since predicted 60 years ago. Irrefutable evidence has still been lacking due to experimental difficulties in verifying the condensation of the charge neutral and non-magnetic spin-singlet excitons. Whilst, condensation of spin-triplet excitons is a promising frontier because spin supercurrent and spin-Seebeck effects will be observable. A canonical cobaltite LaCoO3 under very high magnetic fields is a propitious candidate, yet to be verified. Here, we unveil the exotic phase diagram of LaCoO3 up to 600 T generated using the electromagnetic flux compression method and the state-of-the-art magnetostriction gauge. We found the continuous magnetostriction curves and a bending structure, which suggest the emergence of two distinct spin-triplet exciton condensates. By constructing a phenomenological model, we showed that quantum fluctuations of excitons are crucial for the field-induced successive transitions. The spin-triplet exciton condensation in a cobaltite, which is three-dimensional and thermally equilibrated, opens up a novel venue for spintronics technologies with spin-supercurrent such as a spin Josephson junction.
ABSTRACT
Molecular based spin-1/2 triangular lattice systems such as LiZn2Mo3O8 have attracted research interest. Distortions, defects, and intersite disorder are suppressed in such molecular-based magnets, and intrinsic geometrical frustration gives rise to unconventional and unexpected ground states. Li2AMo3O8 (A = In or Sc) is such a compound where spin-1/2 Mo3O13 clusters in place of Mo ions form the uniform triangular lattice. Their ground states are different according to the A site. Li2InMo3O8 undergoes conventional 120° long-range magnetic order below TN = 12 K whereas isomorphic Li2ScMo3O8 exhibits no long-range magnetic order down to 0.5 K. Here, we report exotic magnetisms in Li2InMo3O8 and Li2ScMo3O8 investigated by muon spin rotation (µSR) and inelastic neutron scattering (INS) spectroscopies using polycrystalline samples. Li2InMo3O8 and Li2ScMo3O8 show completely different behaviors observed in both µSR and INS measurements, representing their different ground states. Li2InMo3O8 exhibits spin wave excitation which is quantitatively described by the nearest neighbor anisotropic Heisenberg model based on the 120° spin structure. In contrast, Li2ScMo3O8 undergoes short-range magnetic order below 4 K with quantum-spin-liquid-like magnetic fluctuations down to the base temperature. Origin of the different ground states is discussed in terms of anisotropies of crystal structures and magnetic interactions.
