RESUMO
This corrects the article DOI: 10.1103/PhysRevLett.129.180402.
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The use of purely organic materials is a promising approach for the miniaturization of devices due to their interesting optical, electronic and magnetic properties. Bisdithiazolyl-based bisDTA compounds have emerged as promising candidates for radical-based single component conductors exhibiting simultaneously magnetic properties. Our computational work focuses on the intriguing magnetism of 4 isostructural pyridine-bridged bisDTA-multifunctional materials triggered by their magnetic and conducting properties being strongly dependent on the different S/Se ratios in the neutral radical skeleton: specifically, bisdithiazolyl (S,S) displays no magnetic order at low temperatures, thiaselenazolyl (Se,S) exhibits spin-canted antiferromagnetism (AFM), and both (S,Se) and bisdiselenazolyl (Se,Se) behave as bulk ferromagnets (FM). Our results reveal that (1) the magnetic response depends on the existence of an intricate network of both AFM and FM spin exchange JAB couplings between neighbouring radicals; and (2) the structural arrangement of π-stacked pairs of radicals sits on a point in the configurational space that is very close to a crossover region where JAB switches from AFM to FM. Indeed, for bulk FM, the experimental response is only accounted for when considering an ab initio optimised crystal structure able to portray adequately the electronic structure of bisDTAs in the region close to the temperature at which magnetic ordering emerges. Magneto-structural correlation maps show the large sensitivity of JAB to very small structural changes with temperature along the π-stacks that lead to drastic changes in the magnetic properties. Clearly, the understanding of magnetism in the title bisDTA compounds is decisive to rationally tailor the properties of multifunctional materials by subtle structural modifications of their crystal packing.
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The magnetic properties of a nanoscale system are inextricably linked to its local environment. In adatoms on surfaces and inorganic layered structures, the exchange interactions result from the relative lattice positions, layer thicknesses, and other environmental parameters. Here, we report on a sample-dependent sign inversion of the magnetic exchange coupling between the three unpaired spins of an organic triradical molecule embedded in a three-terminal device. This ferro-to-antiferromagnetic transition is due to structural distortions and results in a high-to-low spin ground-state change in a molecule traditionally considered to be a robust high-spin quartet. Moreover, the flexibility of the molecule yields an in situ electric tunability of the exchange coupling via the gate electrode. These findings open a route to the controlled reversal of the magnetic states in organic molecule-based nanodevices by mechanical means, electrical gating, or chemical tailoring.
