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.

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.

The tip-enhanced Raman spectroscopy (TERS) provides a non-destructive and label-free molecular detection approach with high sensitivity due to the hotspot excited at tip apex, which depends crucially on the tip parameters. Here, we employed an Au cladded atomic force microscopy probe to investigate enhancement effect of the Au claddings, both in theories and experiments. The simulation optimized a highest enhancement with Au cladding thickness of 50 nm under given experimental condition, being consistent with the experimental results. It provides a practical guide to optimize the probes to improve the TERS sensitivity and exert potentials in further TERS applications.