Strong optical force of a molecule enabled by the plasmonic nanogap hot spot in a tip-enhanced Raman spectroscopy system

Li Long, Jianfeng Chen, Huakang Yu, and Zhi-Yuan Li

Tip-enhanced Raman spectroscopy (TERS) offers a powerful means to enhance the Raman scattering signal of a molecule as the localized surface plasmonic resonance will induce a significant local electric field enhancement in the nanoscale hot spot located within the nanogap of the TERS system. In this work, we theoretically show that this nanoscale hot spot can also serve as powerful optical tweezers to tightly trap a molecule. We calculate and analyze the local electric field and field gradient distribution of this nanogap plasmon hot spot. Due to the highly localized electric field, a three-dimensional optical trap can form at the hot spot. Moreover, the optical energy density and optical force acting on a molecule can be greatly enhanced to a level far exceeding the conventional single laser beam optical tweezers. Calculations show that for a single H2TBPP organic molecule, which is modeled as a spherical molecule with a radius of 𝑟𝑚=1  nm, a dielectric coefficient 𝜀=3, and a polarizability 𝛼=4.5×10−38  C·m2/V, the stiffness of the hot-spot trap can reach a high value of about 2  pN/[(W/cm2)·m] and 40  pN/[(W/cm2)·m] in the direction perpendicular and parallel to the TERS tip axis, which is far larger than the stiffness of single-beam tweezers, ∼0.4  pN/[(W/cm2)·m]. This hard-stiffness will enable the molecules to be stably captured in the plasmon hot spot. Our results indicate that TERS can become a promising tool of optical tweezers for trapping a microscopic object like molecules while implementing Raman spectroscopic imaging and analysis at the same time.

DOI

All-dielectric silicon metalens for two-dimensional particle manipulation in optical tweezers

Teanchai Chantakit, Christian Schlickriede, Basudeb Sain, Fabian Meyer, Thomas Weiss, Nattaporn Chattham, and Thomas Zentgraf

Dynamic control of compact chip-scale contactless manipulation of particles for bioscience applications remains a challenging endeavor, which is restrained by the balance between trapping efficiency and scalable apparatus. Metasurfaces offer the implementation of feasible optical tweezers on a planar platform for shaping the exerted optical force by a microscale-integrated device. Here we design and experimentally demonstrate a highly efficient silicon-based metalens for two-dimensional optical trapping in the near-infrared. Our metalens concept is based on the Pancharatnam–Berry phase, which enables the device for polarization-sensitive particle manipulation. Our optical trapping setup is capable of adjusting the position of both the metasurface lens and the particle chamber freely in three directions, which offers great freedom for optical trap adjustment and alignment. Two-dimensional (2D) particle manipulation is done with a relatively low-numerical-aperture metalens (NAML=0.6). We experimentally demonstrate both 2D polarization-sensitive drag and drop manipulation of polystyrene particles suspended in water and transfer of angular orbital momentum to these particles with a single tailored beam. Our work may open new possibilities for lab-on-a-chip optical trapping for bioscience applications and microscale to nanoscale optical tweezers.

DOI

Synthetic optical vortex beams from the analogous trajectory change of an artificial satellite

Haiping Wang, Liqin Tang, Jina Ma, Xiuyan Zheng, Daohong Song, Yi Hu, Yigang Li, and Zhigang Chen

We propose a method to generate specially shaped high-order singular beams of pre-designed intensity distributions. Such a method does not a priori assume a phase formula, but rather relies on the “cake-cutting and assembly” approach to achieve the azimuthal phase gradient for beam shaping, inspired by the orbital motion trajectory change of an artificial satellite. Based on our method, several typical vortex beams with desired intensity patterns are experimentally generated. As an example, we realize optical trapping and transportation of microorganisms with a triangle-shaped vortex beam, demonstrating the applicability of such unconventional vortex beams in optical trapping and manipulation.

