title: Driven optical matter: Dynamics of electrodynamically coupled nanoparticles in an optical ring vortex.
abstract: To date investigations of the dynamics of driven colloidal systems have focused on hydrodynamic interactions and often employ optical (laser) tweezers for manipulation. However, the optical fields that provide confinement and drive also result in electrodynamic interactions that are generally neglected. We address this issue with a detailed study of interparticle dynamics in an optical ring vortex trap using 150-nm diameter Ag nanoparticles. We term the resultant electrodynamically interacting nanoparticles a driven optical matter system. We also show that a superior trap is created by using a Au nanoplate mirror in a retroreflection geometry, which increases the electric field intensity, the optical drive force, and spatial confinement. Using nanoparticles versus micron sized colloids significantly reduces the surface hydrodynamic friction allowing us to access small values of optical topological charge and drive force. We quantify a further 50% reduction of hydrodynamic friction when the nanoparticles are driven over the Au nanoplate mirrors versus over a mildly electrostatically repulsive glass surface. Further, we demonstrate through experiments and electrodynamics-Langevin dynamics simulations that the optical drive force and the interparticle interactions are not constant around the ring for linearly polarized light, resulting in a strong position-dependent variation in the nanoparticle velocity. The nonuniformity in the optical drive force is also manifest as an increase in fluctuations of interparticle separation, or effective temperature, as the optical driving force is increased. Finally, we resolve an open issue in the literature on periodic modulation of interparticle separation with comparative measurements of driven 300-nm-diameter polystyrene beads that also clearly reveal the significance of electrodynamic forces and interactions in optically driven colloidal systems. Therefore, the modulations in the optical forces and electrodynamic interactions that we demonstrate should not be neglected for dielectric particles and might give rise to some structural and dynamic features that have previously been attributed exclusively to hydrodynamic interactions.
authors.affiliation: Department of Chemistry, The University of Chicago, Chicago, Illinois 60637, USA.
authors.forename: Patrick
authors.initials: P
authors.lastname: Figliozzi
authors.affiliation: James Franck Institute, The University of Chicago, Chicago, Illinois 60637, USA.
authors.forename: Nishant
authors.initials: N
authors.lastname: Sule
authors.affiliation: James Franck Institute, The University of Chicago, Chicago, Illinois 60637, USA.
authors.forename: Zijie
authors.initials: Z
authors.lastname: Yan
authors.affiliation: James Franck Institute, The University of Chicago, Chicago, Illinois 60637, USA.
authors.forename: Ying
authors.initials: Y
authors.lastname: Bao
authors.affiliation: James Franck Institute, The University of Chicago, Chicago, Illinois 60637, USA.
authors.forename: Stanislav
authors.initials: S
authors.lastname: Burov
authors.affiliation: Center for Nanoscale Materials, Argonne National Laboratory, Lemont, Illinois 60439, USA.
authors.forename: Stephen K
authors.initials: SK
authors.lastname: Gray
authors.affiliation: Department of Chemistry, The University of Chicago, Chicago, Illinois 60637, USA.|James Franck Institute, The University of Chicago, Chicago, Illinois 60637, USA.
authors.forename: Stuart A
authors.initials: SA
authors.lastname: Rice
authors.affiliation: Department of Chemistry, The University of Chicago, Chicago, Illinois 60637, USA.|James Franck Institute, The University of Chicago, Chicago, Illinois 60637, USA.
authors.forename: Suriyanarayanan
authors.initials: S
authors.lastname: Vaikuntanathan
authors.affiliation: Department of Chemistry, The University of Chicago, Chicago, Illinois 60637, USA.|James Franck Institute, The University of Chicago, Chicago, Illinois 60637, USA.
authors.forename: Norbert F
authors.initials: NF
authors.lastname: Scherer