Abstract
We demonstrated the strategy of a nanocomposite design by the incorporation of both a delocalized π-electrons system in a closely bound acceptor-donor analogue chromophore, based on charge-polarizable C(60)(>DPAF-C(9)) nanostructure 1, and spin-polarized d-electrons in the form of γ-FeO(x) nanoparticles. Facile intramolecular electron transfer from the DPAF-C(9) donor moiety to the C(60) acceptor cage of 1 upon activation to the excited state with a long lifetime of the charge-separated state forms a possible mechanism to integrate semiconducting and magnetic properties in a single system. We observed an appreciable magnetocurrent (MC) of C(60)(>DPAF-C(9))-encapsulated magnetic γ-FeO(x) nanoparticles in PMMA matrix upon applying a magnetic field from 0 to 300 mT at either 77 K (12% MC) or 300 K (4.5% MC). Interestingly, the detailed analysis of magnetocurrent curve profiles taken at 77 K allowed us to conclude that the measured magnetocurrent may be attributed to the contributions from magnetic field-dependent excited-state populations in semiconducting structure (density-based MC), magnetism from magnetic structure (mobility-based MC), and product of density and mobility-based MC components (π-d electronic coupling). At the higher temperature region up to 300 K, the semiconducting mechanism dominated the determining factor of measured magnetocurrent. This experimental observation indicated the feasibility of combining delocalized π electrons and spin-polarized d electrons through charge transfer to induce internally coupled dual mobility- and density-based MC through the modulation of spin polarization and excited states in semiconducting/magnetic hybrid materials.
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