The Scherer Group Experimental Plasmonics and Biophysics

Web Name: The Scherer Group Experimental Plasmonics and Biophysics

WebSite: http://schererlab.uchicago.edu

ID:143109

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Group,Scherer,The,

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UNDER CONSTRUCTIONVISIT OUR PAGE WITH A DESKTOP WEB BROWSER FOR THE BEST VIEWING EXPERIENCE. MOBILE CAPABILITIES WILL BE OPTIMIZED SOON. STAY TUNED! The Scherer lab utilizes microscopy and simulation techniques to understand non-equilibrium dynamics in a range of chemical and biological systems. we strive to formulate physical interpretations of exotic phenomena through novel image analysis, simulation, and theory. Some of this is done in-house and other aspects are in collaboration with colleagues at uchicago, argonne, and northwestern. we encourage you to read more about our research. Research Reactive optical matter: light-induced motility in electrodynamically asymmetric nano-scale scatterers Light: Science Applications, 7 (105), 2018    From Newton’s third law, which is known as the principle of actio et reactio, we expect the forces between interacting particles to be equal and opposite for closed systems. Otherwise, “nonreciprocal” forces can arise. This has been shown theoretically in the interaction between dissimilar optically trapped particles that are mediated by an external field.  As a result, despite the incident external field not having a transverse component of momentum, the particle pair experiences a force in a direction that is transverse to the light propagation direction. In this letter, we directly measure the net nonreciprocal forces in electrodynamically interacting asymmetric nanoparticle dimers and nanoparticle structures that are illuminated by plane waves and confined to pseudo one-dimensional geometries. We show via electrodynamic theory and simulations that interparticle interactions cause asymmetric scattering from heterodimers. Therefore, the putative nonreciprocal forces are actually a consequence of momentum conservation. Our study demonstrates that asymmetric scatterers exhibit directed motion due to the breakdown of mirror symmetry in their electrodynamic interactions with external fields. Direct visualization of barrier crossing dynamics in a driven optical matter system ACS Nano, 12 (6), 2018    A major impediment to a more complete understanding of barrier crossing and other single-molecule processes is the inability to directly visualize the trajectories and dynamics of atoms and molecules in reactions. Rather, the kinetics are inferred from ensemble measurements or the position of a transducer (e.g., an AFM cantilever) as a surrogate variable. Direct visualization is highly desirable. Here, we achieve the direct measurement of barrier crossing trajectories by using optical microscopy to observe position and orientation changes of pairs of Ag nanoparticles, i.e. passing events, in an optical ring trap. A two-step mechanism similar to a bimolecular exchange reaction or the Michaelis–Menten scheme is revealed by analysis that combines detailed knowledge of each trajectory, a statistically significant number of repetitions of the passing events, and the driving force dependence of the process. We find that while the total event rate increases with driving force, this increase is due to an increase in the rate of encounters. There is no drive force dependence on the rate of barrier crossing because the key motion for the process involves a random (thermal) radial fluctuation of one particle allowing the other to pass. This simple experiment can readily be extended to study more complex barrier crossing processes by replacing the spherical metal nanoparticles with anisotropic ones or by creating more intricate optical trapping potentials. Potential energy surfaces and reaction pathways for light-mediated self-organization of metal nanoparticle clusters Nature Communications, 5 (3751), 2014    Potential energy surfaces are the central concept in understanding the assembly of molecules; atoms form molecules via covalent bonds with structures defined by the stationary points of the surfaces. Similarly, dispersion interactions give Lennard-Jones potentials that describe atomic clusters and liquids. The formation of molecules and clusters can follow various pathways depending on the initial conditions and the potentials. Here we show that analogous mechanistic effects occur in light-mediated self-organization of metal nanoparticles; atoms are replaced by silver nanoparticles that are arranged by electrodynamic (that is, optical trapping and optical binding) interactions. We demonstrate this concept using simple Gaussian optical fields and the formation of stable clusters with various two-dimensional (2D) and three-dimensional (3D) geometries. The formation of specific clusters is ‘path-dependent’; the particle motions follow an electrodynamic potential energy surface. This work paves the way for rational design of photonic clusters with combinations of imposed beam shapes, gradients and optical binding interactions. Three-dimensional optical trapping and orientation of microparticles for coherent X-ray diffraction imaging Proceedings of the National Academy of Sciences, 116 (10), 2019    Obtaining a fundamental understanding of crystal growth and chemical reactions in solution is of broad and enduring interest for materials discovery, structural biology, and catalysis. The recent availability of bright, coherent X-ray sources can enable these fluctuation-driven processes to be monitored in situ through the technique of coherent X-ray diffractive imaging (CXDI), in which the 3D internal structure of microscopic objects is determined with nanometer resolution from the fine structure of diffraction peaks. So far, Bragg CXDI has required immobilization of particles on a substrate, which modifies their structure and chemical activity. Here, we demonstrate Bragg CXDI on a single particle that is trapped and oriented in solution using optical tweezers and thus obtain its 3D structure and strain map. Dark Plasmon Modes in Symmetric Gold Nanoparticle Dimers Illuminated by Focused Cylindrical Vector Beams Journal of Physical Chemistry C, 122 (48), 2018    The plasmon hybridization model of electromagnetic coupling between plasmonic nanoparticles predicts the formation of lower energy “bonding” and higher energy “antibonding” modes in analogy with the quantum mechanical description of chemical bonding. For a