To Örebro University

Self-assembly of nanoparticles by means of interparticle optical forces provides a compelling approach toward contact-free organization and manipulation of nanoscale entities. However, exploration of the rotational degrees of freedom in this process has remained limited, primarily because of the predominant focus on spherical nanoparticles, for which individual particle orientation cannot be determined. Here, we show that gold nanorods, which self-assemble in water under the influence of circularly polarized light, exhibit synchronized rotational motion at kilohertz frequencies. The synchronization is caused by strong optical interactions and occurs despite the presence of thermal diffusion. Our findings elucidate the intricate dynamics arising from the transfer of photon spin angular momentum to optically bound matter and hold promise for advancing the emerging field of light-driven nanomachinery.

Optically trapped nanoparticles can be used as efficient mobile probes of nanoscopic forces and temperatures. However, it is crucial that the trapped particle has minimal influence on the system under study while providing a strong enough optical response to actually allow for optical manipulation. This puts severe constraints on the particle size and thermal properties. In particular, strong optical responses associated with plasmon resonances in noble metal nanoparticles and Mie resonances in high index dielectric particles can significantly affect trap stability through enhanced radiation pressure forces and photoinduced heating. Using Mie theory and hot Brownian motion analysis, we calculate trap stability and photothermal properties for nanospheres composed of the best (Ag) and most widely used (Au) plasmonic materials as well as for crystalline and amorphous Si, the prototypic high-index dielectric, using polystyrene as a low-index reference material. We calculate trap stability properties for optical tweezers based on high numerical aperture optics (NA = 1.2) for three of the most widely used laser wavelengths (532, 785, and 1064 nm) and for the case of trapping in water. The results reveal the specific particle size ranges for which optical tweezing is possible in two and three dimensions and indicate that crystalline Si nanoparticles trapped using near-infrared laser beams are the optimal choice for temperature-sensitive optical manipulation applications with small particles.

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 similar to 100 nm gold nanoparticles trapped by laser tweezers. The results show that particles can be optically confined at controllable distances ranging between similar to 30 and similar to 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.

Nanoparticles made of high index dielectric materials have seen a surge of interest and have been proposed for various applications, such as metalenses, light harvesting and directional scattering. With the advent of fabrication techniques enabling colloidal suspensions, the prospects of optical manipulation of such nanoparticles becomes paramount. High index nanoparticles support electric and magnetic multipolar responses in the visible regime and interference between such modes can give rise to highly directional scattering, in particular a cancellation of back-scattered radiation at the first Kerker condition. Here we present a study of the optical forces on silicon nanoparticles in the visible and near infrared calculated using the transfer matrix method. The zero-backscattering Kerker condition is investigated as an avenue to reduce radiation pressure in an optical trap. We find that while asymmetric scattering does reduce the radiation pressure, the main determining factor of trap stability is the increased particle response near the geometric resonances. The trap stability for non-spherical silicon nanoparticles is also investigated and we find that ellipsoidal deformation of spheres enables trapping of slightly larger particles.

Brownian microparticles diffusing in optical potential-energy landscapes constitute a generic test bed for nonequilibrium statistical thermodynamics and have been used to emulate a wide variety of physical systems, ranging from Josephson junctions to Carnot engines. Here we demonstrate that it is possible to scale down this approach to nanometric length scales by constructing a tilted washboard potential for the rotation of plasmonic gold nanorods. The potential depth and tilt can be precisely adjusted by modulating the light polarization. This allo`ws for a gradual transition from continuous rotation to discrete stochastic jumps, which are found to follow Kramers dynamics in excellent agreement with stochastic simulations. The results widen the possibilities for fundamental experiments in statistical physics and provide insights into how to construct light-driven nanomachines and multifunctional sensing elements.

Gold nanorods can be optically trapped in aqueous solution and forced to rotate at kilohertz rates by circularly polarized laser light. This enables detailed investigations of local environmental parameters and processes, such as medium viscosity and nanoparticle-molecule reactions. Future applications may include nanoactuation and single-cell analysis. However, the influence of photothermal heating on the nanoparticle dynamics needs to be better understood in order to realize widespread and quantitative use. Here we analyze the hot Brownian motion of a rotating gold nanorod trapped in two dimensions by an optical tweezers using experiments and stochastic simulations. We show that, for typical settings, the effective rotational and translational Brownian temperatures are drastically different, being closer to the nanorod surface temperature and ambient temperature, respectively. Further, we show that translational dynamics can have a non-negligible influence on the rotational fluctuations due to the small size of a nanorod in comparison to the focal spot. These results are crucial for the development of gold nanorods into generic and quantitative optomechanical sensor and actuator elements. (C) 2017 Optical Society of America

