ABSTRACTOptical properties and thermal relaxation dynamics of resonantly excited plasmons are important in applications for optoelectronics, biomedicine, energy, and catalysis. Geometric optics of polydimethylsiloxane (PDMS) thin films containing uniformly or asymmetrically distributed polydisperse reduced AuNPs or uniformly distributed monodisperse solution-synthesized AuNPs were recently evaluated using a compact linear algebraic sum. Algebraic calculation of geometric transmission, reflection, and attenuation for AuNP-PDMS films provides a simple, workable alternative to effective medium approximations, computationally expensive methods, and fitting of experimental data. This approach allows for the summative optical responses of a sequence of 2D elements comprising a 3D assembly to be analyzed. Thin PDMS films containing 3-7 micron layers of reduced AuNPs were fabricated with a novel diffusive-reduction synthesis technique. Rapid diffusive reduction of AuNPs into asymmetric PDMS thin films provided superior photothermal response relative to thicker films with AuNPs reduced throughout, with a photon-to-heat conversion of up to 3000°C/watt which represents 3-230-fold increase over previous AuNP-functionalized systems. Later work showed that introduction of AuNPs into PDMS enhanced thermoplasmonic dissipation coincident with internal reflection of incident resonant irradiation. Measured thermal emission and dynamics of AuNP-PDMS thin films exceeded emission and dynamics attributable by finite element analysis to Mie absorption, Fourier heat conduction, Rayleigh convection, and Stefan-Boltzmann radiation. Refractive-index matching experiments and measured temperature profiles indicated AuNP-containing thin films internally reflected light and dissipated power transverse to the film surface. Enhanced thermoplasmonic dissipation from metal-polymer nanocomposite thin films could affect opto- and bio-electronic implementation of these systems.
