Ultrafast Hidden Spin Polarization Dynamics of Bright and Dark Excitons in <mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML" display="inline"><mml:mrow><mml:mn>2</mml:mn><mml:mi mathvariant="normal">H</mml:mi><mml:mtext>−</mml:mtext><mml:msub><mml:mrow><mml:mi>WSe</mml:mi></mml:mrow><mml:mrow><mml:mn>2</mml:mn></mml:mrow></mml:msub></mml:mrow></mml:math>
Mauro Fanciulli, David Bresteau, J. Gaudin, Shuo Dong, Romain Géneaux, Thierry Ruchon, O. Tcherbakoff, J. Minář, O. Heckmann, Christine Richter, K. Hricovíni, Samuel Beaulieu
Abstract
We performed spin-, time- and angle-resolved extreme ultraviolet photoemission spectroscopy of excitons prepared by photoexcitation of inversion-symmetric 2H-WSe_{2} with circularly polarized light. The very short probing depth of XUV photoemission permits selective measurement of photoelectrons originating from the top-most WSe_{2} layer, allowing for direct measurement of hidden spin polarization of bright and momentum-forbidden dark excitons. Our results reveal efficient chiroptical control of bright excitons' hidden spin polarization. Following optical photoexcitation, intervalley scattering between nonequivalent K-K^{'} valleys leads to a decay of bright excitons' hidden spin polarization. Conversely, the ultrafast formation of momentum-forbidden dark excitons acts as a local spin polarization reservoir, which could be used for spin injection in van der Waals heterostructures involving multilayer transition metal dichalcogenides.