DOI

Plasmonic resonant nonlinearity and synthetic optical properties in gold nanorod suspensions

Huizhong Xu, Pepito Alvaro, Yinxiao Xiang, Trevor S. Kelly, Yu-Xuan Ren, Chensong Zhang, and Zhigang Chen

We experimentally demonstrate self-trapping of light, as a result of plasmonic resonant optical nonlinearity, in both aqueous and organic (toluene) suspensions of gold nanorods. The threshold power for soliton formation is greatly reduced in toluene as opposed to aqueous suspensions. It is well known that the optical gradient forces are optimized at off-resonance wavelengths at which suspended particles typically exhibit a strong positive (or negative) polarizability. However, surprisingly, as we tune the wavelength of the optical beam from a continuous-wave (CW) laser, we find that the threshold power is reduced by more than threefold at the plasmonic resonance frequency. By analyzing the optical forces and torque acting on the nanorods, we show theoretically that it is possible to align the nanorods inside a soliton waveguide channel into orthogonal orientations by using merely two different laser wavelengths. We perform a series of experiments to examine the transmission of the soliton-forming beam itself, as well as the polarization transmission spectrum of a low-power probe beam guided along the soliton channel. It is found that the expected synthetic anisotropic properties are too subtle to be clearly observed, in large part due to Brownian motion of the solvent molecules and a limited ordering region where the optical field from the self-trapped beam is strong enough to overcome thermodynamic fluctuations. The ability to achieve tunable nonlinearity and nanorod orientations in colloidal nanosuspensions with low-power CW laser beams may lead to interesting applications in all-optical switching and transparent display technologies.

DOI

Optically induced rotation of Rayleigh particles by arbitrary photonic spin

Guanghao Rui, Ying Li, Sichao Zhou, Yusong Wang, Bing Gu, Yiping Cui, and Qiwen Zhan

Optical trapping techniques hold great interest for their advantages that enable direct handling of nanoparticles. In this work, we study the optical trapping effects of a diffraction-limited focal field possessing an arbitrary photonic spin and propose a convenient method to manipulate the movement behavior of the trapped nanoparticles. In order to achieve controllable spin axis orientation and ellipticity of the tightly focused beam in three dimensions, an efficient method to analytically calculate and experimentally generate complex optical fields at the pupil plane of a high numerical aperture lens is developed. By numerically calculating the optical forces and torques of Rayleigh particles with spherical/ellipsoidal shape, we demonstrate that the interactions between the tunable photonic spin and nanoparticles lead to not only 3D trapping but also precise control of the nanoparticles’ movements in terms of stable orientation, rotational orientation, and rotation frequency. This versatile trapping method may open up new avenues for optical trapping and their applications in various scientific fields.

DOI

Sequential trapping of single nanoparticles using a gold plasmonic nanohole array

Xue Han, Viet Giang Truong, Prince Sunil Thomas, and Síle Nic Chormaic

We have used a gold nanohole array to trap single polystyrene nanoparticles, with a mean diameter of 30 nm, into separated hot spots located at connecting nanoslot regions. A high trap stiffness of approximately [Math Processing Error] at a low-incident laser intensity of [Math Processing Error] at 980 nm was obtained. The experimental results were compared to the simulated trapping force, and a reasonable match was achieved. This plasmonic array is useful for lab-on-a-chip applications and has particular appeal for trapping multiple nanoparticles with predefined separations or arranged in patterns in order to study interactions between them.

DOI

Enhancing plasmonic trapping with a perfect radially polarized beam

Xianyou Wang, Yuquan Zhang, Yanmeng Dai, Changjun Min, and Xiaocong Yuan

Strong plasmonic focal spots, excited by radially polarized light on a smooth thin metallic film, have been widely applied to trap various micro- and nano-sized objects. However, the direct transmission part of the incident light leads to the scattering force exerted on trapped particles, which seriously affects the stability of the plasmonic trap. Here we employ a novel perfect radially polarized beam to solve this problem. Both theoretical and experimental results verify that such a beam could strongly suppress the directly transmitted light to reduce the piconewton scattering force, and an enhanced plasmonic trapping stiffness that is 2.6 times higher is achieved in experiments. The present work opens up new opportunities for a variety of research requiring the stable manipulations of particles.