symmetric metallic nanoparticle dimer excited by linearly polarized light, the hybridization picture predicts that in-phase coupling of the dipole moments is optically allowed, creating bright “modes”, whereas the out-of-phase coupling is dark due to the cancellation of the oppositely oriented dipole moments (in the quasistatic approximation). These bright modes are electric dipolar in nature and readily couple to scalar (i.e., linearly or circularly polarized) beams of light. We show that focused cylindrical vector beams, specifically azimuthally and radially polarized beams, directly excite dark plasmon modes in symmetric gold nanoparticle (AuNP) dimers at normal incidence. We use single-particle spectroscopy and electrodynamics simulations to study the resonance scattering of AuNP dimers illuminated by azimuthally and radially polarized light. The electric field distributions of the focused azimuthal or radial beams are locally polarized perpendicular or parallel to the AuNP dimer axis, but with opposite directions at each particle. Therefore, the associated combinations of single-particle dipole moments are out-of-phase, and the excitation (resonance) is of so-called “dark modes”. In addition, multipole expansion of the fields associated with each scattering spectrum shows that the vector beam excitation involves driving multipolar, e.g., magnetic dipolar and electric quadrupolar, modes, and that they even dominate the scattering spectra (vs electric dipole). This work opens new opportunities for investigating dark plasmon modes in nanostructures, which are difficult to selectively excite by conventional polarized light. Selective Induction of Optical Magnetism Nano Letters, 122 (48), 2018    An extension of the Maxwell–Faraday law of electromagnetic induction to optical frequencies requires spatially appropriate materials and optical beams to create resonances and excitations with curl. Here we employ cylindrical vector beams with azimuthal polarization to create electric fields that selectively drive magnetic responses in dielectric core–metal nanoparticle “satellite” nanostructures. These optical frequency magnetic resonances are induced in materials that do not possess spin or orbital angular momentum. Multipole expansion analysis of the scattered fields obtained from electrodynamics simulations show that the excitation with azimuthally polarized beams selectively enhances magnetic vs electric dipole resonances by nearly 100-fold in experiments. Multipolar resonances (e.g., quadrupole and octupole) are enhanced 5-fold by focused azimuthally versus linearly polarized beams. We also selectively excite electric multipolar resonances in the same identical nanostructures with radially polarized light. This work opens new opportunities for spectroscopic investigation and control of “dark modes”, Fano resonances, and magnetic modes in nanomaterials and engineered metamaterials. Particle tracking by repetitive phase-shift interferometric super resolution microscopy Optics Letters, 43 (12), 2018    Accurate and rapid particle tracking is essential for addressing many research problems in single molecule and cellular biophysics and colloidal soft condensed matter physics. We developed a novel three-dimensional interferometric fluorescent particle tracking approach that does not require any sample scanning. By periodically shifting the interferometer phase, the information stored in the interference pattern of the emitted light allows localizing particles positions with nanometer resolution. This tracking protocol was demonstrated by measuring a known trajectory of a fluorescent bead with sub-5 nm axial localization error at 5 Hz. The interferometric microscopy was used to track the RecA protein in Bacillus subtilis bacteria to demonstrate its compatibility with biological systems. Snapshot 3D tracking of insulin granules in live cells Proceedings of SPIE, 10499, 2018    Rapid and accurate volumetric imaging remains a challenge, yet has the potential to enhance understanding of cell function. We developed and used a multifocal microscope (MFM) for 3D snapshot imaging to allow 3D tracking of insulin granules labeled with mCherry in MIN6 cells. MFM employs a special diffractive optical element (DOE) to simultaneously image multiple focal planes. This simultaneous acquisition of information determines the 3D location of single objects at a speed only limited by the array detector’s frame rate. We validated the accuracy of MFM imaging/tracking with fluorescence beads; the 3D positions and trajectories of single fluorescence beads can be determined accurately over a wide range of spatial and temporal scales. The 3D positions and trajectories of single insulin granules in a 3.2um deep volume were determined with imaging processing that combines 3D decovolution, shift correction, and finally tracking using the Imaris software package. We find that the motion of the granules is superdiffusive, but less so in 3D than 2D for cells grown on coverslip surfaces, suggesting an anisotropy in the cytoskeleton (e.g. microtubules and action). Intracellular insulin transport is a subordinated random walk Proceedings of the National Academy of Sciences, 110 (13), 2013    We quantitatively analyzed particle tracking data on insulin granules expressing fluorescent fusion proteins in MIN6 cells to better understand the motions contributing to intracellular transport and, more generally, the means for characterizing systems far from equilibrium. Care was taken to ensure that the statistics reflected intrinsic features of the individual granules rather than details of the measurement and overall cell state. We find anomalous diffusion. Interpreting such data conventionally requires assuming that a process is either ergodic with particles working against fluctuating obstacles (fractional Brownian motion) or nonergodic with a broad distribution of dwell times for traps (continuous-time random walk). However, we find that statistical tests based on these two models give conflicting results. We resolve this issue by introducing a subordinated scheme in which particles in cages with random dwell times undergo correlated motions owing to interactions with a fluctuating environment. We relate this picture to the underlying microtubule structure by imaging in the presence of vinblastine. Our results provide a simple physical picture for how diverse pools of insulin granules and, in turn, biphasic secretion could arise.

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