Thermophoretic trap for single amyloid fibril and protein aggregation studies.

The study of the aggregation of soluble proteins into highly ordered, insoluble amyloid fibrils is fundamental for the understanding of neurodegenerative disorders. Here, we present a method for the observation of single amyloid fibrils that allows the investigation of fibril growth, secondary nucleation or fibril breakup that is typically hidden in the average ensemble. Our approach of thermophoretic trapping and rotational diffusion measurements is demonstrated for single Aß40, Aß42 and pyroglutamyl-modified amyloid-ß variant (pGlu3-Aß3-40) amyloid fibrils.

Applications and challenges of thermoplasmonics.

Over the past two decades, there has been a growing interest in the use of plasmonic nanoparticles as sources of heat remotely controlled by light, giving rise to the field of thermoplasmonics. The ability to release heat on the nanoscale has already impacted a broad range of research activities, from biomedicine to imaging and catalysis. Thermoplasmonics is now entering an important phase: some applications have engaged in an industrial stage, while others, originally full of promise, experience some difficulty in reaching their potential. Meanwhile, innovative fundamental areas of research are being developed. In this Review, we scrutinize the current research landscape in thermoplasmonics, with a specific focus on its applications and main challenges in many different fields of science, including nanomedicine, cell biology, photothermal and hot-electron chemistry, solar light harvesting, soft matter and nanofluidics.

How Activity Landscapes Polarize Microswimmers without Alignment Forces.

Active-particle suspensions exhibit distinct polarization-density patterns in activity landscapes, even without anisotropic particle interactions. Such polarization without alignment forces is at work in motility-induced phase separation and betrays intrinsic microscopic activity to mesoscale observers. Using stable long-term confinement of a single thermophoretic microswimmer in a dedicated force-free particle trap, we examine the polarized interfacial layer at a motility step and confirm that it does not exert pressure onto the bulk. Our observations are quantitatively explained by an analytical theory that can also guide the analysis of more complex geometries and many-body effects.

Finite-Size Scaling at the Edge of Disorder in a Time-Delay Vicsek Model.

Living many-body systems often exhibit scale-free collective behavior reminiscent of thermal critical phenomena. But their mutual interactions are inevitably retarded due to information processing and delayed actuation. We numerically investigate the consequences for the finite-size scaling in the Vicsek model of motile active matter. A growing delay time initially facilitates but ultimately impedes collective ordering and turns the dynamical scaling from diffusive to ballistic. It provides an alternative explanation of swarm traits previously attributed to inertia.

Thermotaxis of Janus particles.

The interactions of autonomous microswimmers play an important role for the formation of collective states of motile active matter. We study them in detail for the common microswimmer-design of two-faced Janus spheres with hemispheres made from different materials. Their chemical and physical surface properties may be tailored to fine-tune their mutual attractive, repulsive or aligning behavior. To investigate these effects systematically, we monitor the dynamics of a single gold-capped Janus particle in the external temperature field created by an optically heated metal nanoparticle. We quantify the orientation-dependent repulsion and alignment of the Janus particle and explain it in terms of a simple theoretical model for the induced thermoosmotic surface fluxes. The model reveals that the particle's angular velocity is solely determined by the temperature profile on the equator between the Janus particle's hemispheres and their phoretic mobility contrast. The distortion of the external temperature field by their heterogeneous heat conductivity is moreover shown to break the apparent symmetry of the problem.

Self-Propulsion of Janus Particles near a Brush-Functionalized Substrate.

Thermophoresis is a common mechanism that can drive autonomous motion of Janus particles under the right environment. Despite recent efforts to investigate the mechanism underlying the self-propulsion of thermophoretic particles, the interaction of particles with the substrate underneath the particle has remained unclear. In this work, we explore the impact of poly(N-isopropylacrylamide) (PNIPAM)-functionalized substrate with various chain lengths on the active motion of a single polystyrene particle half-coated with gold (Au-PS). We show how the modification of the substrate with polymer brushes enhances the particle velocity, where brush chain length plays a significant role as well. The results demonstrate the intrinsic dependence of particle velocity on the flow boundary condition and the thermo-osmotic slip at the interface.

Microscopic Engine Powered by Critical Demixing.

We experimentally demonstrate a microscopic engine powered by the local reversible demixing of a critical mixture. We show that, when an absorbing microsphere is optically trapped by a focused laser beam in a subcritical mixture, it is set into rotation around the optical axis of the beam because of the emergence of diffusiophoretic propulsion. This behavior can be controlled by adjusting the optical power, the temperature, and the criticality of the mixture.