DOI

Surface enhanced Raman scattering of gold nanoparticles aggregated by a gold-nanofilm-coated nanofiber

Chang Cheng, Juan Li, Hongxiang Lei, and Baojun Li

Aggregation of metal nanoparticles plays an important role in surface enhanced Raman scattering (SERS). Here, a strategy of dynamically aggregating/releasing gold nanoparticles is demonstrated using a gold-nanofilm-coated nanofiber, with the assistance of enhanced optical force and plasmonic photothermal effect. Strong SERS signals of rhodamine 6G are achieved at the hotspots formed in the inter-particle and film-particle nanogaps. The proposed SERS substrate was demonstrated to have a sensitivity of 10−12 M, reliable reproducibility, and good stability.

DOI

Optical trapping of single quantum dots for cavity quantum electrodynamics

Pengfei Zhang, Gang Song, and Li Yu

We report here a nanostructure that traps single quantum dots for studying strong cavity-emitter coupling. The nanostructure is designed with two elliptical holes in a thin silver patch and a slot that connects the holes. This structure has two functionalities: (1) tweezers for optical trapping; (2) a plasmonic resonant cavity for quantum electrodynamics. The electromagnetic response of the cavity is calculated by finite-difference time-domain (FDTD) simulations, and the optical force is characterized based on the Maxwell’s stress tensor method. To be tweezers, this structure tends to trap quantum dots at the edges of its tips where light is significantly confined. To be a plasmonic cavity, its plasmonic resonant mode interacts strongly with the trapped quantum dots due to the enhanced electric field. Rabi splitting and anti-crossing phenomena are observed in the calculated scattering spectra, demonstrating that a strong-coupling regime has been achieved. The method present here provides a robust way to position a single quantum dot in a nanocavity for investigating cavity quantum electrodynamics.

DOI

Single nanoparticle trapping based on on-chip nanoslotted nanobeam cavities

Daquan Yang, Fei Gao, Qi-Tao Cao, Chuan Wang, Yuefeng Ji, and Yun-Feng Xiao

Optical trapping techniques are of great interest since they have the advantage of enabling the direct handling of nanoparticles. Among various optical trapping systems, photonic crystal nanobeam cavities have attracted great attention for integrated on-chip trapping and manipulation. However, optical trapping with high efficiency and low input power is still a big challenge in nanobeam cavities because most of the light energy is confined within the solid dielectric region. To this end, by incorporating a nanoslotted structure into an ultracompact one-dimensional photonic crystal nanobeam cavity structure, we design a promising on-chip device with ultralarge trapping potential depth to enhance the optical trapping characteristic of the cavity. In this work, we first provide a systematic analysis of the optical trapping force for an airborne polystyrene (PS) nanoparticle trapped in a cavity model. Then, to validate the theoretical analysis, the numerical simulation proof is demonstrated in detail by using the three-dimensional finite element method. For trapping a PS nanoparticle of 10 nm radius within the air-slot, a maximum trapping force as high as 8.28 nN/mW and a depth of trapping potential as large as 1.15×105 𝑘B𝑇 mW−1 are obtained, where 𝑘B is the Boltzmann constant and 𝑇 is the system temperature. We estimate a lateral trapping stiffness of 167.17 pN·nm−1· mW−1 for a 10 nm radius PS nanoparticle along the cavity 𝑥-axis, more than two orders of magnitude higher than previously demonstrated on-chip, near field traps. Moreover, the threshold power for stable trapping as low as 0.087 μW is achieved. In addition, trapping of a single 25 nm radius PS nanoparticle causes a 0.6 nm redshift in peak wavelength. Thus, the proposed cavity device can be used to detect single nanoparticle trapping by monitoring the resonant peak wavelength shift. We believe that the architecture with features of an ultracompact footprint, high integrability with optical waveguides/circuits, and efficient trapping demonstrated here will provide a promising candidate for developing a lab-on-a-chip device with versatile functionalities.

