In the past few decades, superparamagnetic
nanoparticles (SPMNPs)
have attracted increasing attention in a wide range of magnetic theranostics
including magnetic biosensors, drug delivery, magnetic separation,
magnetic imaging, hyperthermia therapy, and so on. Superparamagnetic
iron oxide nanoparticles are currently widely used for these purposes
despite their low saturation magnetizations (below 80 emu/g). In pursuit
of higher magnetic signals (spatial resolutions) for magnetic imaging,
higher sensitivity (limit of detection) for biosensing, higher efficiency,
and lower dosage in drug delivery and hyperthermia therapy, magnetic
compounds and alloys that generally have higher saturation magnetizations
are of interest. FeCo SPMNPs are considered promising candidates for
biomedical applications due to their good corrosion resistance, stability,
and high saturation magnetizations (over 220 emu/g). However, the
critical size for FeCo nanoparticles to be superparamagnetic is limited
by a theoretical value of ∼15 nm, making it difficult to further
increase the magnetic moment per SPMNP. Herein, we report a method
to synthesize large single-crystalline FeCo nanoparticle complexes
(NPCs) with an overall size of ∼100 nm while retaining the
superparamagnetic properties. These large FeCo NPCs are synthesized
by self-assembling 3 nm FeCo nanoparticle units through a DC sputtering-based
gas-phase condensation (GPC) method. By controlling the sputtering
parameters like sputtering current density, sputtering pressure, and
carrying gas velocity in the GPC system, the nucleation and growth
of FeCo nanoparticles can be tuned, and different sizes of nanoparticles
can be obtained. The large FeCo NPCs are formed from the second crystallization
of small FeCo nanoparticle units with well-aligned crystalline axes,
which show both high saturation magnetization and superparamagnetic
properties suitable for biomedical applications. It is expected that
with the superparamagnetic behavior and higher magnetic moment per
FeCo NPC, they can potentially bring higher sensitivities to magnetic
biosensors that rely on the magnetic labels, higher efficiency in
hyperthermia therapy, and lower dose requirements for magnetic imaging
and separation.