Tunable Magnetic Domains in Ferrimagnetic MnSb2Te4.

Highly tunable properties make Mn(Bi,Sb)2Te4 a rich playground for exploring the interplay between band topology and magnetism: On one end, MnBi2Te4 is an antiferromagnetic topological insulator, while the magnetic structure of MnSb2Te4 (MST) can be tuned between antiferromagnetic and ferrimagnetic. Motivated to control electronic properties through real-space magnetic textures, we use magnetic force microscopy (MFM) to image the domains of ferrimagnetic MST. We find that magnetic field tunes between stripe and bubble domain morphologies, raising the possibility of topological spin textures. Moreover, we combine in situ transport with domain manipulation and imaging to both write MST device properties and directly measure the scaling of the Hall response with the domain area. This work demonstrates measurement of the local anomalous Hall response using MFM and opens the door to reconfigurable domain-based devices in the M(B,S)T family.

Domain Wall Dynamics in a Ferroelastic Spin Crossover Complex with Giant Magnetoelectric Coupling.

Pinned and mobile ferroelastic domain walls are detected in response to mechanical stress in a Mn3+ complex with two-step thermal switching between the spin triplet and spin quintet forms. Single-crystal X-ray diffraction and resonant ultrasound spectroscopy on [MnIII(3,5-diCl-sal2(323))]BPh4 reveal three distinct symmetry-breaking phase transitions in the polar space group series Cc → Pc → P1 → P1(1/2). The transition mechanisms involve coupling between structural and spin state order parameters, and the three transitions are Landau tricritical, first order, and first order, respectively. The two first-order phase transitions also show changes in magnetic properties and spin state ordering in the Jahn-Teller-active Mn3+ complex. On the basis of the change in symmetry from that of the parent structure, Cc, the triclinic phases are also ferroelastic, which has been confirmed by resonant ultrasound spectroscopy. Measurements of magnetoelectric coupling revealed significant changes in electric polarization at both the Pc → P1 and P1 → P1(1/2) transitions, with opposite signs. All these phases are polar, while P1 is also chiral. Remanent electric polarization was detected when applying a pulsed magnetic field of 60 T in the P1→ P1(1/2) region of bistability at 90 K. Thus, we showcase here a rare example of multifunctionality in a spin crossover material where the strain and polarization tensors and structural and spin state order parameters are strongly coupled.

Thermal and Magnetic Field Switching in a Two-Step Hysteretic MnIII Spin Crossover Compound Coupled to Symmetry Breakings.

A MnIII spin crossover complex with atypical two-step hysteretic thermal switching at 74 K and 84 K shows rich structural-magnetic interplay and magnetic-field-induced spin state switching below 14 T with an onset below 5 T. The spin states, structures, and the nature of the phase transitions are elucidated via X-ray and magnetization measurements. An unusual intermediate phase containing four individual sites, where 1 / 4 are in a pure low spin state, is observed. The splitting of equivalent sites in the high temperature phase into four inequivalent sites is due to a structural reorganization involving a primary and a secondary symmetry-breaking order parameter that induces a crystal system change from orthorhombic→monoclinic and a cell doubling. Further cooling leads to a reconstructive phase transition and a monoclinic low-temperature phase with two inequivalent low-spin sites. The coupling between the order parameters is identified in the framework of Landau theory.

Giant Magnetoelectric Coupling and Magnetic-Field-Induced Permanent Switching in a Spin Crossover Mn(III) Complex.

We investigate giant magnetoelectric coupling at a Mn3+ spin crossover in [MnIIIL]BPh4 (L = (3,5-diBr-sal)2323) with a field-induced permanent switching of the structural, electric, and magnetic properties. An applied magnetic field induces a first-order phase transition from a high spin/low spin (HS-LS) ordered phase to a HS-only phase at 87.5 K that remains after the field is removed. We observe this unusual effect for DC magnetic fields as low as 8.7 T. The spin-state switching driven by the magnetic field in the bistable molecular material is accompanied by a change in electric polarization amplitude and direction due to a symmetry-breaking phase transition between polar space groups. The magnetoelectric coupling occurs due to a γη2 coupling between the order parameter γ related to the spin-state bistability and the symmetry-breaking order parameter η responsible for the change of symmetry between polar structural phases. We also observe conductivity occurring during the spin crossover and evaluate the possibility that it results from conducting phase boundaries. We perform ab initio calculations to understand the origin of the electric polarization change as well as the conductivity during the spin crossover. Thus, we demonstrate a giant magnetoelectric effect with a field-induced electric polarization change that is 1/10 of the record for any material.

