Non-Fourier heat transport in metal-dielectric core-shell nanoparticles under ultrafast laser pulse excitation

Relaxation dynamics of embedded metal nanoparticles after ultrafast laser pulse excitation is driven by thermal phenomena of different origins the accurate description of which is crucial for interpreting experimental results: hot electron gas generation, electron-phonon coupling, heat transfer to the particle environment and heat propagation in the latter. Regardingthis last mechanism, it is well known that heat transport in nanoscale structures and/or at ultrashort timescales may deviate from the predictions of the Fourier law. In these cases heat transport may rather be described by the Boltzmann transport equation. We present a numerical model allowing us to determine the electron and lattice temperature dynamics in a spherical gold nanoparticle core under subpicosecond pulsed excitation, as well as that of the surrounding shell dielectric medium. For this, we have used the electron-phonon coupling equation in the particle with a source term linked with the laser pulse absorption, and the ballistic-diffusive equations for heat conduction in the host medium. Either thermalizing or adiabatic boundary conditions have been considered at the shell external surface. Our results show that the heat transfer rate from the particle to the matrix can be significantly smaller than the prediction of Fourier's law. Consequently, the particle temperature rise is larger and its cooling dynamics might be slower than that obtained by using Fourier's law. This difference is attributed to the nonlocal and nonequilibrium heat conduction in the vicinity of the core nanoparticle. These results are expected to be of great importance for analyzing pump-probe experiments performed on single nanoparticles or nanocomposite media

Influence of Interface Thermal Resistance on Relaxation Dynamics of Metal-Dielectric Nanocomposite Materials under Ultrafast Pulse Laser Excitation

Nanocomposite materials, including noble metal nanoparticles embedded in a dielectric host medium, are interesting because of their optical properties linked to surface plasmon resonance phenomena. For studding of nonlinear optical properties and/or energy transfer process, these materials may be excited by ultrashort pulse laser with a temporal width varying from some femtoseconds to some hundreds of picoseconds. Following of absorption of light energy by metal-dielectric nanocomposite material, metal nanoparticles are heated. Then, the thermal energy is transferred to the host medium through particle-dielectric interface. On the one hand, nonlinear optical properties of such materials depend on their thermal responses to laser pulse, and on the other hand different parameters, such as pulse laser and medium thermodynamic characterizes, govern on the thermal responses of medium to laser pulse. Here, influence of thermal resistance at particle-surrounding medium interface on thermal response of such material under ultrashort pulse laser excitation is investigated. For this, we used three temperature model based on energy exchange between different bodies of medium. The results show that the interface thermal resistance plays a crucial role on nanoparticle cooling dynamics, so that the relaxation characterized time increases by increasing of interface thermal resistance

Counterintuitive thermo-optical response of metal-dielectric nanocomposite materials as a result of local electromagnetic field enhancement

International audienc

Thermo-optical effects of surface plasmons

Surface plasmon resonance sensors have been widely considered due to their sensitivity, accuracy and response speed. In order to stimulate surface plasmons, a crisman structure is used in which the metal layer (mainly gold or silver) is placed on the surface of the prism. Due to temperature changes, various factors such as optical properties of the metal, the prism and the surrounding environment can change, which can, in turn, change the response of the plasmonic sensors. In this paper, the thermal effects on the optical response of a surface plasmon resonance sensor were  theoretically evaluated. The results showed  that the change in temperature led  to significant changes in the reflectivity and phase. The greatest effect was due to the  changes in the optical properties of the metal layer (gold here) due to temperature changes

Influence of laser pulse characteristics on the hot electron contribution to the third-order nonlinear optical response of gold nanoparticles

International audienc

Optimizing performance of plasmonic devices for photonic circuits

We demonstrate the feasibility of fabricating thermo-optic plasmonic devices for variable optical attenuation and/or low-frequency (kHz) signal modulation. Results of finite-element simulations and experimental characterization of prototype devices indicate that a plasmonic device can reach specifications similar to or better than commercially available thermo-optic integrated optical components. Specifically, we have considered the insertion loss, power consumption, footprint, polarization-dependent loss, extinction ratio, and frequency response of the plasmonic devices, in addition to fabrication and material-related issues. The most serious fabrication challenge is to realize metallic nanowire waveguides with a sufficiently accurate cross-section to ensure low polarization-dependent loss at high extinction ratios