Emergent Relativistic Effects in Condensed Matter
From Fundamental Aspects to Electronic Functionality

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08.04.2019

Ultrafast transition between exciton phases in van der Waals heterostructures


P. Merkl, F. Mooshammer, P. Steinleitner, A. Girnghuber, K.-Q. Lin, P. Nagler, J. Holler, C. Schüller,
J. M. Lupton, T. Korn, S. Ovesen, S. Brem, E. Malic, R. Huber

Nature Materials

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 moiré-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, where phase-locked mid- infrared pulses allow us to measure the binding energy of interlayer excitons in WSe 2 /WS 2 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 WSe 2 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.

 

https://www.nature.com/nmat/volumes/18/issues/7
https://www.nature.com/articles/s41563-019-0337-0

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