Quasiparticle spectra from molecules to bulk

Abstract

A stochastic cumulant GW method is presented, allowing us to map the evolution of photoemission spectra, quasiparticle energies, lifetimes and emergence of collective excitations from molecules to bulk-like systems with up to thousands of valence electrons, including Si nanocrystals and nanoplatelet. The quasiparticle energies rise due to their coupling with collective shake-up (plasmon) excitations, and this coupling leads to significant spectral weight loss (up to 50% for the low energy states), shortening the lifetimes and shifting the spectral features to lower energy by as much as 0.6 eV. Such features are common to all the systems studied irrespective of their size and shape. For small and low dimensional systems the surface plasmon resonances affect the frequency of the collective excitation and position of the satellites.

6 pages, 4 figures

References in corpus (5)

• Band structures of plasmonic polarons
• Satellite Band Structure in Silicon Caused by Electron-Plasmon Coupling
• Real time cumulant approach for charge transfer satellites in x-ray photoemission spectra
• Dispersion and lineshape of plasmon satellites in one, two and three dimensions
• Description of quasiparticle and satellite properties via cumulant expansions of the retarded one-particle Green's function

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• Stochastic many-body perturbation theory for Moiré states in twisted bilayer phosphorene
• Efficient treatment of molecular excitations in the liquid phase environment via stochastic many-body theory
• Bethe Salpeter Equation Spectra for Very Large Systems
• Optimized Attenuated Interaction: Enabling Stochastic Bethe-Salpeter Spectra for Large Systems
• Embedding vertex corrections in GW self-energy: theory, implementation, and outlook
• Dopant levels in large nanocrystals using stochastic optimally tuned range-separated hybrid density functional theory
• Spatial Decay and Limits of Quantum Solute-Solvent Interactions
• Nonmonotonic band gap evolution in bent phosphorene nanosheets
• Tuning the range separation parameter in periodic systems