Challenges on optical printing of colloidal nanoparticles.

While colloidal chemistry provides ways to obtain a great variety of nanoparticles with different shapes, sizes, material compositions, and surface functions, their controlled deposition and combination on arbitrary positions of substrates remain a considerable challenge. Over the last ten years, optical printing arose as a versatile method to achieve this purpose for different kinds of nanoparticles. In this article, we review the state of the art of optical printing of single nanoparticles and discuss its strengths, limitations, and future perspectives by focusing on four main challenges: printing accuracy, resolution, selectivity, and nanoparticle photostability.

Kerker Conditions upon Lossless, Absorption, and Optical Gain Regimes.

The directionality and polarization of light show peculiar properties when the scattering by a dielectric sphere can be described exclusively by electric and magnetic dipolar modes. Particularly, when these modes oscillate in phase with equal amplitude, at the so-called first Kerker condition, the zero optical backscattering condition emerges for nondissipating spheres. However, the role of absorption and optical gain in the first Kerker condition remains unexplored. In this work, we demonstrate that either absorption or optical gain precludes the first Kerker condition and, hence, the absence of backscattered radiation light, regardless of the particle's size, incident wavelength, and incoming polarization. Finally, we derive the necessary prerequisites of the second Kerker condition of the zero forward light scattering, finding that optical gain is a compulsory requirement.

Extraordinary Multipole Modes and Ultra-Enhanced Optical Lateral Force by Chirality.

Strong mode coupling and Fano resonances arisen from exceptional interaction between resonant modes in single nanostructures have raised much attention for their advantages in nonlinear optics, sensing, etc. Individual electromagnetic multipole modes such as quadrupoles, octupoles, and their counterparts from mode coupling (toroidal dipole and nonradiating anapole mode) have been well investigated in isolated or coupled nanostructures with access to high Q factors in bound states in the continuum. Albeit the extensive study on ordinary dielectric particles, intriguing aspects of light-matter interactions in single chiral nanostructures is lacking. Here, we unveil that extraordinary multipoles can be simultaneously superpositioned in a chiral nanocylinder, such as two toroidal dipoles with opposite moments, and electric and magnetic sextupoles. The induced optical lateral forces and their scattering cross sections can thus be either significantly enhanced in the presence of those multipoles with high-Q factors, or suppressed by the bound states in the continuum. This work for the first time reveals the complex correlation between multipolar effects, chiral coupling, and optical lateral force, providing a distinct way for advanced optical manipulation.

Band gap formation and Anderson localization in disordered photonic materials with structural correlations.

Disordered dielectric materials with structural correlations show unconventional optical behavior: They can be transparent to long-wavelength radiation, while at the same time have isotropic band gaps in another frequency range. This phenomenon raises fundamental questions concerning photon transport through disordered media. While optical transparency in these materials is robust against recurrent multiple scattering, little is known about other transport regimes like diffusive multiple scattering or Anderson localization. Here, we investigate band gaps, and we report Anderson localization in 2D disordered dielectric structures using numerical simulations of the density of states and optical transport statistics. The disordered structures are designed with different levels of positional correlation encoded by the degree of stealthiness [Formula: see text] To establish a unified view, we propose a correlation-frequency ([Formula: see text]-[Formula: see text]) transport phase diagram. Our results show that, depending only on [Formula: see text], a dielectric material can transition from localization behavior to a band gap crossing an intermediate regime dominated by tunneling between weakly coupled states.

Generalized Brewster effect in high-refractive-index nanorod-based metasurfaces.

The interference between electric and magnetic dipolar fields is known to lead to asymmetric angular distributions of the scattered intensity from small high refractive index (HRI) particles. Properly designed all-dielectric metasurfaces based on HRI spheres have been shown to exhibit zero reflectivity, a generalized Brewster's effect, potentially for any angle, wavelength and polarization of choice. At normal incidence, the effect is related to the absence of backscattering from small dielectric spheres or disks at the, so-called, first Kerker condition. In contrast, homogeneous HRI cylinders do not fulfil the first Kerker condition due to the mismatch between the local electric and magnetic density of states. In this work, we show that although a zero back-scattering condition can never be achieved for individual cylinders, when they are arranged in a periodic array their mutual interaction leads to an anomalous Kerker condition, leading to a generalized Brewster's effect in a nanorod-based metasurface. We derive a coupled electric and magnetic dipole (CEMD) analytical formulation to describe the properties of a periodic array of HRI nanorods in full agreement with exact numerical calculations.

Isotropically polarized speckle patterns.

The polarization of the light scattered by an optically dense and random solution of dielectric nanoparticles shows peculiar properties when the scatterers exhibit strong electric and magnetic polarizabilities. While the distribution of the scattering intensity in these systems shows the typical irregular speckle patterns, the helicity of the incident light can be fully conserved when the electric and magnetic polarizabilities of the scatterers are equal. We show that the multiple scattering of helical beams by a random dispersion of "dual" dipolar nanospheres leads to a speckle pattern exhibiting a perfect isotropic constant polarization, a situation that could be useful in coherent control of light as well as in lasing in random media.