Theory for controlling individual self-propelled micro-swimmers by photon nudging I: directed transport.

Photon nudging is a new experimental method which enables the force-free manipulation and localization of individual self-propelled artificial micro-swimmers in fluidic environments. It uses a weak laser to stochastically and adaptively turn on and off the swimmer's propulsion when the swimmer, through rotational diffusion, points towards or away from its target, respectively. This contribution presents a theoretical framework for the statistics of both 2D and 3D controls. The main results are: the on- and off-time distributions for the controlling laser, the arrival time statistics for the swimmer to reach a remote target, and how the experimentally accessible control parameters influence the control, e.g., the optimal acceptance angle for directed transport. The results are general in that they are independent of the propulsion or the actuation mechanisms. They provide a concrete physical picture for how a single artificial micro-swimmer could be navigated under thermal fluctuations-insights that could also be useful for understanding biological micro-swimmers.

Theory for controlling individual self-propelled micro-swimmers by photon nudging II: confinement.

Photon nudging allows the manipulation and confinement of individual self-propelled micro-swimmers in 2D and 3D environments using feedback controls. Presented in this second part of a two-part contribution are theoretical models that afford the characterization for the positioning distribution associated with active localization. A derivation for the optimal nudging speed and acceptance angle is given for minimal placement uncertainty. The analytical solutions allow for a discussion on the physical underpinning that underlies controllability and optimality.

Thermo-Osmotic Flow in Thin Films.

We report on the first microscale observation of the velocity field imposed by a nonuniform heat content along the solid-liquid boundary. We determine both radial and vertical velocity components of this thermo-osmotic flow field by tracking single tracer nanoparticles. The measured flow profiles are compared to an approximate analytical theory and to numerical calculations. From the measured slip velocity we deduce the thermo-osmotic coefficient for both bare glass and Pluronic F-127 covered surfaces. The value for Pluronic F-127 agrees well with Soret data for polyethylene glycol, whereas that for glass differs from literature values and indicates the complex boundary layer thermodynamics of glass-water interfaces.

Single Molecules Trapped by Dynamic Inhomogeneous Temperature Fields.

We demonstrate a single molecule trapping concept that modulates the actual driving force of Brownian motion--the temperature. By spatially and temporally varying the temperature at a plasmonic nanostructure, thermodiffusive drifts are induced that are used to trap single nano-objects. A feedback controlled switching of local temperature fields allows us to confine the motion of a single DNA molecule for minutes and tailoring complex effective trapping potentials. This new type of thermophoretic microbeaker even provides control over a well-defined number of single molecules and is scalable to large arrays of trapping structures.

Comment on "Optimal detection angle in sub-diffraction resolution photothermal microscopy: application for high sensitivity imaging of biological tissues".

A recent publication [Opt. Express, 22(16), 18833-18842 (2014)] discusses the optimal detection aperture in photothermal single particle microscopy. This new theory is in contradiction with rigorous ab-initio electrodynamic calculations. Nonetheless, the experimentally verified conclusion that a maximum signal occurs at a finite numerical detection aperture remains valid and is in accord with existing models.

Size dependent efficiency of photophoretic swimmers.

We investigate experimentally the efficiency of self-propelled photophoretic swimmers based on metal-coated polymer particles of different sizes. The metal hemisphere absorbs the incident laser power and converts its energy into heat, which dissipates into the environment. A phoretic surface flow arises from the temperature gradient along the particle surface and drives the particle parallel to its symmetry axis. Scaling the particle size from micro to nanometers, the efficiency of converting optical power into motion is expected to rise with the reciprocal size for ideal swimmers. However, due to the finite size of the metal cap, the efficiency of a real swimmer reveals a maximum depending sensitively on the details of the metal cap shape. We compare the experimental results to numerical simulations.

Thermal diffusivity measured using a single plasmonic nanoparticle.

A method to measure thermal diffusivity around a single heated gold nanoparticle is presented. It is based on photothermal single particle microscopy and employs the phase delay of temperature modulation due to finite thermal diffusivity. The phase delay is detected optically averaging over the focal volume of a diffraction limited beam of light. Thermal diffusivity is extracted by comparison to electromagnetic scattering calculations of the photothermal signal. Measurements in the solid (polymer) and liquid (water) are presented and compare well with literature data. The method paves the way for extended measurements of non-diffusive and heterogeneous heat transport in complex media.

Trapping of single nano-objects in dynamic temperature fields.

