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Register a new userOrbitally Driven Spin Pairing in the 3D Non-Magnetic Mott Insulator BaVS3: Evidence from Single Crystal Studies
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Static electrical and magnetic properties of single crystal BaVS_3 were measured over the structural (T_S=240K), metal-insulator (T_MI=69K), and suspected orbital ordering (T_X=30K) transitions. The resistivity is almost isotropic both in the metallic and insulating states. An anomaly in the magnetic anisotropy at T_X signals a phase transition to an ordered low-T state. The results are interpreted in terms of orbital ordering and spin pairing within the lowest crystal field quasi-doublet. The disordered insulator at T_X<T<T_MI is described as a classical liquid of non-magnetic pairs.
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Iron pnictides and selenides display a variety of unusual magnetic phases originating from the interplay between electronic, orbital, and lattice degrees of freedom. Using powder inelastic neutron scattering on the two-leg ladder BaFe2Se3, we fully characterize the static and dynamic spin correlations associated with the Fe4 block state, an exotic magnetic ground state observed in this low-dimensional magnet and in Rb0.89Fe1.58Se2. All the magnetic excitations of the Fe4 block state predicted by an effective Heisenberg model with localized spins are observed below 300 meV and quantitatively reproduced. However, the data only account for 16 mub^2 per Fe2+, approximatively 2/3 of the total spectral weight expected for localized S=2 moments. Our results highlight how orbital degrees of freedom in iron-based magnets can conspire to stabilize an exotic magnetic state.
Ultrafast dynamics across the photoinduced three-dimensional Peierls-like insulator-metal (IM) transition in CuIr$_{2}$S$_{4}$ was investigated by means of the all-optical ultrafast multi-pulse time-resolved spectroscopy. The structural coherence of the low-$T$ broken symmetry state is strongly suppressed on a sub-picosecond timescale above a threshold excitation fluence of $F_{mathrm{c}}approx3$ mJ/cm$^{2}$ (at 1.55-eV photon energy) resulting in a structurally inhomogeneous transient state which persists for several-tens of picoseconds before reverting to the original low-$T$ state. The electronic order shows a transient gap filling at a significantly lower fluence threshold of $sim0.6$~mJ/cm$^{2}$. The data suggest that the photoinduced-transition structural dynamics to the high-$T$ metallic phase is governed by first-order-transition nucleation kinetics that prevents the complete structural transition into the high-$T$ phase even at excitation fluences significantly larger than $F_{mathrm{c}}$. In contrast, the dynamically-decoupled electronic order is suppressed rather independently due to a photoinduced Mott transition.
The spinel-structure CuIr$_{2}$S$_{4}$ compound displays a rather unusual orbitally-driven three-dimensional Peierls-like insulator-metal transition. The low-T symmetry-broken insulating state is especially interesting due to the existence of a metastable irradiation-induced disordered weakly conducting state. Here we study intense femtosecond optical pulse irradiation effects by means of the all-optical ultrafast multi-pulse time-resolved spectroscopy. We show that the structural coherence of the low-T broken symmetry state is strongly suppressed on a sub-picosecond timescale above a threshold excitation fluence resulting in a structurally inhomogeneous transient state which persists for several-tens of picoseconds before reverting to the low-T disordered weakly conducting state. The electronic order shows a transient gap filling at a significantly lower fluence threshold. The data suggest that the photoinduced-transition dynamics to the high-T metallic phase is governed by first-order-transition nucleation kinetics that prevents the complete ultrafast structural transition even when the absorbed energy significantly exceeds the equilibrium enthalpy difference to the high-T metallic phase. In contrast, the dynamically-decoupled electronic order is transiently suppressed on a sub-picosecond timescale rather independently due to a photoinduced Mott transition.
Since the beginnings of the electronic age, a quest for ever faster and smaller switches has been initiated, since this element is ubiquitous and foundational in any electronic circuit to regulate the flow of current. Mott insulators are promising candidates to meet this need as they undergo extremely fast resistive switching under electric field. However the mechanism of this transition is still under debate. Our spatially-resolved {mu}-XRD imaging experiments carried out on the prototypal Mott insulator (V0.95Cr0.05)2O3 show that the resistive switching is associated with the creation of a conducting filamentary path consisting in an isostructural compressed phase without any chemical nor symmetry change. This clearly evidences that the resistive switching mechanism is inherited from the bandwidth-controlled Mott transition. This discovery might hence ease the development of a new branch of electronics dubbed Mottronics.
We present first principles calculations of the magnetic and orbital properties of Ba$_2$NaOsO$_6$ (BNOO), a 5$d^1$ Mott insulator with strong spin orbit coupling (SOC) in its low temperature emergent quantum phases. Our computational method takes into direct consideration recent NMR results that established that BNOO develops a local octahedral distortion preceding the formation of long range magnetic order. We found that the two-sublattice canted ferromagnetic ground state identified in Lu etal, Nature Comm. {bf 8}, 14407 (2017) is accompanied by a two-sublattice staggered orbital ordering pattern in which the $t_{2g}$ orbitals are selectively occupied as a result of strong spin orbit coupling. The staggered orbital order found here using first principles calculations asserts the previous proposal of Chen etal, Phys. Rev. B {bf 82}, 174440 (2010) and Lu etal, Nature Comm. {bf 8}, 14407 (2017), that two-sublattice magnetic structure is the very manifestation of staggered quadrupolar order. Therefore, our results affirm the essential role of multipolar spin interactions in the microscopic description of magnetism in systems with locally entangled spin and orbital degrees of freedom.
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