Stress-Induced Domain Wall Motion in a Ferroelastic Mn3+ Spin Crossover Complex.

Domain wall motion is detected for the first time during the transition to a ferroelastic and spin state ordered phase of a spin crossover complex. Single-crystal X-ray diffraction and resonant ultrasound spectroscopy (RUS) revealed two distinct symmetry-breaking phase transitions in the mononuclear Mn3+ compound [Mn(3,5-diBr-sal2 (323))]BPh4 , 1. The first at 250 K, involves the space group change Cc→Pc and is thermodynamically continuous, while the second, Pc→P1 at 85 K, is discontinuous and related to spin crossover and spin state ordering. Stress-induced domain wall mobility was interpreted on the basis of a steep increase in acoustic loss immediately below the the Pc-P1 transition.

Quantum Oscillations in Flux-Grown SmB_{6} with Embedded Aluminum.

SmB_{6} is a candidate topological Kondo insulator that displays surface conduction at low temperatures. Here, we perform torque magnetization measurements as a means to detect de Haas-van Alphen (dHvA) oscillations in SmB_{6} crystals grown by aluminum flux. We find that dHvA oscillations occur in single crystals containing embedded aluminum, originating from the flux used to synthesize SmB_{6}. Measurements on a sample with multiple, unconnected aluminum inclusions show that aluminum crystallizes in a preferred orientation within the SmB_{6} cubic lattice. The presence of aluminum is confirmed through bulk susceptibility measurements, but does not show a signature in transport measurements. We discuss the ramifications of our results.

Structure-Property Relations in Multiferroic [(CH3)2NH2] M(HCOO)3 ( M = Mn, Co, Ni).

We bring together magnetization, infrared spectroscopy, and lattice dynamics calculations to uncover the magnetic field-temperature ( B- T) phase diagrams and vibrational properties of the [(CH3)2NH2] M(HCOO)3 ( M = Mn2+, Co2+, Ni2+) family of multiferroics. While the magnetically driven transition to the fully saturated state in [(CH3)2NH2]Mn(HCOO)3 takes place at 15.3 T, substitution with Ni or Co drives the critical fields up toward 100 T, an unexpectedly high energy scale for these compounds. Analysis of the infrared spectrum of the Mn and Ni compounds across TC reveals doublet splitting of the formate bending mode which functions as an order parameter of the ferroelectric transition. By contrast, [(CH3)2NH2]Co(HCOO)3 reveals a surprising framework rigidity across the order-disorder transition due to modest distortions around the Co2+ centers. The transition to the ferroelectric state is thus driven by the dimethylammonium cation freezing and the resulting hydrogen bonding. Under applied field, the Mn (and most likely, the Ni) compounds engage the formate bending mode to facilitate the transition to their fully saturated magnetic states, whereas the Co complex adopts a different mechanism involving formate stretching distortions to lower the overall magnetic energy. Similar structure-property relations involving substitution of transition-metal centers and control of the flexible molecular architecture are likely to exist in other molecule-based multiferroics.

High Curie temperature ferromagnetic structures of (Sb2Te3)1-x(MnSb2Te4)x with x = 0.7-0.8.

Magnetic topological materials are promising for realizing novel quantum physical phenomena. Among these, bulk Mn-rich MnSb2Te4 is ferromagnetic due to MnSb antisites and has relatively high Curie temperatures (TC), which is attractive for technological applications. We have previously reported the growth of materials with the formula (Sb2Te3)1-x(MnSb2Te4)x, where x varies between 0 and 1. Here we report on their magnetic and transport properties. We show that the samples are divided into three groups based on the value of x (or the percent septuple layers within the crystals) and their corresponding TC values. Samples that contain x < 0.7 or x > 0.9 have a single TC value of 15-20 K and 20-30 K, respectively, while samples with 0.7 < x < 0.8 exhibit two TC values, one (TC1) at ~ 25 K and the second (TC2) reaching values above 80 K, almost twice as high as any reported value to date for these types of materials. Structural analysis shows that samples with 0.7 < x < 0.8 have large regions of only SLs, while other regions have isolated QLs embedded within the SL lattice. We propose that the SL regions give rise to a TC1 of ~ 20 to 30 K, and regions with isolated QLs are responsible for the higher TC2 values. Our results have important implications for the design of magnetic topological materials having enhanced properties.

