No Arabic abstract
Trivalent americium has a non-magnetic ($J$ = 0) ground state arising from the cancelation of the orbital and spin moments. However, magnetism can be induced by a large molecular field if Am$^{3+}$ is embedded in a ferromagnetic matrix. Using the technique of x-ray magnetic circular dichroism, we show that this is the case in AmFe$_2$. Since $langle J_z rangle$ = 0, the spin component is exactly twice as large as the orbital one, the total Am moment is opposite to that of Fe, and the magnetic dipole operator $langle T_{z} rangle$ can be determined directly; we discuss the progression of the latter across the actinide series.
Spin-orbit Mott insulators composed of $t_{2g}^4$ transition metal ions may host excitonic magnetism due to the condensation of spin-orbital $J=1$ triplons. Prior experiments suggest that the $4d$ antiferromagnet Ca$_{2}$RuO$_{4}$ embodies this notion, but a $J = 0$ nonmagnetic state as a basis of the excitonic picture remains to be confirmed. We use Ru $L_3$-edge resonant inelastic x-ray scattering to reveal archetypal $J$ multiplets with a $J=0$ ground state in the cubic compound K$_{2}$RuCl$_{6}$, which are well described within the $LS$-coupling scheme. This result highlights the critical role of unquenched orbital moments in $4d$-electron compounds and calls for investigations of quantum criticality and excitonic magnetism on various crystal lattices.
Strong spin-orbit coupling (SOC) effects of heavy $d$-orbital elements have long been neglected in describing the ground states of their compounds thereby overlooking a variety of fascinating and yet unexplored magnetic and electronic states, until recently. The spin-orbit entangled electrons in such compounds can get stabilized into unusual spin-orbit multiplet $J$-states which warrants severe investigations. Here we show using detailed magnetic and thermodynamic studies and theoretical calculations the ground state of Ba$_3$ZnIr$_2$O$_9$, a 6$H$ hexagonal perovskite is a close realisation of the elusive $J$~=~0 state. However, we find that local Ir moments are spontaneously generated due to the comparable energy scales of the singlet-triplet splitting driven by SOC and the superexchange interaction mediated by strong intra-dimer hopping. While the Ir ions within the structural Ir$_2$O$_9$ dimer prefers to form a spin-orbit singlet state (SOS) with no resultant moment, substantial interdimer exchange interactions from a frustrated lattice ensure quantum fluctuations till the lowest measured temperatures and stabilize a spin-orbital liquid phase.
Entanglement of spin and orbital degrees of freedom drives the formation of novel quantum and topological physical states. Discovering new spin-orbit entangled ground states and emergent phases of matter requires both experimentally probing the relevant energy scales and applying suitable theoretical models. Here we report resonant inelastic x-ray scattering measurements of the transition metal oxides Ca$_3$LiOsO$_6$ and Ba$_2$YOsO$_6$. We invoke an intermediate coupling approach that incorporates both spin-orbit coupling and electron-electron interactions on an even footing and reveal the ground state of $5d^3$ based compounds, which has remained elusive in previously applied models, is a novel spin-orbit entangled J=3/2 electronic ground state. This work reveals the hidden diversity of spin-orbit controlled ground states in 5d systems and introduces a new arena in the search for spin-orbit controlled phases of matter.
The Per2M(mnt)2 class of organic conductors exhibit a charge density wave (CDW) ground state below about 12 K, which may be suppressed in magnetic fields of order 20 to 30 T. However, for both cases of counter ion M(mnt)2 species studied (M = Au (zero spin) and M = Pt (spin 1/2)), new high field ground states evolve for further increases in magnetic field. We report recent investigations where thermopower, Hall effect, high pressure and additional transport measurements have been carried out to explore these new high field phases.
The magnetic ground state of the hyper-kagome lattice in Na4Ir3O8 is explored via combined bulk magnetization, muon spin relaxation, and neutron scattering measurements. A short-range, frozen, state comprised of quasi-static moments develops below a characteristic temperature of T_F=6 K, revealing an inhomogeneous distribution of spins occupying the entirety of the sample volume. Quasi-static, short-range, spin correlations persist until at least 20 mK and differ substantially from the nominally dynamic response of a quantum spin liquid. Our data demonstrate that an inhomogeneous magnetic ground state arises in Na4Ir3O8 driven either by disorder inherent to the creation of the hyper-kagome lattice itself or stabilized via quantum fluctuations.