Ab-initio density-matrix approach to exciton coherence: phonon scattering, Coulomb interactions and radiative recombination
Fuente:
arXiv
Saved in:
| Main Authors: | , , , |
|---|---|
| Format: | Preprint |
| Published: |
2025
|
| Subjects: | |
| Online Access: | |
| Tags: |
Add Tag
No Tags, Be the first to tag this record!
|
| _version_ | 1866908360016658432 |
|---|---|
| author | Amit, Tomer Vosco, Guy Del Ben, Mauro Refaely-Abramson, Sivan |
| author_facet | Amit, Tomer Vosco, Guy Del Ben, Mauro Refaely-Abramson, Sivan |
| contents | Relaxation processes following light excitation in semiconductors are key in materials-based quantum technology applications. These processes are broadly studied in atomically thin transition metal dichalcogenides (TMDs), quasi-two-dimensional excitonic semiconductors in which atomistic design allows for tunable excited-state properties, such as relaxation lifetimes and photo-induced coherence. In this work, we present a density-matrix-based approach to compute exciton relaxation within a many-body ab initio perspective. We expand our previously developed Lindblad density-matrix formalism to capture multi-channel electron-hole pair relaxation processes, including phonon and Coulomb scattering as well as radiative recombination, and study their effect on the time-resolved excited-state propagation. Using monolayer MoSe$_2$ as a prototypical example, we examine many-body effects on the time-dependent dynamics of photoactive excitations, exploring how the electron-hole pair interactions are reflected in variations of the excitation energy, spectral signature, and state coherence. Our method supplies a detailed understanding of exciton relaxation mechanisms in realistic materials, offering a previously unexplored pathway to study excited-state dynamics in semiconductors from first principles. |
| format | Preprint |
| id |
arxiv_https___arxiv_org_abs_2505_07021 |
| institution | arXiv |
| publishDate | 2025 |
| record_format | arxiv |
| spellingShingle | Ab-initio density-matrix approach to exciton coherence: phonon scattering, Coulomb interactions and radiative recombination Amit, Tomer Vosco, Guy Del Ben, Mauro Refaely-Abramson, Sivan Materials Science Relaxation processes following light excitation in semiconductors are key in materials-based quantum technology applications. These processes are broadly studied in atomically thin transition metal dichalcogenides (TMDs), quasi-two-dimensional excitonic semiconductors in which atomistic design allows for tunable excited-state properties, such as relaxation lifetimes and photo-induced coherence. In this work, we present a density-matrix-based approach to compute exciton relaxation within a many-body ab initio perspective. We expand our previously developed Lindblad density-matrix formalism to capture multi-channel electron-hole pair relaxation processes, including phonon and Coulomb scattering as well as radiative recombination, and study their effect on the time-resolved excited-state propagation. Using monolayer MoSe$_2$ as a prototypical example, we examine many-body effects on the time-dependent dynamics of photoactive excitations, exploring how the electron-hole pair interactions are reflected in variations of the excitation energy, spectral signature, and state coherence. Our method supplies a detailed understanding of exciton relaxation mechanisms in realistic materials, offering a previously unexplored pathway to study excited-state dynamics in semiconductors from first principles. |
| title | Ab-initio density-matrix approach to exciton coherence: phonon scattering, Coulomb interactions and radiative recombination |
| topic | Materials Science |
| url | https://arxiv.org/abs/2505.07021 |