Field-tunable toroidal moment in a chiral-lattice magnet.

Ferrotoroidal order, which represents a spontaneous arrangement of toroidal moments, has recently been found in a few linear magnetoelectric materials. However, tuning toroidal moments in these materials is challenging. Here, we report switching between ferritoroidal and ferrotoroidal phases by a small magnetic field, in a chiral triangular-lattice magnet BaCoSiO4 with tri-spin vortices. Upon applying a magnetic field, we observe multi-stair metamagnetic transitions, characterized by equidistant steps in the net magnetic and toroidal moments. This highly unusual ferri-ferroic order appears to come as a result of an unusual hierarchy of frustrated isotropic exchange couplings revealed by first principle calculations, and the antisymmetric exchange interactions driven by the structural chirality. In contrast to the previously known toroidal materials identified via a linear magnetoelectric effect, BaCoSiO4 is a qualitatively new multiferroic with an unusual coupling between several different orders, and opens up new avenues for realizing easily tunable toroidal orders.

Cryogenic goniometer for measurements in pulsed magnetic fields fabricated via additive manufacturing technique.

Complex high-precision mechanical devices can be fabricated using a three-dimensional printing technology with the help of computer-aided design. Using 3D stereolithography, we have constructed a cryogenic goniometer for measurements in pulsed magnetic fields of up to 100 T, at temperatures as low as 0.5 K. We review the properties of several materials tested in developing the goniometer and report on its design and performance. The goniometer allows samples to be rotated in situ to a precision of 0.2° so that the field can be applied at many different angles to the samples' symmetry directions. Following its success, we establish that 3D printing is now a viable technology for pulsed field and other cryogenic probes.

Author Correction: Influence of microstructure on superconductivity in KxFe2-ySe2 and evidence for a new parent phase K2Fe7Se8.

An amendment to this paper has been published and can be accessed via a link at the top of the paper.

Measurement of the angle dependence of magnetostriction in pulsed magnetic fields using a piezoelectric strain gauge.

We present a high resolution method for measuring magnetostriction in millisecond pulsed magnetic fields at cryogenic temperatures with a sensitivity of 1.11×10-11/Hz . The sample is bonded to a thin piezoelectric plate such that when the sample's length changes, it strains the piezoelectric and induces a voltage change. This method is more sensitive than a fiber-Bragg grating method. It measures two axes simultaneously instead of one. The gauge is small and versatile, functioning in DC and millisecond pulsed magnetic fields. We demonstrate its use by measuring the magnetostriction of Ca3Co1.03Mn0.97O6 single crystals in pulsed magnetic fields. By comparing our data to new and previously published results from a fiber-Bragg grating magnetostriction setup, we confirm that this method detects magnetostriction effects. We also demonstrate the small size and versatility of this technique by measuring angle dependence with respect to the applied magnetic field in a rotator probe in 65 T millisecond pulsed magnetic fields.

Influence of microstructure on superconductivity in KxFe2-ySe2 and evidence for a new parent phase K2Fe7Se8.

The search for new superconducting materials has been spurred on by the discovery of iron-based superconductors whose structure and composition is qualitatively different from the cuprates. The study of one such material, KxFe2-ySe2 with a critical temperature of 32 K, is made more difficult by the fact that it separates into two phases-a dominant antiferromagnetic insulating phase K2Fe4Se5, and a minority superconducting phase whose precise structure is as yet unclear. Here we perform electrical and magnetization measurements, scanning electron microscopy and microanalysis, X-ray diffraction and scanning tunnelling microscopy on KxFe2-ySe2 crystals prepared under different quenching processes to better understand the relationship between its microstructure and its superconducting phase. We identify a three-dimensional network of superconducting filaments within this material and present evidence to suggest that the superconducting phase consists of a single Fe vacancy for every eight Fe-sites arranged in a √8 x √10 parallelogram structure.