An antiferromagnetically (AFM) coupled biradical based on oxoverdazyl and nitronylnitroxide was synthesized in 46 % yield using Sonogashira coupling. The obtained heterobiradical evidenced distinct properties of both radical entities in solution. Depending on the solvent, the prepared biradical crystallized in two different forms. SQUID magnetization measurements on Form II showed coupling constants J intraII /k B = À 2.1 K and zJ interII / k B = À 11.5 K. Consequently, total intermolecular exchange interactions are five times larger than the intramolecular ones. Further, DFT calculations explained this phenomenon and indicated the advantage of Form I for further in-depth investigations.Weakly antiferromagnetically coupled (AFM) crystalline spin-1 = 2 dimers can serve to investigate critical phenomena such as, the formation of triplon excitations and their interactions in a magnetic field strong enough to close the singlet-triplet gap of the biradicals. Depending on the interdimer exchange interaction (J inter ) relative to the intradimer exchange interaction (J intra ) different dimensionalities of spin systems in a crystalline solid can be observed, such as one-dimensional (1D) spin-ladder systems showing Luttinger-liquid behavior, [1] two-dimensional (2D) Berezinskii-Kosterlitz-Thouless networks, [2] or three-dimensional (3D) Bose-Einstein condensation (BEC) of triplon excitations. [3] Therefore a control of J intra as well as J inter is essential and we have shown earlier that this is possible in organic biradicals, where the intramolecular interactions can be fine-tuned through the applied spacer between the radical units. [4] Besides changing the bridge between the two radical units, two different stable radicals can also be applied for varying the exchange interaction with a given spacer as exhibited for a tetramethoxypyrene with mixed nitronylnitroxide and iminonitroxide. [5] Earlier, we tested two nitronylnitroxides (NN) depicted as A [6,7] in Figure 1 and two iminonitroxides (IN) shown as B [8] with a tolane bridge (1,2-bis(phenyl) acetylene) for achieving 2D and 3D ordering of triplon excitations of these spin dimers in the crystal lattice.. Therefore in the present work, we consider a combination of nitronylnitroxide (NN) and oxoverdazyl radicals (VZ), which is derived from the described homobiradicals A and B (Figure 1). While it is difficult to achieve such a hetero-biradical upon two different kinds of condensation of dialdehyde precursors, Sonogashira [a] Dr.Figure 1. Homobiradicals A and B and the newly designed heterobiradical 1 with tolane bridge.coupling between the two different radical fragments is considered as a prospective pathway.The hetero-biradical 1 was prepared by using a convergent approach that included the reaction between ethynyl-and iodo-substituted radicals (Scheme 1). Both building blocks were synthesized via well-established procedures: verdazyl 2 was prepared from 4-iodobenzaldehyde via published method [9] and the NNR 3 was synthesized according to Klyatskaya et al. [10] Th...

Geometrical frustration among interacting spins combined with strong quantum fluctuations destabilize long-range magnetic order in favor of more exotic states such as spin liquids. By following this guiding principle, a number of spin liquid candidate systems were identified in quasi-two-dimensional (quasi-2D) systems. For 3D, however, the situation is less favorable as quantum fluctuations are reduced and competing states become more relevant. Here we report a comprehensive study of thermodynamic, magnetic and dielectric properties on single crystalline and pressed-powder samples of PbCuTe2O6, a candidate material for a 3D frustrated quantum spin liquid featuring a hyperkagome lattice. Whereas the low-temperature properties of the powder samples are consistent with the recently proposed quantum spin liquid state, an even more exotic behavior is revealed for the single crystals. These crystals show ferroelectric order at TFE ≈ 1 K, accompanied by strong lattice distortions, and a modified magnetic response—still consistent with a quantum spin liquid—but with clear indications for quantum critical behavior.

Alongside the development of artificially created magnetic nanostructures, micro-Hall magnetometry has proven to be a versatile tool to obtain high-resolution hysteresis loop data and access dynamical properties. Here we explore the application of First Order Reversal Curves (FORC)-a technique well-established in the field of paleomagnetism for studying grain-size and interaction effects in magnetic rocks-to individual and dipolar-coupled arrays of magnetic nanostructures using micro-Hall sensors. A proof-of-principle experiment performed on a macroscopic piece of a floppy disk as a reference sample well known in the literature demonstrates that the FORC diagrams obtained by magnetic stray field measurements using home-built magnetometers are in good agreement with magnetization data obtained by a commercial vibrating sample magnetometer. We discuss in detail the FORC diagrams and their interpretation of three different representative magnetic systems, prepared by the direct-write Focused Electron Beam Induced Deposition (FEBID) technique: (1) an isolated Co-nanoisland showing a simple square-shaped hysteresis loop, (2) a more complex CoFe-alloy nanoisland exhibiting a wasp-waist-type hysteresis, and (3) a cluster of interacting Co-nanoislands. Our findings reveal that the combination of FORC and micro-Hall magnetometry is a promising tool to investigate complex magnetization reversal processes within individual or small ensembles of nanomagnets grown by FEBID or other fabrication methods. The method provides sub-μm spatial resolution and bridges the gap of FORC analysis, commonly used for studying macroscopic samples and rather large arrays, to studies of small ensembles of interacting nanoparticles with the high moment sensitivity inherent to micro-Hall magnetometry.

Dynamic susceptibility, commonly referred to as AC susceptibility, χAC, is a powerful tool to characterize a material’s magnetic properties in the presence of a magnetic field B, such as magnetic ordering or spin-relaxation phenomena. The standard technique for accessing χAC is based on measurements of the voltage which is induced in a coil by changes of a sample’s magnetization in response to a small oscillating magnetic field. Importantly, this setup allows for a phase-sensitive detection of the susceptibility, thereby providing information on the magnetization dynamics. This method is frequently used in the low-field range, up to several Tesla, where DC fields are readily available. However, there is a growing demand for such magnetic measurements at higher fields, conveniently accessible by the use of pulse-field technology. Whereas various techniques are available for measuring the in-phase part of the susceptibility χAC′, none of them allows for the determination of the out-of-phase part χAC″. Here we present a realization of an AC susceptometer for measurements of both the in- and out-of-phase component at frequencies up to 47 kHz and an oscillating amplitude of 1.5 mT in a pulsed magnetic field. With this setup, a magnetic signal of 3.6 × 10−6 emu can be resolved. As the setup also enables susceptibility measurements to be performed before and after the field pulse, it can be used to detect temperature changes in response to changes of the magnetic field. This will be demonstrated by measurements on the low-dimensional spin-1/2 system CuSO4·5H2O.