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The temperature distribution throughout arrays of illuminated metal nanoparticles is investigated numerically and experimentally. The two cases of continuous and femtosecond-pulsed illumination are addressed. In the case of continuous illumination, two distinct regimes are evidenced: a temperature confinement regime, where the temperature increase remains confined at the vicinity of each nanosource of heat, and a temperature delocalization regime, where the temperature is uniform throughout the whole nanoparticle assembly despite the heat sources' nanometric size. We show that the occurrence of one regime or another simply depends on the geometry of the nanoparticle distribution. In particular, we derived (i) simple expressions of dimensionless parameters aimed at predicting the degree of temperature confinement and (ii) analytical expressions aimed at estimating the actual temperature increase at the center of an assembly of nanoparticles under illumination, preventing heavy numerical simulations. All these theoretical results are supported by experimental measurements of the temperature distribution on regular arrays of gold nanoparticles under illumination. In the case of femtosecond-pulsed illumination, we explain the two conditions that must be fulfilled to observe a further enhanced temperature spatial confinement.

Self-assembled plasmonic nanoparticle networks (PNN) composed of chains of 12 nm diameter crystalline gold nanoparticles exhibit a longitudinally coupled plasmon mode centered at 700 nm. We have exploited this longitudinal absorption band to efficiently confine light fields and concentrate heat sources in the close vicinity of these plasmonic chain networks. The mapping of the two phenomena on the same superstructures was performed by combining two-photon luminescence and fluorescence polarization anisotropy imaging techniques. Besides the light and heat concentration, we show experimentally that the planar spatial distribution of optical field intensity can be simply modulated by controlling the linear polarization of the incident optical excitation. On the contrary, the heat production, which is obtained here by exciting the structures within the optically transparent window of biological tissues, is evenly spread over the entire PNN. This contrasts with the usual case of localized heating in continuous nanowires, thus opening opportunities for these networks in light-induced hyperthermia applications. Furthermore, we propose a unified theoretical framework to account for both the nonlinear optical and thermal near-fields around PNN. The associated numerical simulations, based on a Green's function formalism, are in excellent agreement with the experimental images. This formalism therefore provides a versatile tool for the accurate engineering of optical and thermodynamical properties of complex plasmonic colloidal architectures.

Using the Green’s dyadic method, we investigated numerically the heat generation in gold nanoparticles when illuminated at their plasmonic resonance. Two kinds of structures are discussed—colloidal-like nanoparticles and lithographic planar nanostructures—putting special emphasis on the influence of the object’s morphology at a constant metal volume. The mechanism of heating is explained and discussed by mapping the heating power density inside the structures. This work aims at giving an intuitive and original understanding of the relative heating efficiency of a wide set of morphologies and could stand for a basis recipe to design optimized plasmonic nanoheaters. [ABSTRACT FROM AUTHOR]