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Geometrically confined magnetic particles due to their unique response toexternal magnetic fields find a variety of applications, including magneticguidance, heat and drug delivery, magneto-mechanical actuation, and contrastenhancement. Highly sensitive detection and imaging techniques based onnonlinear properties of nanomagnets were recently proposed as innovativestrong-translational potential methods applicable in complex, often opaque,biological systems. Here we report on significant enhancement of the detectioncapability using optical-lithography-defined, ferromagnetic iron-nickel alloydisk-shaped particles. We show that an irreversible transition between astrongly non-collinear (vortex) and single domain states, driven by analternating magnetic field translates into a nonlinear magnetic response thatenables ultrasensitive detection of these particles. The record sensitivity of~ 3.5x10-9 emu, which is equivalent to ~39 pg of magnetic material isdemonstrated at room temperature for arrays of patterned disks. We also showthat unbound disks re-suspended in aqueous buffer can be successfully detectedand quantified in real-time when administrated into a live animal allowing fortracing their biodistribution. Use of nanoscale ferromagnetic particles withengineered nonlinear properties opens prospects for further enhancingsensitivity, scalability and tunability of noise-free magnetic tag detection inhigh-background environments for various applications spanning from biosensingand medical imaging to anti-counterfeiting technologies.

Ultrasensitive Detection Enabled by Nonlinear Magnetization of Nanomagnetic Labels