Hoeing Dominik, Schulz Florian, Mueller Niclas S, Reich Stephanie, Lange Holger
Institute for Physical Chemistry, Universität Hamburg, Martin-Luther-King Platz 6, 20146 Hamburg, Germany.
Department of Physics, Freie Universität Berlin, Arnimallee 14, 14195 Berlin, Germany.
J Chem Phys. 2020 Feb 14;152(6):064710. doi: 10.1063/1.5131696.
The excitation of dark plasmons, i.e., coupled plasmon modes with a vanishing net dipole, is expected to favor Landau damping over radiative damping. Dark plasmon excitation might, therefore, lead to an increased absorption of energy within gold nanoparticles, resulting in a strong generation of hot electrons compared to the generation via bright plasmons. We performed transient-absorption spectroscopy on gold nanoparticle films to assess the initial electronic temperature before thermalization. We observe a significant increase in the electron-phonon coupling time when dark plasmon modes are excited in these films. The results indicate an efficient energy absorption due to the suppressed radiative decay of dark plasmon modes and a subsequent energy transformation into hot electrons.
暗等离激元的激发,即具有零净偶极矩的耦合等离激元模式,预计相较于辐射阻尼更有利于朗道阻尼。因此,暗等离激元激发可能会导致金纳米颗粒内能量吸收增加,与通过亮等离激元产生相比,会强烈地产生热电子。我们对金纳米颗粒薄膜进行了瞬态吸收光谱分析,以评估热化之前的初始电子温度。我们观察到,当在这些薄膜中激发暗等离激元模式时,电子 - 声子耦合时间显著增加。结果表明,由于暗等离激元模式辐射衰减的抑制,能量吸收效率提高,随后能量转化为热电子。