Multimodality imaging based on complementary detection principles has broad clinical applications and promises to improve the accuracy of medical diagnosis. This means that a tracer particle advantageously incorporates multiple functionalities into a single delivery vehicle. In the present work, we explore a unique combination of MRI and photoacoustic tomography (PAT) to detect picomolar concentrations of nanoparticles. The nanoconstruct consists of ferromagnetic (Co) particles coated with gold (Au) for biocompatibility and a unique shape that enables optical absorption over a broad range of frequencies. The end result is a dual-modality probe useful for the detection of trace amounts of nanoparticles in biological tissues, in which MRI provides volume detection, whereas PAT performs edge detection.dual-modality imaging ͉ ferromagnetic nanoparticle ͉ molecular imaging ͉ MRI contrast ͉ photoacoustic tomography W e have synthesized nanoparticles for dual-modality (1-7)MRI and photoacoustic tomography (PAT). The incorporation of MRI and PAT into a single probe offers the unique possibility of combining the complementary strategies of contrastbased volume imaging and edge detection. Our nanoconstruct consists of zero-valence ferromagnetic cobalt (Co) particles (8) with a gold (Au) coating for biocompatibility and a unique shape rendering increased optical absorption over a broad range of frequencies (9)(10)(11)(12)(13)(14)(15)(16)(17)(18)(19). This research theme follows the rapid developments in nanotechnology, diagnostic radiology, and targeted molecular imaging (20), whereby nanoparticulate contrast agents, with the desirable properties of high chemical specificity, biocompatibility, and a reasonable half-life, are administered within a specific region of interest. In nanoparticle-based imaging studies, higher particle concentrations lead to better signal-to-noise contrasts, but this also poses a tradeoff with the toxicity. Therefore, one of the most important parameters when developing particle-based contrast is the safest and lowest nanoparticle concentration that offers sufficient contrast sensitivity.In MRI, magnetic materials such as gadolinium chelates and magnetic nanoparticles are often used (21-23) to enhance image contrast. The magnetic nanoparticles are passivated by biocompatible coatings such as dextrin, citrate, polystyrene/divinylbenzene, and elemental gold. These coatings also detoxify the particles, resulting in enhanced lifetimes in vivo. Typical examples of magnetic nanoparticulate core-shell configurations include magnetitedextrin, magnetite-silica (24) and iron-gold (25).Laser-based PAT (9-19) is a hybrid imaging modality [see supporting information (SI) Fig. S1]. It uses a pulsed laser source to illuminate a biological sample. Light absorption by the tissue results in a transient temperature rise on the order of 10 mK. The rapid thermoelastic expansion excites ultrasonic waves that are measured by using broadband ultrasonic transducers conformally arranged around the sample. Finally, a modif...