The prospect of self-propelled artificial machines small enough to navigate within biological matter has fascinated and inspired researchers and the public alike since the dawn of nanotechnology. Despite many obstacles toward the realization of such devices, impressive progress on the development of its basic building block, the nanomotor, has been made over the past decade. Here, we review this emerging area with a focus on inorganic nanomotors driven or activated by light. We outline the distinct challenges and opportunities that differentiate nanomotors from micromotors based on a discussion of how stochastic forces influence the active motion of small particles. We introduce the relevant light–matter interactions and discuss how these can be utilized to classify nanomotors into three broad classes: nanomotors driven by optical momentum transfer, photothermal heating, and photocatalysis, respectively. On the basis of this classification, we then summarize and discuss the diverse body of nanomotor literature. We finally give a brief outlook on future challenges and possibilities in this rapidly evolving research area.
Label-free characterization of single biomolecules aims to complement fluorescence microscopy in situations where labeling compromises data interpretation, is technically challenging or even impossible. However, existing methods require the investigated species to bind to a surface to be visible, thereby leaving a large fraction of analytes undetected. Here, we present nanofluidic scattering microscopy (NSM), which overcomes these limitations by enabling label-free, real-time imaging of single biomolecules diffusing inside a nanofluidic channel. NSM facilitates accurate determination of molecular weight from the measured optical contrast and of the hydrodynamic radius from the measured diffusivity, from which information about the conformational state can be inferred. Furthermore, we demonstrate its applicability to the analysis of a complex biofluid, using conditioned cell culture medium containing extracellular vesicles as an example. We foresee the application of NSM to monitor conformational changes, aggregation and interactions of single biomolecules, and to analyze single-cell secretomes.
In comparison to nanoplasmonic structures, resonant high-index dielectric nanoantennas hold several advantages that may benefit nanophotonic applications, including CMOS compatibility and low ohmic losses. One such application area might be label-free refractometric sensing, where changes in individual antenna resonance properties are used to quantify changes in the surrounding refractive index, for example, due to biomolecular binding. Here, we analyze and compare the sensing performance of silicon and gold nanodisks using a common and unbiased testing framework. We find that the all-dielectric system is fully capable of effectively monitoring small changes in bulk refractive index and biomolecular coverage, but the sensitivity is five to ten times lower than the plasmonic counterpart. However, this drawback is partly compensated for by a more linear response to adsorbate layer thickness changes and an approximately four times smaller susceptibility to photothermal heating. Finally, dielectric sensors may show promise if certain strategies are employed to improve their performance, which could thus bridge the gap between the two systems.
Antibody-antigen interactions are complex events central to immune response, in vivo and in vitro diagnostics, and development of therapeutic substances. We developed an ultrastable single-molecule localized surface plasmon resonance (LSPR) sensing platform optimized for studying antibody-antigen interaction kinetics over very long time scales. The setup allowed us to perform equilibrium fluctuations analysis of the PEG/anti-PEG interaction. By time and frequency domain analysis, we demonstrate that reversible adsorption of monovalently bound anti-PEG antibodies is the dominant factor affecting the LSPR fluctuations. The results suggest that equilibrium fluctuation analysis can be an alternative to established methods for determination of interaction rates. In particular, the methodology is suited to analyze molecular systems whose properties change during the initial interaction phases, for example, due to mass transport limitations or, as demonstrated here, because the effective association rate constant varies with surface concentration of adsorbed molecules.
Active particles break out of thermodynamic equilibrium thanks to their directed motion, which leads to complex and interesting behaviors in the presence of confining potentials. When dealing with active nanoparticles, however, the overwhelming presence of rotational diffusion hinders directed motion, leading to an increase of their effective temperature, but otherwise masking the effects of self-propulsion. Here, we demonstrate an experimental system where an active nanoparticle immersed in a critical solution and held in an optical harmonic potential features far-from-equilibrium behavior beyond an increase of its effective temperature. When increasing the laser power, we observe a cross-over from a Boltzmann distribution to a non-equilibrium state, where the particle performs fast orbital rotations about the beam axis. These findings are rationalized by solving the Fokker-Planck equation for the particle’s position and orientation in terms of a moment expansion. The proposed self-propulsion mechanism results from the particle’s non-sphericity and the lower critical point of the solution.
Particles that diffuse in close proximity to a surface are expected to behave differently than in free solution because the surface interaction will influence a number of physical properties, including the hydrodynamic, optical, and thermal characteristics of the particle. Understanding the influence of such effects is particularly important in view of the increasing interest in laser tweezing of colloidal resonant nanoparticles for applications such as nanomotors and optical printing and for investigations of unconventional optical forces. Therefore, we used total internal reflection microscopy to probe the interaction between a glass surface and individual ∼100 nm gold nanoparticles trapped by laser tweezers. The results show that particles can be optically confined at controllable distances ranging between ∼30 and ∼90 nm from the surface, depending on the radiation pressure of the trapping laser and the ionic screening of the surrounding liquid. Moreover, the full particle–surface distance probability distribution can be obtained for single nanoparticles by analyzing temporal signal fluctuations. The experimental results are in excellent agreement with Brownian dynamics simulations that take the full force field and photothermal heating into account. At the observed particle–surface distances, translational friction coefficients increase by up to 60% compared to freely diffusing particles, whereas the rotational friction and thermal dissipation are much less affected. The methodology used here is general and can be adapted to a range of single nanoparticle–surface interaction investigations.
Optical rotation of laser tweezed nanoparticles offers a convenient means for optical to mechanical force transduction and sensing at the nanoscale. Plasmonic nanoparticles are the benchmark system for such studies, but their rapid rotation comes at the price of high photoinduced heating due to Ohmic losses. We show that Mie resonant silicon nanorods with characteristic dimensions of ∼220 × 120 nm 2 can be optically trapped and rotated at frequencies up to 2 kHz in water using circularly polarized laser light. The temperature excess due to heating from the trapping laser was estimated by phonon Raman scattering and particle rotation analysis. We find that the silicon nanorods exhibit slightly improved thermal characteristics compared to Au nanorods with similar rotation performance and optical resonance anisotropy. Altogether, the results indicate that silicon nanoparticles have the potential to become the system of choice for a wide range of optomechanical applications at the nanoscale.
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