We postulate that the oscillations originate from temperature-dependent changes in the buoyancy of the dispersion, leading to organized convective flows. We observed oscillations in the extinction intensity at ∼523 nm corresponding to the extinction of AuSs (see Figure ). This observation hints at the possibility of the oscillations originating from hydrodynamic flows, changing the amount of NPs in the UV-Vis-NIR probe volume. Notably, we observed a coloured chemical hydrodynamic wave-like pattern in the solution, providing additional evidence for the hydrodynamic origins of the oscillations (see the optical image in Figure ). This hydrodynamic wave-like pattern is produced by the convective motion of the solvent dragging with itself, the NP mixture. Similar flow-based oscillations have been shown in the literature, but they require higher sample volume and a need for a volatile solvent to establish a strong enough temperature gradient for observing oscillations. The distinct benefit of using plasmonic NPs is their ability to establish potent enough temperature gradients even at 200 µL solutions, compared to 3 mL volumes required in earlier pioneering works. To induce oscillation, the following critical parameters were established: temperature gradient, thermoresponsiveness and feedback loop asymmetry. We confirmed these parameters through a series of negative control experiments which led to stationary, non-oscillatory responses. First, no oscillation was observed for CTAB-coated AuNRs instead of DNA (see Figure ). Second, the use of unary building blocks either AuSs or AuNRs generated a stationary state that was attributed to poor photothermal heating (in the case of AuSs) (Figure ), or negligible redshifts in the extinction spectrum upon assembly (in the case of AuNRs) (Figure ). Third, using a laser wavelength of 670 nm failed to generate oscillatory dynamics that is due to its inability to induce asymmetry in the system since both unassembled and assembled states possess similar extinction. These experiments underscore and reiterate the critical need for thermoresponsive assembly, as well as the significant increase in extinction at the laser illumination during the assembly, as essential components for obtaining the oscillating response. Finally, we ruled out the contribution of reversible assembly/disassembly of NPs to oscillatory features. The LSPR shift is a signature of decreased interparticle distance that increases plasmon coupling and thereby controls the photothermal effect. In the present case, the LSPR shifts at the λmax was negligible throughout the oscillations (see Figure ).