Momentum-Resolved Observation of Exciton Formation Dynamics in Monolayer WS2Click to copy article linkArticle link copied!
- Robert Wallauer*Robert Wallauer*Email: [email protected]Fachbereich Physik, Philipps-Universität, Marburg 35032, GermanyMore by Robert Wallauer
- Raul Perea-CausinRaul Perea-CausinDepartment of Physics, Chalmers University of Technology, Gothenburg SE-412 96, SwedenMore by Raul Perea-Causin
- Lasse Münster
- Sarah Zajusch
- Samuel Brem
- Jens Güdde
- Katsumi TanimuraKatsumi TanimuraThe Institute of Scientific and Industrial Research, Osaka University, Osaka 5670047, JapanMore by Katsumi Tanimura
- Kai-Qiang LinKai-Qiang LinDepartment of Physics, University of Regensburg, Regensburg 93040, GermanyMore by Kai-Qiang Lin
- Rupert HuberRupert HuberDepartment of Physics, University of Regensburg, Regensburg 93040, GermanyMore by Rupert Huber
- Ermin Malic*Ermin Malic*Email: [email protected]Fachbereich Physik, Philipps-Universität, Marburg 35032, GermanyDepartment of Physics, Chalmers University of Technology, Gothenburg SE-412 96, SwedenMore by Ermin Malic
- Ulrich HöferUlrich HöferFachbereich Physik, Philipps-Universität, Marburg 35032, GermanyZentrum für Materialwissenschaften, Philipps-Universität, Marburg 35032, GermanyMore by Ulrich Höfer
Abstract

The dynamics of momentum-dark exciton formation in transition metal dichalcogenides is difficult to measure experimentally, as many momentum-indirect exciton states are not accessible to optical interband spectroscopy. Here, we combine a tunable pump, high-harmonic probe laser source with a 3D momentum imaging technique to map photoemitted electrons from monolayer WS2. This provides momentum-, energy- and time-resolved access to excited states on an ultrafast time scale. The high temporal resolution of the setup allows us to trace the early-stage exciton dynamics on its intrinsic time scale and observe the formation of a momentum-forbidden dark KΣ exciton a few tens of femtoseconds after optical excitation. By tuning the excitation energy, we manipulate the temporal evolution of the coherent excitonic polarization and observe its influence on the dark exciton formation. The experimental results are in excellent agreement with a fully microscopic theory, resolving the temporal and spectral dynamics of bright and dark excitons in WS2.
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The Altmetric Attention Score is a quantitative measure of the attention that a research article has received online. Clicking on the donut icon will load a page at altmetric.com with additional details about the score and the social media presence for the given article. Find more information on the Altmetric Attention Score and how the score is calculated.