Distinct Optical Magnetism in Gold and Silver Probed by Dynamic Metamolecules

Abstract

Here, we report plasmonic metamolecules with dynamically controllable optical magnetism. A dynamic meta-molecule (DMM) is constructed by decorating gold or silver nanobeads on a thermoresponsive poly(N-isopropylacrylamide) (PNIPAM) hydrogel sphere, which generates uniform coresatellite-type assembly structures with an interbead distance, allowing for strong interparticle coupling. Experimental and simulation results revealed strong magnetic dipole and quadrupole modes observable in the far field both for gold and silver DMMs when the temperature was set above the lower critical solution temperature (LCST) of PNIPAM. Interestingly, gold DMMs showed stronger and more pronounced magnetic resonances than silver DMMs, despite the general notion that silver nanostructures possess superior plasmonic properties. The strong magnetic coupling and structural uniformity along with the ability to dynamically control the assembly structure allowed us to probe distinct optical magnetism in gold and silver and experimentally observe magnetic quadrupole in solution-phase metamolecules for the first time.