Unveiling Dipolar Interaction‐Driven Magnetic Field Inhomogeneities in T ₂ MRI Contrast Agents

Abstract Modulating local magnetic field inhomogeneities, combined with ultra‐high‐field MRI (UHF‐MRI) is a promising strategy to enhance the performance of next‐generation T ₂ contrast agents (CAs). Although dipolar interactions likely contribute to contrast enhancement, their role in magnetic inhomogeneities and proton dephasing remains poorly understood, limiting further optimization. In this study, the fundamental role of dipolar interactions on the modulation of the transverse relaxivity (r ₂ ) of iron oxide‐based CAs is demonstrated by shaping local magnetic field inhomogeneities. A nanoscale‐distance‐tuned model system is developed by coating superparamagnetic iron oxide nanoprobes with silica shells of increasing thickness, thereby modulating the intensity of the dipolar interactions. An exponential dependence of r ₂ on dipolar interaction strength is observed, with a sharp initial increase followed by a plateau as interactions reached their effective range, resulting in up to a sevenfold enhancement compared to interaction‐free CAs. Furthermore, the dependence of r ₂ on B ₀ is evaluated across conventional field‐MRI (1.4 and 3.0 T) to UHF‐MRI (7.0 and 11.7 T), in both interacting and non‐interacting CA systems, revealing a nonlinear behavior. These findings establish dipolar interaction control as a key parameter for optimizing T ₂ ‐CAs performance, advancing the design of next‐generation MRI nanoprobes for diagnostic applications.