Mongin Denis, Maioli Paolo, Burgin Julien, Langot Pierre, Cottancin Emmanuel, D'Addato Sergio, Canut Bruno, Treguer Mona, Crut Aurélien, Vallée Fabrice, Del Fatti Natalia
Université de Lyon, CNRS, Université Claude Bernard Lyon 1, Institut Lumière Matière, UMR 5306, F-69622 Villeurbanne, France.
J Phys Condens Matter. 2019 Feb 27;31(8):084001. doi: 10.1088/1361-648X/aaf7eb. Epub 2019 Jan 8.
Using time-resolved ultrafast pump-probe spectroscopy we investigated the electron-lattice energy transfer in small copper nanospheres with diameters ranging from 3.2 to 23 nm, either embedded in a glass or dispersed in a solvent. Electron-lattice scattering rate is shown to increase with size reduction, in agreement with our previous results obtained on gold and silver nanoparticles in the low excitation regime. We attribute this effect to the reduction of the screening efficiency of electron-phonon interactions close to the nanoparticle surface. To understand the discrepancy between the results on the electron-lattice scattering in different metals reported in the literature (reduction, no dependence or increase with nanoparticle size), we discuss the experimental conditions required for the accurate determination of electron-lattice energy transfer time from time-resolved investigations in the weak and strong excitation regimes and present power-dependent experiments on gold nanospheres in solution. Our findings are derived from a theoretical analysis based on the two-temperature model predictions and on a complete modeling of the nanoparticle transient extinction cross-section through the resolution of Boltzmann equation in the presence of hot electrons.
我们使用时间分辨超快泵浦-探测光谱技术,研究了直径在3.2至23纳米范围内、嵌入玻璃或分散在溶剂中的小铜纳米球中的电子-晶格能量转移。结果表明,电子-晶格散射率随尺寸减小而增加,这与我们之前在低激发态下对金和银纳米颗粒获得的结果一致。我们将这种效应归因于靠近纳米颗粒表面的电子-声子相互作用屏蔽效率的降低。为了理解文献中报道的不同金属中电子-晶格散射结果之间的差异(随纳米颗粒尺寸减小、无依赖性或增加),我们讨论了在弱激发态和强激发态下通过时间分辨研究准确测定电子-晶格能量转移时间所需的实验条件,并展示了溶液中金纳米球的功率相关实验。我们的研究结果源自基于双温度模型预测的理论分析,以及通过求解存在热电子时的玻尔兹曼方程对纳米颗粒瞬态消光截面进行的完整建模。