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Pulsed laser-induced dewetting (PLiD) of Ag 0.5 Ni 0.5 thin films results in phase-separated bimetallic nanoparticles with size distributions that depend on the initial thin film thickness. Co-sputtering of Ag and Ni is used to generate the as-deposited (AD) nanogranular supersaturated thin films. The magnetic and optical properties of the AD thin films and PLiD nanoparticles are characterized using a vibrating sample magnetometer, optical absorption spectroscopy, and electron energy loss spectroscopy (EELS). Magnetic measurements demonstrate that Ag 0.5 Ni 0.5 nanoparticles are ferromagnetic at room temperature when the nanoparticle diameters are &gt;20 nm and superparamagnetic &lt;20 nm. Optical measurements show that all nanoparticle size distributions possess a local surface plasmon resonance (LSPR) peak that red-shifts with increasing diameter. Following PLiD, a Janus nanoparticle morphology is observed in scanning transmission electron microscopy, and low-loss EELS reveals size-dependent Ag and Ni LSPR dipole modes, while higher order modes appear only in the Ag hemisphere. PLiD of Ag-Ni thin films is shown to be a viable technique to generate bimetallic nanoparticles with both magnetic and plasmonic functionality.

Optical and Magnetic Properties of Ag–Ni Bimetallic Nanoparticles Assembled via Pulsed Laser-Induced Dewetting