Contributor info: Prof. Gianluca Stefanucci

Gianluca Stefanucci, Enrico Perfetto

SciPost Phys. 18, 009 (2025) · published 9 January 2025 | Toggle abstract · pdf

The ultrafast conversion of coherent excitons into incoherent excitons, as well as the subsequent exciton diffusion and thermalization, are central topics in current scientific research due to their relevance in optoelectronics, photovoltaics and photocatalysis. Current approaches to the exciton dynamics rely on model Hamiltonians that depend on already screened electron-electron and electron-phonon couplings. In this work, we subject the state-of-the-art methods to scrutiny using the ab initio Hamiltonian for electrons and phonons. We offer a rigorous and intuitive proof demonstrating that the exciton dynamics governed by model Hamiltonians is affected by an overscreening of the electron-phonon interaction. The introduction of an auxiliary exciton species, termed the irreducible exciton, enables us to formulate a theory free from overscreening and derive the excitonic Bloch equations. These equations describe the time-evolution of coherent, irreducible, and incoherent excitons during and after the optical excitation. They are applicable beyond the linear regime, and predict that the total number of excitons is preserved when the external fields are switched off.

Gianluca Stefanucci, Enrico Perfetto

SciPost Phys. 16, 073 (2024) · published 13 March 2024 | Toggle abstract · pdf

Starting from the ab initio many-body theory of electrons and phonons, we go through a series of well defined simplifications to derive a set of coupled equations of motion for the electronic occupations and polarizations, nuclear displacements as well as phononic occupations and coherences. These are the semiconductor electron-phonon equations (SEPE), sharing the same scaling with system size and propagation time as the Boltzmann equations. At the core of the SEPE is the mirrored Generalized Kadanoff-Baym Ansatz (GKBA) for the Green's functions, an alternative to the standard GKBA which we show to lead to unstable equilibrium states. The SEPE treat coherent and incoherent degrees of freedom on equal footing, widen the scope of the semiconductor Bloch equations and Boltzmann equations, and reduce to them under additional simplifications. The new features of the SEPE pave the way for first-principles studies of phonon squeezed states and coherence effects in time-resolved absorption and diffraction experiments.