Ultrafast transition between exciton phases in van der Waals heterostructures

TL;DR

This study demonstrates ultrafast measurement of Coulomb correlations and exciton phase transitions in van der Waals heterostructures, revealing dynamic formation and transformation of interlayer excitons with potential for optoelectronic applications.

Contribution

It introduces a novel ultrafast spectroscopy technique to directly measure interlayer exciton binding energies and track their phase transitions in real time.

Findings

Measured interlayer exciton binding energy via 1s-2p resonance.

Observed ultrafast transformation from exciton gas to interlayer excitons.

Demonstrated stacking angle influences exciton coexistence and resonance renormalization.

Abstract

Heterostructures of atomically thin van der Waals bonded monolayers have opened a unique platform to engineer Coulomb correlations, shaping excitonic, Mott insulating, or superconducting phases. In transition metal dichalcogenide heterostructures, electrons and holes residing in different monolayers can bind into spatially indirect excitons with a strong potential for optoelectronics, valleytronics, Bose condensation, superfluidity, and moir\'e-induced nanodot lattices. Yet these ideas require a microscopic understanding of the formation, dissociation, and thermalization dynamics of correlations including ultrafast phase transitions. Here we introduce a direct ultrafast access to Coulomb correlations between monolayers; phase-locked mid-infrared pulses allow us to measure the binding energy of interlayer excitons in WSe2/WS2 hetero-bilayers by revealing a novel 1s-2p resonance, explained by a fully quantum mechanical model. Furthermore, we trace, with subcycle time resolution, the transformation of an exciton gas photogenerated in the WSe2 layer directly into interlayer excitons. Depending on the stacking angle, intra- and interlayer species coexist on picosecond scales and the 1s-2p resonance becomes renormalized. Our work provides a direct measurement of the binding energy of interlayer excitons and opens the possibility to trace and control correlations in novel artificial materials.