Formation of moir\'e interlayer excitons in space and time

TL;DR

This study uses femtosecond photoemission microscopy to directly observe the ultrafast formation and wavefunction confinement of moiré interlayer excitons in van-der-Waals heterostructures, revealing their dynamics in space and time.

Contribution

It provides the first direct experimental measurement of the formation dynamics and real-space wavefunction modulation of moiré interlayer excitons.

Findings

Interlayer excitons form within 50 fs via tunneling at K valleys.

Momentum microscopy maps exciton signatures in the mini Brillouin zone.

Wavefunction confinement modulated by moiré potential is quantitatively measured.

Abstract

Moir\'e superlattices in atomically thin van-der-Waals heterostructures hold great promise for an extended control of electronic and valleytronic lifetimes, the confinement of excitons in artificial moir\'e lattices, and the formation of novel exotic quantum phases. Such moir\'e-induced emergent phenomena are particularly strong for interlayer excitons, where the hole and the electron are localized in different layers of the heterostructure. In order to exploit the full potential of correlated moir\'e and exciton physics, a thorough understanding of the ultrafast interlayer exciton formation process and the real-space wavefunction confinement in the moir\'e potential is indispensable. However, direct experimental access to these parameters is limited since most excitonic quasiparticles are optically dark. Here we show that femtosecond photoemission momentum microscopy provides quantitative access to these key properties of the moir\'e interlayer excitons. We find that interlayer excitons are dominantly formed on the sub-50~fs timescale via interlayer tunneling at the K valleys of the Brillouin zones. In addition, we directly measure energy-momentum fingerprints of the moir\'e interlayer excitons by mapping their spectral signatures within the mini Brillouin zone that is built up by the twisted heterostructure. From these momentum-fingerprints, we gain quantitative access to the modulation of the exciton wavefunction within the moir\'e potential in real-space. Our work provides the first direct access to the interlayer moir\'e exciton formation dynamics in space and time and reveals new opportunities to study correlated moir\'e and exciton physics for the future realization of exotic quantum phases of matter.