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Stefano Sacanna

Publications and source records attributed to Stefano Sacanna.

8 recordsLinked to original sources

Sampling Free Energy Landscapes of Ionic Colloidal Crystal Systems using Machine-Learned Proxy Collective Variables

Charged colloids coated with a polymer brush can be designed to preferentially self-assemble into different crystal structures by varying easy-to-tune experimental conditions. For a given set of conditions, we have observed in experiments and simulations a distribution of thermodynamically (meta)stable self-assembled crystal structures. Properly quantifying the free energy landscape of these colloidal systems is essential for rationally choosing conditions to preferentially target particular crystal structures. For some of the structures we have formed, standard crystalline order parameters are not able to differentiate between crystals or between crystals and amorphous aggregates. We show that local environment similarity descriptors are able to distinguish the relevant metastable states, but are too expensive for use in biased MD simulations. Here, we adopt an approach from machine-learned interaction potentials showing that SE(3)-equivariant transformer networks can serve as an efficient-to-evaluate machine-learned proxy. As a result, we can compute the relative free energies of accessible colloidal structures as a function of different experimentally-relevant physical knobs that can steer our system between two observed crystal types. As an example application, we then show how changing surface potentials of positive and negative colloids while maintaining the same attractive energy can shift which crystal structure is favored.

cond-mat.stat-mech

PACSim: A Flexible Simulation Framework for Polymer-Attenuated Coulombic Self-Assembly

Polymer-Attenuated Coulombic Self-Assembly (PACS) is a flexible experimental approach for generating crystals from simple colloidal building blocks. The central components are charged spherical particles coated with a polymer brush that prevents irreversible aggregation. Whether oppositely charged colloids crystallize, and which structures they form, depends on several factors, including colloid concentration, charge, and size, as well as the salt concentration of the solution. Molecular dynamics (MD) simulations are a powerful tool for predicting the outcomes of PACS assembly experiments and also provide particle-level insight into the assembly processes. Here, we present an open-source simulation framework, PACSim, that enables MD simulation studies of assembly by PACS across a range of experimentally relevant scenarios. PACSim is built on top of OpenMM, a flexible MD simulation framework that readily supports the implementation of different interaction potentials, as well as integration with other tools such as enhanced-sampling and machine-learning frameworks. We describe the motivation for PACSim, outline its features, report methodological advancements inspired by this framework, and provide examples of its use.

cond-mat.soft

The free surface of a colloidal chiral fluid: waves and instabilities from odd stress and Hall viscosity

In simple fluids, such as water, invariance under parity and time-reversal symmetry imposes that the rotation of constituent 'atoms' are determined by the flow and that viscous stresses damp motion. Activation of the rotational degrees of freedom of a fluid by spinning its atomic building blocks breaks these constraints and has thus been the subject of fundamental theoretical interest across classical and quantum fluids. However, the creation of a model liquid which isolates chiral hydrodynamic phenomena has remained experimentally elusive. Here we report the creation of a cohesive two-dimensional chiral liquid consisting of millions of spinning colloidal magnets and study its flows. We find that dissipative viscous edge pumping is a key and general mechanism of chiral hydrodynamics, driving uni-directional surface waves and instabilities, with no counterpart in conventional fluids. Spectral measurements of the chiral surface dynamics reveal the presence of Hall viscosity, an experimentally long sought property of chiral fluids. Precise measurements and comparison with theory demonstrate excellent agreement with a minimal but complete chiral hydrodynamic model, paving the way for the exploration of chiral hydrodynamics in experiment.

