Magnetic/plasmonic hybrid nanoparticles are highly desirable for multimodal bioimaging and biosensing. Although the synthesis of heterodimeric nanoparticles has been reported, the products are usually hydrophobic so that post-treatment procedures are required to transfer them into water which are often difficult to perform and cause damages to the structures. Direct synthesis of hydrophilic hybrid nanostructures has remained a grand challenge albeit its immediate advantage of biocompatibility. Herein we report a general seed-mediated approach to the synthesis of hydrophilic and biocompatible M−Fe 3 O 4 (M = Au, Ag, and Pd) heterodimers, in which the size of metals and Fe 3 O 4 can be independently regulated in a wide range. Benefiting from the aqueous synthesis, this approach can be further extended to design more complex heterodimeric structures such as AgPt alloy −Fe 3 O 4 , Au core @Pd shell −Fe 3 O 4 , and Au shell −Fe 3 O 4 . The hydrophilic nature of our heterodimers makes them readily useful for biomedical applications without the need of additional ligand exchange processes in contrast to those prepared in nonpolar solvents. These nanoscale magnetic/ plasmonic heterostructures were shown to be ideally suited for integrated biomedical diagnoses, such as magnetic resonance imaging, photoacoustic imaging, optical coherence tomography, and computed tomography, in virtue of their biocompatibility and combined tunable magnetic and plasmonic properties.

Plasmonic nanomaterials with strong absorption at near-infrared frequencies are promising photothermal therapy agents (PTAs). The pursuit of high photothermal conversion efficiency has been the central focus of this research field. Here, we report the development of plasmonic nanoparticle clusters (PNCs) as highly efficient PTAs and provide a semiquantitative approach for calculating their resonant frequency and absorption efficiency by combining the effective medium approximation (EMA) theory and full-wave electrodynamic simulations. Guided by the theoretical prediction, we further develop a universal strategy of space-confined seeded growth to prepare various PNCs. Under optimized growth conditions, we achieve a record photothermal conversion efficiency of up to ∼84% for gold-based PNCs, which is attributed to the collective plasmon-coupling-induced near-unity absorption efficiency. We further demonstrate the extraordinary photothermal therapy performance of the optimized PNCs in in vivo application. Our work demonstrates the high feasibility and efficacy of PNCs as nanoscale PTAs.

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