The magnetic actuation of deposited drops has mainly relied on volume forces exerted on the liquid to be transported, which is poorly efficient with conventional diamagnetic liquids such as water and oil, unless magnetosensitive particles are added. Herein, we describe a new and additive‐free way to magnetically control the motion of discrete liquid entities. Our strategy consists of using a paramagnetic liquid as a deformable substrate to direct, using a magnet, the motion of various floating liquid entities, ranging from naked drops to liquid marbles. A broad variety of liquids, including diamagnetic (water, oil) and nonmagnetic ones, can be efficiently transported using the moderate magnetic field (ca. 50 mT) produced by a small permanent magnet. Complex trajectories can be achieved in a reliable manner and multiplexing potential is demonstrated through on‐demand drop fusion. Our paramagnetofluidic method advantageously works without any complex equipment or electric power, in phase with the necessary development of robust and low‐cost analytical and diagnostic fluidic devices.

Monolayers of soft colloidal particles confined at fluid interfaces are at the core of a broad range of technological processes, from the stabilization of responsive foams and emulsions to advanced lithographic techniques. However, establishing a fundamental relation between their internal architecture, which is controlled during synthesis, and their structural and mechanical properties upon interfacial confinement remains an elusive task. To address this open issue, which defines the monolayer’s properties, we synthesize core–shell microgels, whose soft core can be chemically degraded in a controlled fashion. This strategy allows us to obtain a series of particles ranging from analogues of standard batch-synthesized microgels to completely hollow ones after total core removal. Combined experimental and numerical results show that our hollow particles have a thin and deformable shell, leading to a temperature-responsive collapse of the internal cavity and a complete flattening after adsorption at a fluid interface. Mechanical characterization shows that a critical degree of core removal is required to obtain soft disk-like particles at an oil–water interface, which present a distinct response to compression. At low packing fractions, the mechanical response of the monolayer is dominated by the outer polymer chains forming a corona surrounding the particles within the interfacial plane, regardless of the presence of a core. By contrast, at high compression, the absence of a core enables the particles to deform in the direction orthogonal to the interface and to be continuously compressed without altering the monolayer structure. These findings show how fine, single-particle architectural control during synthesis can be engineered to determine the interfacial behavior of microgels, enabling one to link particle conformation with the resulting material properties.

The self-assembly of colloids at fluid interfaces is a well-studied research field both for gaining fundamental insights and for material fabrication. The fluid interface allows the confinement of particles in two dimensions and may act as a template for guiding their organization into soft and reconfigurable structures. Additives (e.g., surfactants, salts, and polymers) in the colloidal suspension are routinely used as a practical and effective tool to drive particle adsorption and tune their interfacial organization. However, some phenomena lying at the heart of the accumulation and self-assembly of particles at fluid interfaces remain poorly understood. This Feature Article aims to critically analyze the mechanisms involved in the adsorption and self-organization of micro- and nanoparticles at various fluid interfaces. In particular, we address the role of additives in both promoting the adsorption of particles from the bulk suspension to the fluid interface and in mediating the interactions between interfacial particles. We emphasize how different types of additives play a crucial role in controlling the interactions between suspended particles and the fluid interface as well as the interactions between adsorbed particles, thus dictating the final self-assembled structure. We also critically summarize the main experimental protocols developed for the complete adsorption of particles initially suspended in the bulk. Furthermore, we highlight some special properties (e.g., reconfigurability upon external stimulation and dissipative self-assembly) and the application potential of structures formed by colloid self-organization at fluid interfaces mediated/promoted by additives. We believe our contribution serves both as a practical roadmap to scientists coming from other fields and as a valuable information resource for all researchers interested in this exciting research field.

The reconfiguration of individual soft and deformable particles upon adsorption at a fluid interface underpins many aspects of their dynamics and interactions, ultimately regulating the properties of monolayers of relevance for applications. In this work, we demonstrate that atomic force microscopy can be used for the in situ reconstruction of the three-dimensional conformation of model poly( N -isopropylacrylamide) microgels adsorbed at an oil-water interface. We image the particle topography from both sides of the interface to characterize its in-plane deformation and to visualize the occurrence of asymmetric swelling in the two fluids. In addition, the technique enables investigating different fluid phases and particle architectures, as well as studying the effect of temperature variations on particle conformation in situ. We envisage that these results open up an exciting range of possibilities to provide microscopic insights into the single-particle behavior of soft objects at fluid interfaces and into the resulting macroscopic material properties.