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Achieving control over the motion of dissolved particles in liquid metals isof importance for the meticulous realization of hierarchical particleassemblies in a variety of nanofabrication processes. Brownian forces canimpede the motion of such particles, impacting the degree of perfection thatcan be realized in assembled structures. Here we show that light inducedMarangoni flow in liquid metals (i.e., liquid-gallium) with Laguerre-gaussian(LG) lasers as heating sources, is an effective approach to overcome Brownianforces on particles, giving rise to predictable assemblies with high degree oforder. We show that by carefully engineering surface tension gradients inliquid-gallium using non-gaussian LG lasers, the Marangoni and convective flowthat develops in the fluid drives the trajectory of randomly dispersedparticles to assemble into 100 um wide ring-shaped particle assemblies. Carefulcontrol over the parameters of the LG laser (i.e., laser mode, spot size, andintensity of the electric field) can tune the temperature and fluid dynamics ofthe liquid-gallium as well as the balance of forces on the particle. This inturn can tune the structure of the ring-shaped particle assembly with a highdegree of fidelity. The use of light to control the motion of particles inliquid metals represents a tunable and rapidly reconfigurable approach tospatially design surface tension gradients in fluids for more complex assemblyof particles and small-scale solutes. This work can be extended to a variety ofliquid-metals, complementary to what has been realized in particle assembly outof ferrofluids using magnetic fields.

Light Induced Surface Tension Gradients for Hierarchical Assembly of Particles from Liquid Metals