Orientational Dynamics of Magnetic Iron Oxide Nanoparticles in a Hydrogel: Observation by Magnetic Linear Dichroism...

For the success of biomedical applications of magnetic iron oxide nanoparticles (MION), such as magnetic hyperthermia and magnetic particle imaging, it is essential to understand the orientational dynamics of MION in a complex fluid under an alternating field. Here, using the magnetic linear dichroism (MLD) measurement, we directly observed the orientational behavior of MION in a hydrogel under a damped oscillating magnetic field (DOMF) of 33 kHz in frequency. Hydrophobically modified ethoxylated urethane (HEUR) is examined as the network polymer because the mesh size of the network is controllable with its concentration. We used two MIONs: a bare MION (MION1) and a MION coated with an amphiphilic polymer (MION2). Where the mesh size of the gel network is larger than the particle's hydrodynamic diameter, MION1 in the hydrogel rotates in the same manner in a simple solution, although the macroscopic rheological property of the medium is quite different. Meanwhile, the orientational behavior of MION2 is dramatically changed by the addition of HEUR molecules even below the minimum gelation concentration, indicating that MION2 is associated with the flower micelles of HEUR. By analyzing the MLD waveform, the orientational behavior of MION1 in the HEUR gel under a DOMF can be explained with single-mode relaxation, whereas that of MION2 is complicated; a rapid partial rotation near the particle and a whole slow rotation of the particle-flower micelle associate are superimposed. It is hard to distinguish this difference in orientational behaviors from the dynamic magnetization curve because the dominant magnetization reversal process is Néel rotation, the rotation of the magnetic moment in the particle. The MLD measurement is a potential tool for optimizing biomedical techniques utilizing MIONs and for nanorheology or colloid science in a complex matrix such as a hydrogel or cytoplasmic matrix.