Enantioselective transport of chiral spheres using focused femtosecond laser pulses.

Optical tweezers are commonly used for manipulating chiral particles by tailoring the properties of the electromagnetic field or of the particles themselves. Non-linearity provides additional degree of freedom to control the manipulation by changing the trapping conditions. In this work, we leverage the nonlinear optical properties of a medium by illuminating it with a circularly polarized laser pulse, enabling single particle enantioselection for the chiral spheres immersed in it. By adjusting the power of the laser pulses, we demonstrate stable trapping of chiral spheres with one handedness near the focal region, while spheres with the opposite handedness are repelled. This enables the chiral resolution of racemic mixtures. Additionally, we perturbed the stable equilibrium position of the trap by driving the sample stage, leading to the emergence of a new stable equilibrium position achieved under the action of the Stokes force. Here we show that the chirality of each individually trapped particle can also be characterized by the rotation of the equilibrium position. Since the power of the laser pulses can be experimentally controlled, this scheme is practical to perform enantioselection, chiral characterization, and chiral resolution of a single chiral sphere with arbitrarily small chirality parameters.

Tunable Anomalous Scattering and Negative Asymmetry Parameter in a Gain-Functionalized Low Refractive Index Sphere.

Usually, low refractive index passive spheres exhibit strong forward scattering and a positive asymmetry parameter due to weak interference between the electric and magnetic scattering channels. In this work, we investigate, analytically and numerically, the forward scattering of light by a gain-functionalized low refractive index dielectric sphere. It is shown that by tuning the optical gain one can optimize the interference, which provides a novel paradigm to achieve the zero forward scattering and negative asymmetry parameter even for a low refractive index sphere. As a result, a low-density collection of such identical back scatterers provides an anomalous regime, where the scattering mean free path and extinction mean free path are greater than the transport mean free path. Furthermore, we also provide the numerical guideline to achieve the larger extinction mean free path without achieving preferential back-scattering.

Enantioselection and chiral sorting of single microspheres using optical pulling forces.

We put forward a novel, twofold scheme that enables, at the same time, all-optical enantioselection and sorting of single multipolar chiral microspheres based on optical pulling forces exerted by two non-collinear, non-structured, circularly polarized light sources. Our chiral resolution method can be externally controlled by varying the angle between their incident wavevectors, allowing for fine-tuning of the range of chiral indices for enantioselection. Enantioselectivity is achieved by choosing angles such that only particles with the same handedness of the light sources are pulled. This proposal allows one to achieve all-optical sorting of chiral microspheres with arbitrarily small chiral parameters, thus outperforming current optical methods.

Theory of optical tweezing of dielectric microspheres in chiral host media and its applications.

We report for the first time the theory of optical tweezers of spherical dielectric particles embedded in a chiral medium. We develop a partial-wave (Mie) expansion to calculate the optical force acting on a dielectric microsphere illuminated by a circularly-polarized, highly focused laser beam. When choosing a polarization with the same handedness of the medium, the axial trap stability is improved, thus allowing for tweezing of high-refractive-index particles. When the particle is displaced off-axis by an external force, its equilibrium position is rotated around the optical axis by the mechanical effect of an optical torque. Both the optical torque and the angle of rotation are greatly enhanced in the presence of a chiral host medium when considering radii a few times larger than the wavelength. In this range, the angle of rotation depends strongly on the microsphere radius and the chirality parameter of the host medium, opening the way for a quantitative characterization of both parameters. Measurable angles are predicted even in the case of naturally occurring chiral solutes, allowing for a novel all-optical method to locally probe the chiral response at the nanoscale.

Enantioselective manipulation of single chiral nanoparticles using optical tweezers.

We put forward an enantioselective method for chiral nanoparticles using optical tweezers. We demonstrate that the optical trapping force in a typical, realistic optical tweezing setup with circularly-polarized trapping beams is sensitive to the chirality of core-shell nanoparticles, allowing for efficient enantioselection. It turns out that the handedness of the trapped particles can be selected by choosing the appropriate circular polarization of the trapping beam. The chirality of each individual trapped nanoparticle can be characterized by measuring the rotation of the equilibrium position under the effect of a transverse Stokes drag force. We show that the chirality of the shell gives rise to an additional twist, leading to a strong enhancement of the optical torque driving the rotation. Both methods are shown to be robust against variations of size and material parameters, demonstrating that they are particularly useful in (but not restricted to) several situations of practical interest in chiral plasmonics, where enantioselection and characterization of single chiral nanoparticles, each and every one with its unique handedness and optical properties, are in order. In particular, our method could be employed to unveil the chiral response arising from disorder in individual plasmonic raspberries, synthesized by close-packing a large number of metallic nanospheres around a dielectric core.