Theory of exciton dynamics in time-resolved ARPES: intra- and intervalley scattering in two-dimensional semiconductors

Abstract

Time- and angle-resolved photoemission spectroscopy (trARPES) is a powerful spectroscopic method to measure the ultrafast electron dynamics directly in momentum-space. However, band gap materials with exceptional strong Coulomb interaction such as monolayer transition metal dichlacogenides (TMDC) exhibit tightly bound excitons, which dominate their optical properties. This rises the question whether excitons, in particular their formation and relaxation dynamics, can be detected in photoemission. Here, we develope a fully microscopic theory of the temporal dynamics of excitonic time- and angle resolved photoemission with particular focus on the phonon-mediated thermalization of optically excited excitons to momentum-forbidden dark exciton states. We find that trARPES is able to probe the ultrafast exciton formation and relaxation throughout the Brillouin zone.

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Cited by in corpus (39)

• Directly visualizing the momentum forbidden dark excitons and their dynamics in atomically thin semiconductors
• Time- and Angle-Resolved Photoemission Studies of Quantum Materials
• Exciton-Phonon Interaction and Relaxation Times from First Principles
• Theory of Exciton-Phonon Coupling
• Momentum-resolved observation of exciton formation dynamics in monolayer WS${}_2$
• Direct measurement of key exciton properties: energy, dynamics and spatial distribution of the wave function
• Exciton-Scattering-Induced Dephasing in Two-Dimensional Semiconductors
• Exciton optics, dynamics and transport in atomically thin semiconductors
• Observation of an excitonic Mott transition through ultrafast core-$\text{cum}$-conduction photoemission spectroscopy
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• Momentum-Resolved Exciton Coupling and Valley Polarization Dynamics in Monolayer WS${}_2$
• Ultrafast dynamics of bright and dark excitons in monolayer WSe${}_2$ and heterobilayer WSe${}_2$/MoS${}_2$
• Quenching of Intervalley Exchange Coupling in the Presence of Momentum-Dark States in TMDCs
• Dynamically screened vertex correction to $GW$
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• What do the two times in two-time correlation functions mean for interpreting tr-ARPES?
• Probing excitons with time-resolved momentum microscopy
• Direct visualization of hybrid excitons in van der Waals heterostructures
• Ultrafast creation and melting of nonequilibrium excitonic condensates in bulk WSe${}_2$
• Excitonic Bloch equations from first principles
• Time-domain study of coupled collective excitations in quantum materials
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