physics.flu-dyn

Targeted Assembly and Synchronization of Self-Spinning Microgears

Self-assembly is the autonomous organization of components into patterns or structures: an essential ingredient of biology and a desired route to complex organization. At equilibrium, the structure is encoded through specific interactions, at an unfavorable entropic cost for the system. An alternative approach, widely used by Nature, uses energy input to bypass the entropy bottleneck and develop features otherwise impossible at equilibrium. Dissipative building blocks that inject energy locally were made available by recent advance in colloidal science but have not been used to control self-assembly. Here we show the robust formation of self-powered rotors and dynamical superstructures from active particles and harness non-equilibrium phoretic phenomena to tailor interactions and direct self-assembly. We use a photoactive component that consumes fuel, hematite, to devise phototactic microswimmers that form self-spinning microgears following spatiotemporal light patterns. The gears are coupled via their chemical clouds and constitute the elementary bricks of synchronized superstructures, which autonomously regulate their dynamics. The results are quantitatively rationalized on the basis of a stochastic description of diffusio-phoretic oscillators dynamically coupled by chemical gradients to form directional interactions. Our findings demonstrate that non-equilibrium phenomena can be harnessed to shape interactions and program hierarchical constructions. It lays the groundwork for the self-assembly of dynamical architectures and synchronized micro-machinery.

cond-mat.soft

Unstable fronts and stable "critters" formed by microrollers

Condensation of objects into stable clusters occurs naturally in equilibrium and driven systems. It is commonly held that potential interactions, depletion forces, or sensing are the only mechanisms which can create long-lived compact structures. Here we show that persistent motile structures can form spontaneously from hydrodynamic interactions alone with no sensing or potential interactions. We study this structure formation in a system of colloidal rollers suspended and translating above a floor, using both experiments and large-scale 3D simulations. In this system, clusters originate from a previously unreported fingering instability, where fingers pinch off from an unstable front to form autonomous "critters", whose size is selected by the height of the particles above the floor. These critters are a stable state of the system, move much faster than individual particles, and quickly respond to a changing drive. With speed and direction set by a rotating magnetic field, these active structures offer interesting possibilities for guided transport, flow generation, and mixing at the microscale.

cond-mat.soft

Trochoidal trajectories of self-propelled Janus particles in a diverging laser beam

We describe colloidal Janus particles with metallic and dielectric faces that swim vigorously when illuminated by defocused optical tweezers without consuming any chemical fuel. Rather than wandering randomly, these optically-activated colloidal swimmers circulate back and forth through the beam of light, tracing out sinuous rosette patterns. We propose a model for this mode of light-activated transport that accounts for the observed behavior through a combination of self-thermophoresis and optically-induced torque. In the deterministic limit, this model yields trajectories that resemble rosette curves known as hypotrochoids.

cond-mat.soft

Artificial Rheotaxis

Motility is a basic feature of living microorganisms, and how it works is often determined by environmental cues. Recent efforts have focused on develop- ing artificial systems that can mimic microorganisms, and in particular their self-propulsion. Here, we report on the design and characterization of syn- thetic self-propelled particles that migrate upstream, known as positive rheo- taxis. This phenomenon results from a purely physical mechanism involving the interplay between the polarity of the particles and their alignment by a viscous torque. We show quantitative agreement between experimental data and a simple model of an overdamped Brownian pendulum. The model no- tably predicts the existence of a stagnation point in a diverging flow. We take advantage of this property to demonstrate that our active particles can sense and predictably organize in an imposed flow. Our colloidal system represents an important step towards the realization of biomimetic micro-systems withthe ability to sense and respond to environmental changes

cond-mat.soft

Characterization of anisotropic nano-particles by using depolarized dynamic light scattering in the near field

Light scattering techniques are widely used in many fields of condensed and sof t matter physics. Usually these methods are based on the study of the scattered light in the far field. Recently, a new family of near field detection schemes has been developed, mainly for the study of small angle light scattering. These techniques are based on the detection of the light intensity near to the sample, where light scattered at different directions overlaps but can be distinguished by Fourier transform analysis. Here we report for the first time data obtained with a dynamic near field scattering instrument, measuring both polarized and depolarized scattered light. Advantages of this procedure over the traditional far field detection include the immunity to stray light problems and the possibility to obtain a large number of statistical samples for many different wave vectors in a single instantaneous measurement. By using the proposed technique we have measured the translational and rotational diffusion coefficients of rod-like colloidal particles. The obtained data are in very good agreement with the data acquired with a traditional light scattering apparatus.

physics.optics