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

TL;DR

This study uses attosecond spectroscopy to reveal the dual atomic and solid-like nature of excitons in MgF2, providing insights into their ultrafast dynamics crucial for future optoelectronic applications.

Contribution

It demonstrates the first direct observation of sub-femtosecond exciton dynamics and distinguishes their atomic and bulk characteristics using phase-resolved attosecond spectroscopy.

Findings

Excitons exhibit both atomic-like and solid-like behaviors on different time scales.

Attosecond transient reflection spectroscopy can resolve ultrafast exciton responses.

Bulk exciton character persists even in strongly localized quasi-particles.

Abstract

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.