Demonstration of zero optical backscattering from single nanoparticles.

We present the first experimental demonstration of zero backscattering from nanoparticles at optical frequencies as originally discussed by Kerker et al. [ Kerker , M. ; Wang , D. ; Giles , C. J. Opt. Soc. A 1983 , 73 , 765 ]. GaAs pillars were fabricated on a fused silica substrate and the spectrum of the backscattered radiation was measured in the wavelength range 600-1000 nm. Suppression of backscattering occurred at ~725 nm, agreeing with calculations based on the discrete dipole approximation. Particles with zero backscattering provide new functionality for metamaterials and optical antennas.

Sensing with magnetic dipolar resonances in semiconductor nanospheres.

In this work we propose two novel sensing principles of detection that exploit the magnetic dipolar Mie resonance in high-refractive-index dielectric nanospheres. In particular, we theoretically investigate the spectral evolution of the extinction and scattering cross sections of these nanospheres as a function of the refractive index of the external medium (next). Unlike resonances in plasmonic nanospheres, the spectral position of magnetic resonances in high-refractive-index nanospheres barely shifts as next changes. Nevertheless, there is a drastic reduction in the extinction cross section of the nanospheres when next increases, especially in the magnetic dipolar spectral region, which is accompanied with remarkable variations in the radiation patterns. Thanks to these changes, we propose two new sensing parameters, which are based on the detection of: i) the intensity variations in the transmitted or backscattered radiation by the dielectric nanospheres at the magnetic dipole resonant frequency, and ii) the changes in the radiation pattern at the frequency that satisfies Kerker's condition of near-zero forward radiation. To optimize the sensitivity, we consider several semiconductor materials and particles sizes.

Light spin forces in optical traps: comment on "Trapping metallic Rayleigh particles with radial polarization".

An incomplete modeling of the scattering forces on a Rayleigh particle without taking into account the light spin forces in "Trapping metallic Rayleigh particles with radial polarization" by Q. Zhan, leads to erroneous statements on the advantages of using radial polarization to trap metallic particles.

Scattering forces and electromagnetic momentum density in crossed circularly polarized standing waves.

We analyze the forces on a small dipolar particle and the electromagnetic momentum density in a configuration consisting in two perpendicular circularly polarized stationary waves. The field distribution shows regions in which the electric and magnetic fields are parallel corresponding to a null Poynting vector. Although the average value of the momentum density, proportional to the Poynting vector, is zero in these regions, there are scattering forces acting on small particles due to light's spin force. The total scattering force suggests a new definition of the average value of the momentum density for free propagating electromagnetic fields.

Scattering forces and electromagnetic momentum density in crossed circularly polarized standing waves.

We analyze the forces on a small dipolar particle and the electromagnetic momentum density in a configuration consisting in two perpendicular circularly polarized stationary waves. The field distribution shows regions in which the electric and magnetic fields are parallel corresponding to a null Poynting vector. Although the average value of the momentum density, proportional to the Poynting vector, is zero in these regions, there are scattering forces acting on small particles due to light's spin force. The total scattering force suggests a new definition of the average value of the momentum density for free propagating electromagnetic fields.

Plasmonic nanoparticle chain in a light field: a resonant optical sail.

Optical trapping and driving of small objects has become a topic of increasing interest in multidisciplinary sciences. We propose to use a chain made of metallic nanoparticles as a resonant light sail, attached by one end point to a transparent object and propelling it by the use of electromagnetic radiation. Driving forces exerted on the chain are theoretically studied as a function of radiation's wavelength and chain's alignments with respect to the direction of radiation. Interestingly, there is a window in the frequency spectrum in which null-torque equilibrium configuration, with minimum geometric cross section, corresponds to a maximum in the driving force.

A Chirality-Based Quantum Leap.

