Elucidating optical field directed hierarchical self-assembly of homogenous versus heterogeneous nanoclusters with femtosecond optical tweezers

Insights into the morphology of nanoclusters would facilitate the design of nano-devices with improved optical, electrical, and magnetic responses. We have utilized optical gradient forces for the directed self-assembly of colloidal clusters using high-repetition-rate femtosecond laser pulses to delineate their structure and dynamics. We have ratified our experiments with theoretical models derived from the Langevin equation and defined the valid ranges of applicability. Our femtosecond optical tweezer-based technique characterizes the in-situ formation of hierarchical self-assembled clusters of homomers as well as heteromers by analyzing the back focal plane displacement signal. This technique is able to efficiently distinguish between nano-particles in heterogeneous clusters and is in accordance with our theory. Herein, we report results from our technique, and also develop a model to describe the mechanism of such processes where corner frequency changes. We show how the corner frequency changes enables us to recognize the structure and dynamics of the coagulation of colloidal homogeneous and heterogeneous clusters in condensed media over a broad range of nanoparticle sizes. The methods described here are advantageous, as the backscatter position-sensitive detection probes the in-situ self-assembly process while other light scattering approaches are leveraged for the characterization of isolated clusters.