Single-Nanoparticle Dynamics in Opto-Thermal Tweezers: Resolving the Temporal Resolution of Depletion Force Trapping.

Optothermal tweezers enable the manipulation of a wide range of nano-objects through optically induced depletion forces. Despite significant advances, the temporal dynamics of optothermal trapping remain elusive as existing methodologies rely almost exclusively on time and ensemble averaging. Consequently, stable trapping cannot be distinguished from local transient accumulation, where the time-averaged concentration increases, but particles exhibit rapid, dynamic motion in and out of the trap. Here, we investigate optothermal trapping with single-nanoparticle-level analysis and submillisecond temporal resolution. Our data resolve the elusive dynamics of 40 nm polystyrene nanoparticles trapped within depletion force potentials in polyethylene glycol solutions, enabling us to differentiate the conditions leading to extended trapping times from those leading to transient localization. Numerical simulations corroborate our experimental findings, elucidating how the interplay between thermophoresis and diffusiophoresis governs nanoparticle dynamics. These insights deepen our mechanistic understanding of optothermal trapping and unlock opportunities for single-molecule studies, nanoscale assembly, and targeted drug delivery.