In this article we explore the dynamics of a Brownian particle in a feedback-free dynamic thermophoretic trap. The trap contains a focused laser beam heating a circular gold structure locally and creating a repulsive thermal potential for a Brownian particle. In order to confine a particle the heating beam is steered along the circumference of the gold structure leading to a non-trivial motion of the particle. We theoretically find a stability condition by switching to a rotating frame, where the laser beam is at rest. Particle trajectories and stable points are calculated as a function of the laser rotation frequency and are experimentally confirmed. Additionally, the effect of Brownian motion is considered. The present study complements the dynamic thermophoretic trapping with a theoretical basis and will enhance the applicability in micro- and nanofluidic devices.

Energy-redistribution signatures in transmission microscopy of Rayleigh and Mie particles.

We describe the transmission characteristics for the interaction of an arbitrary beam with (possibly multilayered) spherical particles of arbitrary size and electric permeability. Within the generalized Lorenz-Mie theory, expressions that generalize the total cross sections to their fractional counterparts are presented, which allow for an analytic quantification of transmission signals, both on-axis and off-axis. For Gaussian (Davis) beams, the relative angular domain of collection as compared to the beam's angle of divergence determines sensitively the shape and magnitude of the interference signal. Depending on the particle's position within the beam, the transmission signatures related to a pure energy redistribution as well as to accompanying absorption are discussed for Rayleigh particles in terms of their complex-valued polarizability. Implications for positioning, temperature control, spectroscopy, and optimized extinction measurements are discussed.

Distortion of power law blinking with binning and thresholding.

Fluorescence intermittency is a random switching between emitting (on) and non-emitting (off) periods found for many single chromophores such as semiconductor quantum dots and organic molecules. The statistics of the duration of on- and off-periods are commonly determined by thresholding the emission time trace of a single chromophore and appear to be power law distributed. Here we test with the help of simulations if the experimentally determined power law distributions can actually reflect the underlying statistics. We find that with the experimentally limited time resolution real power law statistics with exponents α(on/off) ≳ 1.6, especially if α(on) ≠ α(off) would not be observed as such in the experimental data after binning and thresholding. Instead, a power law appearance could simply be obtained from the continuous distribution of intermediate intensity levels. This challenges much of the obtained data and the models describing the so-called power law blinking.

Harnessing synthetic active particles for physical reservoir computing.

The processing of information is an indispensable property of living systems realized by networks of active processes with enormous complexity. They have inspired many variants of modern machine learning, one of them being reservoir computing, in which stimulating a network of nodes with fading memory enables computations and complex predictions. Reservoirs are implemented on computer hardware, but also on unconventional physical substrates such as mechanical oscillators, spins, or bacteria often summarized as physical reservoir computing. Here we demonstrate physical reservoir computing with a synthetic active microparticle system that self-organizes from an active and passive component into inherently noisy nonlinear dynamical units. The self-organization and dynamical response of the unit are the results of a delayed propulsion of the microswimmer to a passive target. A reservoir of such units with a self-coupling via the delayed response can perform predictive tasks despite the strong noise resulting from the Brownian motion of the microswimmers. To achieve efficient noise suppression, we introduce a special architecture that uses historical reservoir states for output. Our results pave the way for the study of information processing in synthetic self-organized active particle systems.

Photothermal single particle Rutherford scattering microscopy.

We demonstrate that the quantum-mechanical description of Rutherford scattering has a photonic counterpart in a new form of single particle photothermal microscopy. Using a split detector we provide experimental evidence that photons are deflected by a photothermal potential that is created by a local refractive index change around a heated nanoparticle. The deflection experienced is shown to be the analog to the deflection of a massive particle wave packet in unscreened spinless Coulomb scattering. The experimentally found focal detection geometry reveals a lateral split feature which will allow new correlation-based velocimetry experiments of absorbing particles with ultrahigh sensitivity.

Photothermal signal distribution analysis (PhoSDA).

Photothermal correlation spectroscopy (PhoCS) is a powerful counterpart to fluorescence correlation spectroscopy (FCS). Using PhoCS it is possible to probe the dynamics of non-fluorescent and non-bleaching ultra-stable metal-nanoparticles in solution and biological specimen, where they can be used as tracers and markers. This paper complements the absorption correlation method by a histogram analysis framework, the photothermal signal distribution analysis (PhoSDA). It is hereby possible to extract individual absorbent tracer concentrations, size dispersions, heterogeneous populations and focal geometry parameters which are otherwise inaccessible by correlation analysis.