Here we investigate the energy transfer rates of a Förster resonance energy transfer (FRET) pair positioned in close proximity to a 5 nm gold nanoparticle (AuNP) on a DNA origami construct. We study the distance dependence of the FRET rate by varying the location of the donor molecule, D, relative to the AuNP while maintaining a fixed location of the acceptor molecule, A. The presence of the AuNP induces an alteration in the spontaneous emission of the donor (including radiative and non-radiative rates) which is strongly dependent on the distance between the donor and AuNP surface. Simultaneously, the energy transfer rates are enhanced at shorter D-A (and D-AuNP) distances. Overall, in addition to the direct influence of the acceptor and AuNP on the donor decay there is also a significant increase in decay rate not explained by the sum of the two interactions. This leads to enhanced energy transfer between donor and acceptor in the presence of a 5 nm AuNP. We also demonstrate that the transfer rate in the three "particle" geometry (D + A + AuNP) depends approximately linearly on the transfer rate in the donor-AuNP system, suggesting the possibility to control FRET process with electric field induced by 5 nm AuNPs close to the donor fluorophore. It is concluded that DNA origami is a very versatile platform for studying interactions between molecules and plasmonic nanoparticles in general and FRET enhancement in particular.

Optically thin perfect light absorbers could find many uses in science and technology. However, most physical realizations of perfect absorption for the optical range rely on plasmonic excitations in nanostructured metallic metasurfaces, for which the absorbed light energy is quickly lost as heat due to rapid plasmon decay. Here we show that a silicon metasurface excited in a total internal reflection configuration can absorb at least 97% of incident near-infrared light due to interferences between coherent electric and magnetic dipole scattering from the silicon nanopillars that build up the metasurface and the reflected wave from the supporting glass substrate. This "near-perfect" absorption phenomenon loads more than 50 times more light energy into the semiconductor than what would be the case for a uniform silicon sheet of equal surface density, irrespective of incident polarization. We envisage that the concept could be used for the development of novel light harvesting and optical sensor devices.

Plasmonic gold nanorods are prime candidates for a variety of biomedical, spectroscopy, data storage, and sensing applications. It was recently shown that gold nanorods optically trapped by a focused circularly polarized laser beam can function as extremely efficient nanoscopic rotary motors. The system holds promise for-applications ranging from nanofluidic flow control and nanorobotics to biomolecular actuation and analysis. However, to fully exploit this potential, one needs to be able to control and understand heating effects associated with laser trapping. We investigated photothermal heating of individual rotating gold nanorods by simultaneously probing their localized surface plasmon resonance spectrum and rotational Brownian dynamics over extended periods of time. The data reveal an extremely slow nanoparticle reshaping process, involving migration of the order of a few hundred atoms per minute, for moderate laser powers and a trapping wavelength close to plasmon resonance. The plasmon spectroscopy and Brownian analysis allows for separate temperature estimates based on the refractive index and the viscosity of the water surrounding a trapped nanorod. We show that both measurements yield similar effective temperatures, which correspond to the actual temperature at a distance of the order 10-15 nm from the particle surface. Our results shed light on photothermal processes on the nanoscale and will be useful in evaluating the applicability and performance of nanorod motors and optically heated nanoparticles for a variety of applications.

Efficient and robust artificial nanomotors could provide a variety of exciting possibilities for applications in physics, biology and chemistry, including nanoelectromechanical systems, biochemical sensing, and drug delivery. However, the application of current man-made nanomotors is limited by their sophisticated fabrication techniques, low mechanical output power and severe environmental requirements, making their performance far below that of natural biomotors. Here we show that single-crystal gold nanorods can be rotated extremely fast in aqueous solutions through optical torques dominated by plasmonic resonant scattering of circularly polarized laser light with power as low as a few mW. The nanorods are trapped in 2D against a glass surface, and their rotational dynamics is highly dependent on their surface plasmon resonance properties. They can be kept continuously rotating for hours with limited photothermal side effects and they can be applied for detection of molecular binding with high sensitivity. Because of their biocompatibility, mechanical and thermal stability, and record rotation speeds reaching up to 42 kHz (2.5 million revolutions per minute), these rotary nanomotors could advance technologies to meet a wide range of future nanomechanical and biomedical needs in fields such as nanorobotics, nanosurgery, DNA manipulation and nano/microfluidic flow control.