Weak-to-Strong Light-Matter Coupling and Dissipative Dynamics from First Principles
Fuente:
arXiv
Salvato in:
| Autori principali: | , , , |
|---|---|
| Natura: | Preprint |
| Pubblicazione: |
2020
|
| Soggetti: | |
| Accesso online: | |
| Tags: |
Aggiungi Tag
Nessun Tag, puoi essere il primo ad aggiungerne!!
|
| _version_ | 1866929389280690176 |
|---|---|
| author | Wang, Derek S. Neuman, Tomáš Flick, Johannes Narang, Prineha |
| author_facet | Wang, Derek S. Neuman, Tomáš Flick, Johannes Narang, Prineha |
| contents | Cavity-mediated light-matter coupling can dramatically alter opto-electronic and physico-chemical properties of a molecule. Ab initio theoretical predictions of these systems need to combine non-perturbative, many-body electronic structure theory-based methods with cavity quantum electrodynamics and theories of open quantum systems. Here we generalize quantum-electrodynamical density functional theory to account for dissipative dynamics and describe coupled cavity-molecule interactions in the weak-to-strong-coupling regimes. Specifically, to establish this generalized technique, we study excited-state dynamics and spectral responses of benzene and toluene under weak-to-strong light-matter coupling. By tuning the coupling we achieve cavity-mediated energy transfer between electronic excited states. This generalized ab initio quantum-electrodynamical density functional theory treatment can be naturally extended to describe cavity-mediated interactions in arbitrary electromagnetic environments, accessing correlated light-matter observables and thereby closing the gap between electronic structure theory and quantum optics. |
| format | Preprint |
| id |
arxiv_https___arxiv_org_abs_2002_10461 |
| institution | arXiv |
| publishDate | 2020 |
| record_format | arxiv |
| spellingShingle | Weak-to-Strong Light-Matter Coupling and Dissipative Dynamics from First Principles Wang, Derek S. Neuman, Tomáš Flick, Johannes Narang, Prineha Quantum Physics Chemical Physics Computational Physics Optics Cavity-mediated light-matter coupling can dramatically alter opto-electronic and physico-chemical properties of a molecule. Ab initio theoretical predictions of these systems need to combine non-perturbative, many-body electronic structure theory-based methods with cavity quantum electrodynamics and theories of open quantum systems. Here we generalize quantum-electrodynamical density functional theory to account for dissipative dynamics and describe coupled cavity-molecule interactions in the weak-to-strong-coupling regimes. Specifically, to establish this generalized technique, we study excited-state dynamics and spectral responses of benzene and toluene under weak-to-strong light-matter coupling. By tuning the coupling we achieve cavity-mediated energy transfer between electronic excited states. This generalized ab initio quantum-electrodynamical density functional theory treatment can be naturally extended to describe cavity-mediated interactions in arbitrary electromagnetic environments, accessing correlated light-matter observables and thereby closing the gap between electronic structure theory and quantum optics. |
| title | Weak-to-Strong Light-Matter Coupling and Dissipative Dynamics from First Principles |
| topic | Quantum Physics Chemical Physics Computational Physics Optics |
| url | https://arxiv.org/abs/2002.10461 |