Dressed jeff-1/2 objects in mixed-valence lacunar spinel molybdates

The lacunar-spinel chalcogenides exhibit magnetic centers in the form of transition-metal tetrahedra. On the basis of density-functional computations, the electronic ground state of an Mo413+ tetrahedron has been postulated as single-configuration a12 e4 t25, where a1, e, and t2 are symmetry-adapted linear combinations of single-site Mo t2g atomic orbitals. Here we unveil the many-body tetramer wave-function: we show that sizable correlations yield a weight of only 62% for the a12 e4 t25 configuration. While spin–orbit coupling within the peculiar valence orbital manifold is still effective, the expectation value of the spin–orbit operator and the g factors deviate from figures describing nominal t5 jeff = 1/2 moments. As such, our data documents the dressing of a spin–orbit jeff = 1/2 object with intra-tetramer excitations. Our results on the internal degrees of freedom of these magnetic moments provide a solid theoretical starting point in addressing the intriguing phase transitions observed at low temperatures in these materials

Dressed j eff-1/2 objects in mixed-valence lacunar spinel molybdates

The lacunar-spinel chalcogenides exhibit magnetic centers in the form of transition-metal tetrahedra. On the basis of density-functional computations, the electronic ground state of an Mo413+ tetrahedron has been postulated as single-configuration a12 e4 t25, where a1, e, and t2 are symmetry-adapted linear combinations of single-site Mo t2g atomic orbitals. Here we unveil the many-body tetramer wave-function: we show that sizable correlations yield a weight of only 62% for the a12 e4 t25 configuration. While spin–orbit coupling within the peculiar valence orbital manifold is still effective, the expectation value of the spin–orbit operator and the g factors deviate from figures describing nominal t5jeff = 1/2 moments. As such, our data documents the dressing of a spin–orbit jeff = 1/2 object with intra-tetramer excitations. Our results on the internal degrees of freedom of these magnetic moments provide a solid theoretical starting point in addressing the intriguing phase transitions observed at low temperatures in these materials

Fast non-volatile electric control of antiferromagnetic states

Electrical manipulation of antiferromagnetic states, a cornerstone of antiferromagnetic spintronics, is a great challenge, requiring novel material platforms. Here we report the full control over antiferromagnetic states by voltage pulses in the insulating Co$_3$O$_4$ spinel. We show that the strong linear magnetoelectric effect emerging in its antiferromagnetic state is fully governed by the orientation of the N\'eel vector. As a unique feature of Co$_3$O$_4$, the magnetoelectric energy can easily overcome the weak magnetocrystalline anisotropy, thus, the N\'eel vector can be manipulated on demand, either rotated smoothly or reversed suddenly, by combined electric and magnetic fields. We succeed with switching between antiferromagnetic states of opposite N\'eel vectors by voltage pulses within a few microsecond in macroscopic volumes. These observations render quasi-cubic antiferromagnets, like Co$_3$O$_4$, an ideal platform for the ultrafast (pico- to nanosecond) manipulation of microscopic antiferromagnetic domains and may pave the way for the realization of antiferromagnetic spintronic devices.Comment: 7 pages, 3 figure

Magnetic avalanche of non-oxide conductive domain walls

Atomically sharp domain walls (DWs) in ferroelectrics are considered as an ideal platform to realize easy-to-reconfigure nanoelectronic building blocks, created, manipulated and erased by external fields. However, conductive DWs have been exclusively observed in oxides, where DW mobility and conductivity is largely influenced by stoichiometry and defects. In contrast, we here report on conductive DWs in the non-oxide ferroelectric GaV$_4$S$_8$, where charge carriers are provided intrinsically by multivalent V$_4$ molecular clusters. We show that this new mechanism gives rise to DWs composed of nanoscale stripes with alternating electron and hole conduction, unimaginable in oxides. By exerting magnetic control on these segments we promote the mobile and effectively 2D DWs into dominating the 3D conductance, triggering abrupt conductance changes as large as eight orders of magnitude. The flexible valency, as origin of these novel hybrid DWs with giant conductivity, demonstrates that non-oxide ferroelectrics can be the source of novel phenomena beyond the realm of oxide electronics.Comment: 8 pages, 4 figure

Squeezing the periodicity of Néel-type magnetic modulations by enhanced Dzyaloshinskii-Moriya interaction of 4d electrons

In polar magnets, such as GaV$_{4}$S$_{8}$, GaV$_{4}$Se$_{8}$ and VOSe$_{2}$O$_{5}$, modulated magnetic phases namely the cycloidal and the Néel-type skyrmion lattice states were identified over extended temperature ranges, even down to zero Kelvin. Our combined small-angle neutron scattering and magnetization study shows the robustness of the Néel-type magnetic modulations also against magnetic fields up to 2 T in the polar GaMo$_{4}$S$_{8}$. In addition to the large upper critical field, enhanced spin-orbit coupling stabilize cycloidal, Néel skyrmion lattice phases with sub-10 nm periodicity and a peculiar distribution of the magnetic modulation vectors. Moreover, we detected an additional single-q state not observed in any other polar magnets. Thus, our work demonstrates that non-centrosymmetric magnets with 4d and 5d electron systems may give rise to various highly compressed modulated states

Macroscopic Manifestation of Domain-wall Magnetism and Magnetoelectric Effect in a N\'eel-type Skyrmion Host

We report a magnetic state in GaV$_4$Se$_8$ which emerges exclusively in samples with mesoscale polar domains and not in polar mono-domain crystals. Its onset is accompanied with a sharp anomaly in the magnetic susceptibility and the magnetic torque, distinct from other anomalies observed also in polar mono-domain samples upon transitions between the cycloidal, the N\'eel-type skyrmion lattice and the ferromagnetic states. We ascribe this additional transition to the formation of magnetic textures localized at structural domain walls, where the magnetic interactions change stepwise and spin textures with different spiral planes, hosted by neighbouring domains, need to be matched. A clear anomaly in the magneto-current indicates that the domain-wall-confined magnetic states also have strong contributions to the magnetoelectric response. We expect polar domain walls to commonly host such confined magnetic edge states, especially in materials with long wavelength magnetic order