Lucchini Matteo, Sato Shunsuke A, Lucarelli Giacinto D, Moio Bruno, Inzani Giacomo, Borrego-Varillas Rocío, Frassetto Fabio, Poletto Luca, Hübener Hannes, De Giovannini Umberto, Rubio Angel, Nisoli Mauro
Department of Physics, Politecnico di Milano, 20133, Milano, Italy.
Institute for Photonics and Nanotechnologies, IFN-CNR, 20133, Milano, Italy.
Nat Commun. 2021 Feb 15;12(1):1021. doi: 10.1038/s41467-021-21345-7.
The electro-optical properties of most semiconductors and insulators of technological interest are dominated by the presence of electron-hole quasi-particles, called excitons. The manipulation of excitons in dielectrics has recently received great attention, with possible applications in different fields including optoelectronics and photonics. Here, we apply attosecond transient reflection spectroscopy in a sequential two-foci geometry and observe sub-femtosecond dynamics of a core-level exciton in bulk MgF single crystals. Furthermore, we access absolute phase delays, which allow for an unambiguous comparison with theoretical calculations. Our results show that excitons surprisingly exhibit a dual atomic- and solid-like character, which manifests itself on different time scales. While the former is responsible for a femtosecond optical Stark effect, the latter dominates the attosecond excitonic response. Further theoretical investigation reveals a link with the exciton sub-femtosecond nanometric motion and allows us to envision a new route to control exciton dynamics in the close-to-petahertz regime.
大多数具有技术应用价值的半导体和绝缘体的电光特性由电子 - 空穴准粒子(称为激子)主导。近年来,电介质中激子的操控受到了广泛关注,有望应用于包括光电子学和光子学在内的不同领域。在此,我们采用序列双焦点几何结构的阿秒瞬态反射光谱技术,观测了块状MgF单晶中芯能级激子的亚飞秒动力学过程。此外,我们还获得了绝对相位延迟,这使得我们能够与理论计算进行明确的比较。我们的结果表明,激子令人惊讶地呈现出原子和固体双重特性,这在不同的时间尺度上表现出来。前者导致了飞秒级的光学斯塔克效应,而后者则主导了阿秒级的激子响应。进一步的理论研究揭示了与激子亚飞秒纳米级运动的联系,并使我们能够设想在接近拍赫兹频率范围内控制激子动力学的新途径。