DOI

All-optical manipulation of micrometer-sized metallic particles

Yuquan Zhang, Xiujie Dou, Yanmeng Dai, Xianyou Wang, Changjun Min, and Xiaocong Yuan

Optical traps use focused laser beams to generate forces on targeted objects ranging in size from nanometers to micrometers. However, for their high coefficients of scattering and absorption, micrometer-sized metallic particles were deemed non-trappable in three dimensions using a single beam. This barrier is now removed. We demonstrate, both in theory and experiment, three-dimensional (3D) dynamic all-optical manipulations of micrometer-sized gold particles under high focusing conditions. The force of gravity is found to balance the positive axial optical force exerted on particles in an inverted optical tweezers system to form two trapping positions along the vertical direction. Both theoretical and experimental results confirm that stable 3D manipulations are achievable for these particles regardless of beam polarization and wavelength. The present work opens up new opportunities for a variety of in-depth research requiring metallic particles.

DOI

Optical forces of focused femtosecond laser pulses on nonlinear optical Rayleigh particles

Liping Gong, Bing Gu, Guanghao Rui, Yiping Cui, Zhuqing Zhu, and Qiwen Zhan

The principle of optical trapping is conventionally based on the interaction of optical fields with linear-induced polarizations. However, the optical force originating from the nonlinear polarization becomes significant when nonlinear optical nanoparticles are trapped by femtosecond laser pulses. Herein we develop the time-averaged optical forces on a nonlinear optical nanoparticle using high-repetition-rate femtosecond laser pulses, based on the linear and nonlinear polarization effects. We investigate the dependence of the optical forces on the magnitudes and signs of the refractive nonlinearities. It is found that the self-focusing effect enhances the trapping ability, whereas the self-defocusing effect leads to the splitting of the potential well at the focal plane and destabilizes the optical trap. Our results show good agreement with the reported experimental observations and provide theoretical support for capturing nonlinear optical particles.

DOI

Light-driven crystallization of polystyrene micro-spheres

Jing Liu and Zhi-Yuan Li

We investigate the dynamic crystallization processes of colloidal photonic crystals, which are potentially invaluable for solving a number of existing and emerging technical problems in regards to controlled fabrication of crystals, such as size normalization, stability improvement, and acceleration of synthesis. In this paper, we report systematic high-resolution optical observation of the spontaneous crystallization of monodisperse polystyrene (PS) micro-spheres in aqueous solution into close-packed arrays in a static line optical tweezers. The experiments demonstrate that the crystal structure is mainly affected by the minimum potential energy of the system; however, the crystallization dynamics could be affected by various mechanical, physical, and geometric factors. The complicated dynamic transformation process from 1D crystallization to 2D crystallization and the creation and annihilation of dislocations and defects via crystal relaxation are clearly illustrated. Two major crystal growth modes, the epitaxy growth pattern and the inserted growth pattern, have been identified to play a key role in shaping the dynamics of the 1D and 2D crystallization process. These observations offer invaluable insights for in-depth research about colloidal crystal crystallization.

