Magneto-fluorescent nanocomposites: experimental and theoretical linkage for the optimization of magnetic hyperthermia†

Magneto-fluorescent nanocomposites have been recognized as an emerging class of materials displaying great potential for improved magnetic hyperthermia assisted by optical imaging. In this study, we have designed a series of hybrid composites that consist of zinc doped ZnxFe3-xO4 ferrites functionalized by polyethylene-glycol (PEG8000) and an orange-emitting platinum complex [Pt(phen)Cl-2]. Experimental and theoretical studies on the optimization of their magnetically-mediated heating properties were conducted. PEG was assembled around particles' surface by two different approaches; in situ and post-PEGylation. PEGylation ensured the optimal distance between the magnetic core and Pt(ii)-complex to maintain significant luminescence in the composite. The successful inclusion of the complex to the organic matrix was confirmed by a variety of spectroscopic techniques. A theoretical model was developed, based on linear response theory, in order to examine the composites' power losses dependence on their properties. Within this model, inter-particle interactions were quantified by inserting a mean dipolar energy term in the estimation of Neel relaxation time, and consequently, the size and concentration that maximize power loss were derived (20 nm and 4 mg mL(-1)). Moreover, a decrease in the anisotropy of nanoparticles resulted in an increase in specific loss power values. Theoretical estimations are validated by experimental data when heating aqueous dispersions of composites in 24 kA m(-1), 765 kHz AMF for various values of concentration and size. Magnetic hyperthermia results showed that the theory-predicted values of optimum concentration and size delivered the maximum-specific loss power which was found equal to 545 W g(-1). By the present approach, a quantitative link between the particles' dipolar interactions and their heating properties is established, while opening new perspectives to nanotheranostic applications.