Real-time GW: Toward an ab initio description of the ultrafast carrier and exciton dynamics in two-dimensional materials

Abstract

We demonstrate the feasibility of the time-linear scaling formulation of the $GW$ method [Phys. Rev. Lett. {\bf 124}, 076601 (2020)] for {\it ab initio} simulations of optically driven two-dimensional materials. The time-dependent $GW$ equations are derived and solved numerically in the basis of Bloch states. We address carrier multiplication and relaxation in photo-excited graphene and find deviations from the typical exponential behavior predicted by the Markovian Boltzmann approach. For resonantly pumped semiconductor we discover a self-sustained screening cascade leading to the Mott transition of coherent excitons. Our results draw attention to the importance of non-Markovian and dynamical screening effects in out-of-equilibrium phenomena.

6 pages, 4 figures

References in corpus (12)

• The electronic properties of graphene
• Dielectric function, screening, and plasmons in 2D graphene
• Photo-excitation Cascade and Multiple Carrier Generation in Graphene
• The GW compendium: A practical guide to theoretical photoemission spectroscopy
• Excitons versus electron-hole plasma in monolayer transition metal dichalcogenide semiconductors
• Electron-Hole Generation and Recombination Rates for Coulomb Scattering in Graphene
• Inelastic carrier lifetime in graphene
• Photo-excited Carrier Dynamics and Impact Excitation Cascade in Graphene
• Dynamically screened vertex correction to $GW$
• Photoinduced dynamics of organic molecules using nonequilibrium Green's functions with second-Born, $GW$, $T$-matrix and three-particle ladder correlations
• From carriers and virtual excitons to exciton populations: Insights into time-resolved ARPES spectra from an exactly solvable model
• Photo-induced Dirac cone flattening in BaNiS${}_2$

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