A simple scheme is presented for remotely maneuvering individual microscopic swimmers by means of ondemand photo-induced actuation, where a laser gently and intermittently pushed the swimmer along its body axis (photon nudging) through a combination of radiation-pressure force and photophoretic pull.The proposed strategy utilized rotational random walks to reorient the micro-swimmer and turned on its propulsion only when the swimmer was aligned with the target location (adaptive control). A Langevin-type equation of motion was formulated, integrating these two ideas to describe the dynamics of the stochastically controlled swimmer. The strategy was examined using computer simulations and illustrated in a proof-of-principle experiment steering a gold-coated Janus micro-sphere moving in three dimensions. The physical parameters relevant to the two actuating forces under the experimental conditions were investigated theoretically and experimentally, revealing that a $7 K temperature differential on the micro-swimmer surface could generate a propelling photophoretic strength of $0.1 pN. The controllability and positioning error were discussed using both experimental data and Langevin dynamics simulations, where the latter was further used to identify two key unitless control parameters for manipulation accuracy and efficiency; they were the number of random-walk turns the swimmer experienced on the experimental timescale (the revolution number) and the photonnudge distance within the rotational diffusion time (the propulsion number). A comparison of simulation and experiment indicated that a near-optimal micron-precision motion control was achieved.
Single-particle tracking experiments have been used widely to study the heterogeneity of a sample. Segments with dissimilar diffusive behaviors are associated with different intermediate states, usually by visual inspection of the tracking trace. A likelihood-based, systematic approach is presented to remove this incertitude. Maximum likelihood estimators are derived for the determination of diffusion coefficients. A likelihood ratio test is applied to the localization of the changes in them. Simulations suggest that the proposed procedure is statistically robust and is able to quantitatively recover time-dependent changes in diffusion coefficients even in the presence of large measurement noise.
Confocal optical microscopes offer unparalleled high sensitivity and three-dimensional (3D) imaging capability but require slow point-by-point scanning; they are inefficient for imaging moving objects. We propose a more efficient solution. Instead of indiscriminate scanning, we let the focus of the microscope pursue the object of interest such that no time is wasted on uninformative background, allowing us to visualize 3D trajectories of fluorescent nanoparticles in solution with millisecond temporal and ~200 nm spatial resolution.
We report the first application of three-dimensional (3D) single-particle tracking (SPT) to hydrodynamic size characterization of gold nanoparticles in water. Nanoparticles undergoing Brownian motion were dynamically locked at the focal point of a microscope objective, one at a time, by rapid counteractive movements of the sample container. The hydrodynamic radius was derived from the recorded trajectory of each individual nanoparticle. The directly measured size and size distribution using 3D-SPT were in agreement with those obtained using the conventional dynamic light scattering (DLS) and using transmission electron microscopy (TEM), respectively.
Metallic nanoparticles synthesized by solution-phase chemistry usually exhibit various polygonal morphologies. The shape is known to have a great impact on a nanoparticle's optical properties, for instance, the surface plasmon resonance frequency. It remains unclear, however, whether the scattering spectrum of nanoparticles is generally anisotropic in the far field as a result. This simple question turns out to be extremely challenging to address because of the particle-to-particle shape inhomogeneity in a bulk sample, and the high sensitivity of surface plasmon resonance to local environments. We report the observation of scattering angle-dependent spectra using a newly developed single-particle tracking spectroscopy (SPS). Furthermore, we show that SPS has provided a way to directly visualize the rotational random walk of individual gold nanoparticles in water for the first time.
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