Femtosecond Thermal and Nonthermal Hot Electron Tunneling inside a Photoexcited Tunnel Junction

TL;DR

This paper investigates femtosecond laser-induced hot electron tunneling in metallic nanojunctions, revealing the nonthermal nature of hot electron dynamics and their role in ultrafast photocurrent generation.

Contribution

It provides the first real-time microscopic analysis of nonthermal and thermal hot electron tunneling in laser-excited tunnel junctions using phase-resolved THz measurements.

Findings

Nonthermal hot electron tunneling dominates ultrafast photocurrents.

Electronic temperature evolution can be probed via THz-field modulation.

Thermalized hot electrons contribute to delayed tunneling processes.

Abstract

Efficient operation of electronic nanodevices at ultrafast speeds requires understanding and control of the currents generated by femtosecond bursts of light. Ultrafast laser-induced currents in metallic nanojunctions can originate from photo-assisted hot electron tunneling or lightwave-induced tunneling. Both processes can drive localized photocurrents inside a scanning tunneling microscope (STM) on femto- to attosecond time scales, enabling ultrafast STM with atomic spatial resolution. Femtosecond laser excitation of a metallic nanojunction, however, also leads to the formation of a transient thermalized electron distribution, but the tunneling of thermalized hot electrons on time scales faster than electron-lattice equilibration is not well understood. Here, we investigate ultrafast electronic heating and transient thermionic tunneling inside a metallic photoexcited tunnel junction and its role in the generation of ultrafast photocurrents in STM. Phase-resolved sampling of broadband THz pulses via the THz-field-induced modulation of ultrafast photocurrents allows us to probe the electronic temperature evolution inside the STM tip, and to observe the competition between instantaneous and delayed tunneling due to nonthermal and thermal hot electron distributions in real time. Our results reveal the pronounced nonthermal character of photo-induced hot electron tunneling, and provide a detailed microscopic understanding of hot electron dynamics inside a laser-excited tunnel junction.