There is increasing interest in the study of chiral degrees of freedom occurring in matter and in electromagnetic fields. Opportunities in quantum sciences will likely exploit two main areas that are the focus of this Review: (1) recent observations of the chiral-induced spin selectivity (CISS) effect in chiral molecules and engineered nanomaterials and (2) rapidly evolving nanophotonic strategies designed to amplify chiral light-matter interactions. On the one hand, the CISS effect underpins the observation that charge transport through nanoscopic chiral structures favors a particular electronic spin orientation, resulting in large room-temperature spin polarizations. Observations of the CISS effect suggest opportunities for spin control and for the design and fabrication of room-temperature quantum devices from the bottom up, with atomic-scale precision and molecular modularity. On the other hand, chiral-optical effects that depend on both spin- and orbital-angular momentum of photons could offer key advantages in all-optical and quantum information technologies. In particular, amplification of these chiral light-matter interactions using rationally designed plasmonic and dielectric nanomaterials provide approaches to manipulate light intensity, polarization, and phase in confined nanoscale geometries. Any technology that relies on optimal charge transport, or optical control and readout, including quantum devices for logic, sensing, and storage, may benefit from chiral quantum properties. These properties can be theoretically and experimentally investigated from a quantum information perspective, which has not yet been fully developed. There are uncharted implications for the quantum sciences once chiral couplings can be engineered to control the storage, transduction, and manipulation of quantum information. This forward-looking Review provides a survey of the experimental and theoretical fundamentals of chiral-influenced quantum effects and presents a vision for their possible future roles in enabling room-temperature quantum technologies.

Light control of silver nanoparticle's diffusion.

The diffusion of silver nanoparticles in water at 298K inside an optical vortex lattice is analyzed in detail by numerical simulations. At power densities of the order of those used to trap nanoparticles with optical tweezers, the dynamic response shows three different regimes depending on the light wavelength. In the first one particles get trapped inside the light vortices following almost closed trajectories. In the second one, around the plasmon resonance, the diffusion constant is dramatically enhanced with respect to the Brownian motion. In the third one, at longer wavelengths, nanoparticles are confined during a few seconds in quasi-one-dimensional optical traps.

Nanogeometry matters: unexpected decrease of capillary adhesion forces with increasing relative humidity.

The sticking effect between hydrophilic surfaces occurring at increasing relative humidity (RH) is an everyday phenomenon with uncountable implications. Here experimental evidence is presented for a counterintuitive monotonous decrease of the capillary adhesion forces between hydrophilic surfaces with increasing RH for the whole humidity range. It is shown that this unexpected result is related to the actual shape of the asperity at the nanometer scale: a model based on macroscopic thermodynamics predicts this decrease in the adhesion force for a sharp object ending in an almost flat nanometer-sized apex, in full agreement with experiments. This anomalous decrease is due to the fact that a significant growth of the liquid meniscus formed at the contact region with increasing humidity is hindered for this geometry. These results are relevant in the analysis of the dynamical behavior of nanomenisci. They could also have an outstanding value in technological applications, since the undesirable sticking effect between surfaces occurring at increasing RH could be avoided by controlling the shape of the surface asperities at the nanometric scale.

Giant enhanced diffusion of gold nanoparticles in optical vortex fields.

We study the diffusion of a metal nanoparticle in the nonconservative force field of an optical vortex lattice. Radiation pressure in the vortex array is shown to induce a giant enhancement over the free thermal diffusion. Langevin dynamics simulations show that the diffusion coefficient of (50 nm radius) gold particles at room temperature is enhanced by 2 orders of magnitude at power densities of the order or smaller than those used to trap nanoparticles with optical tweezers.

Chirality-assisted lateral momentum transfer for bidirectional enantioselective separation.

Lateral optical forces induced by linearly polarized laser beams have been predicted to deflect dipolar particles with opposite chiralities toward opposite transversal directions. These "chirality-dependent" forces can offer new possibilities for passive all-optical enantioselective sorting of chiral particles, which is essential to the nanoscience and drug industries. However, previous chiral sorting experiments focused on large particles with diameters in the geometrical-optics regime. Here, we demonstrate, for the first time, the robust sorting of Mie (size ~ wavelength) chiral particles with different handedness at an air-water interface using optical lateral forces induced by a single linearly polarized laser beam. The nontrivial physical interactions underlying these chirality-dependent forces distinctly differ from those predicted for dipolar or geometrical-optics particles. The lateral forces emerge from a complex interplay between the light polarization, lateral momentum enhancement, and out-of-plane light refraction at the particle-water interface. The sign of the lateral force could be reversed by changing the particle size, incident angle, and polarization of the obliquely incident light.

Living Nanospear for Near-Field Optical Probing.

Optical nanoprobes, designed to emit or collect light in the close proximity of a sample, have been extensively used to sense and image at nanometer resolution. However, the available nanoprobes, constructed from artificial materials, are incompatible and invasive when interfacing with biological systems. In this work, we report a fully biocompatible nanoprobe for subwavelength probing of localized fluorescence from leukemia single-cells in human blood. The bioprobe is built on a tapered fiber tip apex by optical trapping of a yeast cell (1.4 µm radius) and a chain of Lactobacillus acidophilus cells (2 µm length and 200 nm radius), which act as a high-aspect-ratio nanospear. Light propagating along the bionanospear can be focused into a spot with a full width at half-maximum (fwhm) of 190 nm on the surface of single cells. Fluorescence signals are detected in real time at subwavelength spatial resolution. These noninvasive and biocompatible optical probes will find applications in imaging and manipulation of biospecimens.