Formation of moiré interlayer excitons in space and time

Abstract

Moiré 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 moiré lattices, and the formation of novel exotic quantum phases. Such moiré-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 moiré and exciton physics, a thorough understanding of the ultrafast interlayer exciton formation process and the real-space wavefunction confinement in the moiré 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 moiré 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 moiré 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 moiré potential in real-space. Our work provides the first direct access to the interlayer moiré exciton formation dynamics in space and time and reveals new opportunities to study correlated moiré and exciton physics for the future realization of exotic quantum phases of matter.

arXiv comment7 pages main text, 11 pages SI

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• Spin- and time-resolved photoelectron spectroscopy and diffraction studies using time-of-flight momentum microscopes
• Interlayer exciton polaritons in homobilayers of transition metal dichalcogenides