Optical tweezers have proved to be a powerful tool with a wide range of applications. The gradient force plays a vital role in the stable optical trapping of nano-objects. The scalar method is convenient and effective for analyzing the gradient force in traditional optical trapping. However, when the third-order nonlinear effect of the nano-object is stimulated, the scalar method cannot adequately present the optical response of the metal nanoparticle to the external optical field. Here, we propose a theoretical model to interpret the nonlinear gradient force using the vector method. By combining the optical Kerr effect, the polarizability vector of the metallic nanoparticle is derived. A quantitative analysis is obtained for the gradient force as well as for the optical potential well. The vector method yields better agreement with reported experimental observations. We suggest that this method could lead to a deeper understanding of the physics relevant to nonlinear optical trapping and binding phenomena.

Stable optical trapping of gold nanoparticles is essential and desirable because of its wide applications in nanotechnology. While several factors have been proposed to affect optical trapping stability, the sample's volume fraction during optical trapping has often been neglected. To address this, by utilizing the effective medium theory, we analyze the stability of optical trapping of a gold nanoparticle in human serum albumin solutions, HIV-1,virus solutions, and gold nanoparticle solutions in this article. Our comparative analysis of the optical force and potential on a single gold nanoparticle in solutions of varying volume fractions reveals that both parameters decrease with increasing volume fraction. This finding can aid in more effective control of gold nanoparticles in various applications.

Nonlinear responses of nanoparticles induce enlightening phenomena in optical tweezers. With the gradual increase in optical intensity, effects from saturable absorption (SA) and reverse SA (RSA) arise in sequence and thereby modulate the nonlinear properties of materials. In current nonlinear optical traps, however, the underlying physical mechanism is mainly confined within the SA regime because threshold values required to excite the RSA regime are extremely high. Herein, we demonstrate, both in theory and experiment, nonlinear optical tweezing within the RSA regime, proving that a fascinating composite trapping state is achievable at ultrahigh intensities through an optical force reversal induced through nonlinear absorption. Integrated results help in perfecting the nonlinear optical trapping system, thereby providing beneficial guidance for wider applications of nonlinear optics.

Single molecule detection and analysis play important roles in many current biomedical researches. The deep-nanoscale hotspots, being excited and confined in a plasmonic nanocavity, make it possible to simultaneously enhance the nonlinear light-matter interactions and molecular Raman scattering for label-free detections. Here, we theoretically show that a nanocavity formed in a tip-enhanced Raman scattering (TERS) system can also achieve valid optical trapping as well as TERS signal detection for a single molecule. In addition, the nonlinear responses of metallic tip and substrate film can change their intrinsic physical properties, leading to the modulation of the optical trapping force and the TERS signal. The results demonstrate a new degree of freedom brought by the nonlinearity for effectively modulating the optical trapping and Raman detection in single molecule level. This proposed platform also shows a great potential in various fields of research that need high-precision surface imaging.