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Anisotropic potentials in Janus colloids provide additional freedom to control particle aggregation into structures of different sizes and morphologies. In this work, we perform Brownian dynamics simulations of a dilute suspension of magnetic spherical Janus colloids with their magnetic dipole moments shifted radially towards the surface of the particle in order to gain valuable microstructural insight. Properties such as the mean cluster size, orientational ordering, and nucleation and growth are examined dynamically. Differences in the structure of clusters and in the aggregation process are observed depending on the dipolar shift ( s )—the ratio between the displacement of the dipole and the particle radius—and the dipolar coupling constant ( λ )—the ratio between the magnetic dipole–dipole and Brownian forces. Using these two dimensionless quantities, a structural “phase” diagram is constructed. Each phase corresponds to unique nucleation and growth behavior and orientational ordering of dipoles inside clusters. At small λ , the particles aggregate and disaggregate resulting in short-lived clusters at small s , while at high s the particles aggregate in permanent triplets (long-lived clusters). At high λ , the critical nuclei formed during the nucleation process are triplets and quadruplets with unique orientational ordering. These small clusters then serve as building blocks to form larger structures, such as single-chain, loop-like, island-like, worm-like, and antiparallel-double-chain clusters. This study shows that dipolar shifts in colloids can serve as a control parameter in applications where unique size, morphology, and aggregation kinetics of clusters are required. 

There is significant interest in the utility of asymmetric nanoaperture arrays as substrates for the surface-enhanced detection, fluorescence, and imaging of individual molecules. This work introduces obliquely-cut, out-of-plane, coaxial layered structures on an aperture edge. We refer to these structures as nanofingernails, which emphasizes their curved, oblique, and out-of-plane features. Broadband coupling into chiral hybrid plasmon modes and helicity-dependent near-field scattering without circular dichroism are demonstrated. The unusually-broadband, multipolar modes of nanofingernail micropore structures exhibit phase retardation effects that may be useful for achieving spatial overlap at different frequencies. The nanofingernail geometry shows new potential for simultaneous polarization-enhanced hyperspectral imaging on apertured, plasmonic surfaces. 

The self-assembly of colloidal magnetic Janus particles with a laterally displaced (or shifted), permanent dipole in a quasi-two-dimensional system is studied using Brownian dynamics simulations. The rate of formation of clusters and their structures are quantified for several values of dipolar shift from the particle center, which is nondimensionalized using the particle's radius so that it takes values ranging from 0 to 1, and examined under different magnetic interaction strengths relative to Brownian motion. For dipolar shifts close to 0, chain-like structures are formed, which grow at long times following a power law, while particles of shift higher than 0.2 generally aggregate in ring-like clusters that experience limited growth. In the case of shifts between 0.4 and 0.5, the particles tend to aggregate in clusters of 3 to 6, while for all shifts higher than 0.6 clusters rarely contain more than 3 particles due to the antiparallel dipole orientations that are most stable at those shifts. The strength of the magnetic interactions hastens the rate at which clusters are formed; however, the effect it has on cluster size is lessened by increases in the shift of the dipoles. These results contribute to better understand the dynamics of magnetic Janus particles and can help the synthesis of functionalized materials for specific applications such as drug delivery.