论文标题

通过Attosexond Spectroscopicy揭示局部激子的交织原子和批量性质

Unravelling the intertwined atomic and bulk nature of localised excitons by attosecond spectroscopy

论文作者

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

论文摘要

大多数半导体和技术感兴趣的绝缘子的电流特性主要由称为激子的电子孔准粒子的存在。在电介质中对这些类似氢的准粒子的操纵已获得了极大的兴趣,其名称具有兴奋性,预计在包括光电和光子学在内的各种应用中具有很大的潜力。在先进的技术应用中这种剥削激子的关键步骤是对它们的动力学性质的详细理解。然而,鉴于电子设备向Petahertz政权扩展所需的扩展,在几秒钟和attsement时尺度上展开的超快速过程仍然很大程度上尚未开发。在这里,我们将attsond瞬态反射光谱应用于顺序的两局几何形状,并观察块核级激子的子段动力学,该动力学在块状MGF $ _2 $单晶中。借助我们唯一的设置,我们可以访问绝对相位延迟,从而可以与基于Wannier-Mott模型的理论计算进行明确的比较。我们的结果表明,激烈的表现出双重原子和坚固的特征,它在不同的时间尺度上表现出来。虽然前者负责飞秒的光学鲜明效应,但后者占主导地位的激子反应,并由与晶体的相互作用来源。对激子定位的作用的进一步研究证明,批量特征也持续到强烈局部的准粒子,并使我们能够设想一条新的途径来控制近距离佩特赫兹策略中的激子动力学。

The electro-optical properties of most semiconductors and insulators of technological interest are dominated by the presence of electron-hole quasiparticles called excitons. The manipulation of these hydrogen-like quasi-particles in dielectrics, has received great interest under the name excitonics that is expected to be of great potential for a variety of applications, including optoelectronics and photonics. A crucial step for such exploitation of excitons in advanced technological applications is a detailed understanding of their dynamical nature. However, the ultrafast processes unfolding on few-femtosecond and attosecond time scales, of primary relevance in view of the desired extension of electronic devices towards the petahertz regime, remain largely unexplored. 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$_2$ single crystals. With our unique setup, we can access absolute phase delays which allow for an unambiguous comparison with theoretical calculations based on the Wannier-Mott model. 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 and originates by the interaction with the crystal. Further investigation of the role of exciton localization proves that the bulk character persists also for strongly localised quasi-particles and allows us to envision a new route to control exciton dynamics in the close-to-petahertz regime.

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