First-principles approach to excitons in time-resolved and angle-resolved photoemission spectra

Abstract

We show that any {\em quasi-particle} or GW approximation to the self-energy does not capture excitonic features in time-resolved (TR) photoemission spectroscopy. In this work we put forward a first-principles approach and propose a feasible diagrammatic approximation to solve this problem. We also derive an alternative formula for the TR photocurrent which involves a single time-integral of the lesser Green's function. The diagrammatic approximation applies to the {\em relaxed} regime characterized by the presence of quasi-stationary excitons and vanishing polarization. The main distinctive feature of the theory is that the diagrams must be evaluated using {\em excited} Green's functions. As this is not standard the analytic derivation is presented in detail. The final result is an expression for the lesser Green's function in terms of quantities that can all be calculated {\em ab initio}. The validity of the proposed theory is illustrated in a one-dimensional model system with a direct gap. We discuss possible scenarios and highlight some universal features of the exciton peaks. Our results indicate that the exciton dispersion can be observed in TR {\em and} angle-resolved photoemission.

15 pages, 8 figures

References in corpus (30)

• Time-dependent transport in interacting and non-interacting mesoscopic systems
• Yambo: an \textit{ab initio} tool for excited state calculations
• Ab initio calculation of excitonic effects in the optical spectra of semiconductors
• Ultrafast Dynamics of Defect-Assisted Electron-Hole Recombination in Monolayer MoS2
• Ultrafast Optical Excitation of a Persistent Surface-State Population in the Topological Insulator Bi2Se3
• Time-Dependent Partition-Free Approach in Resonant Tunneling Systems
• Measurement of intrinsic Dirac fermion cooling on the surface of a topological insulator Bi${}_2$Se${}_3$ using time- and angle-resolved photoemission spectroscopy
• Theoretical description of time-resolved photoemission spectroscopy: application to pump-probe experiments
• Kadanoff-Baym approach to quantum transport through interacting nanoscale systems: From the transient to the steady-state regime
• Ballistic conductance of magnetic Co and Ni nanowires with ultrasoft pseudo-potentials
• Real-time Kadanoff-Baym approach to plasma oscillations in a correlated electron gas
• A real-time approach to the optical properties of solids and nano-structures: the time-dependent Bethe-Salpeter equation
• Transient excitons at metal surfaces
• Successes and Failures of Kadanoff-Baym Dynamics in Hubbard Nanoclusters
• Ultrafast photodoping and effective Fermi-Dirac distribution of the Dirac particles in Bi2Se3
• Simulating pump-probe photo-electron and absorption spectroscopy on the attosecond time-scale with time-dependent density-functional theory
• Charge dynamics in molecular junctions: Nonequilibrium Green's Function approach made fast
• First-principles nonequilibrium Green's function approach to transient photoabsorption: Application to atoms
• Non-equilibrium Bethe-Salpeter equation for transient photo-absorption spectroscopy
• Ultrafast exciton formation at the ZnO(10$\overline{\text{1}}$0) surface
• Time-dependent many-body treatment of electron-boson dynamics: application to plasmon-accompanied photoemission
• Competition between the electronic and phonon-mediated scattering channels in the out-of-equilibrium carrier dynamics of semiconductors: an ab-initio approach
• Non equilibrium optical properties in semiconductors from first--principles: a combined theoretical and experimental study of bulk silicon
• A minimal model for excitons within time-dependent density-functional theory
• Tailored pump-probe transient spectroscopy with time-dependent density-functional theory: controlling absorption spectra
• One-step theory of pump-probe photoemission
• Complete collisions approximation to the Kadanoff-Baym equation: a first--principles implementation
• Ab initio simulation of photoemission spectroscopy in solids: Plane-wave pseudopotential approach, with applications to normal-emission spectra of Cu(001) and Cu(111)
• Ultra-nonlocality in density functional theory for photo-emission spectroscopy
• One-step theory of two-photon photoemission

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