<p>The study of active colloidal microswimmers with
tunable phoretic and self-organizational behaviors is important for understanding
out-of-equilibrium systems and the design of functional, adaptive matter. Solubilizing,
self-propelling droplets have emerged as a rich chemical platform for
exploration of active behaviors, but isotropic droplets rely on spontaneous
symmetry breaking to sustain motion. The introduction of permanent asymmetry,
e.g. in the form of a biphasic Janus droplet, has not been explored previously
as a comprehensive design strategy for active droplets, despite the widespread
use of Janus structures in motile solid particles. Here, we uncover the
chemomechanical framework underlying the self-propulsion of active, biphasic
Janus oil droplets solubilizing in aqueous surfactant. We elucidate how droplet
propulsion is influenced by the degree of oil mixing, droplet shape, and oil
solubilization rates for a range of oil combinations. A key finding is that for
droplets containing both a mobile (solubilizing) and non-mobile oil, the degree
of partitioning of the mobile oil across the Janus droplets’ oil-oil interface plays
a pivotal role in determining the droplet speed and swimming direction. As a
result, we observe propulsion speeds of Janus droplets more than an
order-of-magnitude faster than chasing pairs of single emulsion droplets which
lack an oil-oil interface. In addition, spatiotemporal control over droplet
swimming speed and orientation is demonstrated through the application of local
thermal gradients applied via induced via joule heading and laser spot
illumination. We also explore the interactions between collections of Janus droplets
including the spontaneous formation of multi-droplet spinning clusters that
rotate predictably based on symmetry. Our findings provide key insights as to
how the chemistry and structure of multiphase fluids can be harnessed to design
microswimmers with programmable active and collective behaviors.</p><br>