Quantitative Study of the Nonlinearly Enhanced Photoacoustic/Photothermal Effect by Strong LSPR-Coupled Nanoassemblies.

The extensive exploration of the collective optical and thermal effects for localized surface plasmon resonance (LSPR)-coupled nanoassemblies has propelled much recent research and development in fields of photoacoustic (PA) imaging and photothermal (PT) therapy, while the rational design and proper engineering of these assemblies under quantitative guidance is still a highly challenging task. In this work, by utilizing the finite element analysis (FEA) method and taking gold nanochains as example, the authors quantitatively studied the coupling optical/thermal response of the nanoassemblies and the associated nonlinearly enhanced PA/PT effect. Results show that compared with their individuals, the strong electromagnetic/thermal coupling between the individuals of the nanoassemblies results in a several-time enhancement of the per-particle-weighted optical absorption, consequential thermal field enhancement, and initial PA pressure, resulting in nonlinearly amplified energy conversion from incident light to heat and PA waves. The dependence of the nonlinear PA/PT enhancement on the assembly chain length, the size of the individuals, the interparticle distance, and the size uniformity of the building blocks is quantitatively discussed. PA experiments on gold nanochains and gold nanospheres are performed to validate the proposition, and the experiments well silhouetted the theoretical discussion. This work paves the way for the rational construction and optimization of plasmonic nanoassemblies with improved PA/PT conversion efficiency.