DOI

Optical forces exerted on a graphene-coated dielectric particle by a focused Gaussian beam

Yang Yang, Zhe Shi, Jiafang Li, and Zhi-Yuan Li

In this paper, we derive the analytical expression for the multipole expansion coefficients of scattering and interior fields of a graphene-coated dielectric particle under the illumination of an arbitrary optical beam. By using this arbitrary beam theory, we systematically investigate the optical forces exerted on the graphene-coated particle by a focused Gaussian beam. Via tuning the chemical potential of the graphene, the optical force spectra could be modulated accordingly at resonant excitation. The hybridized whispering gallery mode of the electromagnetic field inside the graphene-coated polystyrene particle is more intensively localized than the pure polystyrene particle, which leads to a weakened morphology-dependent resonance in the optical forces. These investigations could open new perspectives for dynamic engineering of optical manipulations in optical tweezers applications.

DOI

Optical trapping and orientation of Escherichia coli cells using two tapered fiber probes

Jianbin Huang, Xiaoshuai Liu, Yao Zhang, and Baojun Li

We report on the optical trapping and orientation of Escherichia coli (E. coli) cells using two tapered fiber probes. With a laser beam at 980 nm wavelength launched into probe I, an E. coli chain consisting of three cells was formed at the tip of probe I. After launching a beam at 980 nm into probe II, the E. coli at the end of the chain was trapped and oriented via the optical torques yielded by two probes. The orientation of the E. coli was controlled by adjusting the laser power of probe II. Experimental results were interpreted by theoretical analysis and numerical simulations.

DOI

Ray-optics model for optical force and torque on a spherical metal-coated Janus microparticle

Jing Liu, Chao Zhang, Yiwu Zong, Honglian Guo, and Zhi-Yuan Li

In this paper, we develop a theoretical method based on ray optics to calculate the optical force and torque on a metallo-dielectric Janus particle in an optical trap made from a tightly focused Gaussian beam. The Janus particle is a 2.8 μm diameter polystyrene sphere half-coated with gold thin film several nanometers in thickness. The calculation result shows that the focused beam will push the Janus particle away from the center of the trap, and the equilibrium position of the Janus particle, where the optical force and torque are both zero, is located in a circular orbit surrounding the laser beam axis. The theoretical results are in good agreement qualitatively and quantitatively with our experimental observation. As the ray-optics model is simple in principle, user friendly in formalism, and cost effective in terms of computation resources and time compared with other usual rigorous electromagnetics approaches, the developed theoretical method can become an invaluable tool for understanding and designing ways to control the mechanical motion of complicated microscopic particles in various optical tweezers.

DOI

Microscopic and macroscopic manipulation of gold nanorod and its hybrid nanostructures

Jiafang Li, Honglian Guo, and Zhi-Yuan Li

Gold nanorods (GNRs) have potential applications ranging from biomedical sciences and emerging nanophotonics. In this paper, we will review some of our recent studies on both microscopic and macroscopic manipulation of GNRs. Unique properties of GNR nanoparticles, such as efficient surface plasmon amplifications effects, are introduced. The stable trapping, transferring, positioning and patterning of GNRs with nonintrusive optical tweezers will be shown. Vector beams are further employed to improve the trapping performance. On the other hand, alignment of GNRs and their hybrid nanostructures will be described by using a film stretch method, which induces the anisotropic and enhanced absorptive nonlinearities from aligned GNRs. Realization and engineering of polarized emission from aligned hybrid GNRs will be further demonstrated, with relative excitation–emission efficiency significantly enhanced. Our works presented in this review show that optical tweezers possess great potential in microscopic manipulation of metal nanoparticles and macroscopic alignment of anisotropic nanoparticles could help the macroscopic samples to flexibly represent the plasmonic properties of single nanoparticles for fast, cheap, and high-yield applications.
DOI

All-optical particle trap using orthogonally intersecting beams

K. D. Leake, A. R. Hawkins, and H. Schmidt

We analyze the properties of a dual-beam trap of orthogonally intersecting beams in the geometrical optics regime. We derive analytical expressions for the trapping location and stability criteria for trapping a microparticle with uncollimated Gaussian beams. An upper limit for the beam waist is found. Optical forces and particle trajectories are calculated numerically for the realistic case of a microparticle in intersecting liquid-core waveguides.
DOI