The Optical Signatures of Stochastic Processes in Many-Body Exciton Scattering
- PMID: 36854178
- DOI: 10.1146/annurev-physchem-102822-100922
The Optical Signatures of Stochastic Processes in Many-Body Exciton Scattering
Abstract
We review our recent quantum stochastic model for spectroscopic lineshapes in the presence of a coevolving and nonstationary background population of excitations. Starting from a field theory description for interacting bosonic excitons, we derive a reduced model whereby optical excitons are coupled to an incoherent background via scattering as mediated by their screened Coulomb coupling. The Heisenberg equations of motion for the optical excitons are then driven by an auxiliary stochastic population variable, which we take to be the solution of an Ornstein-Uhlenbeck process. Here, we present an overview of the theoretical techniques we have developed as applied to predicting coherent nonlinear spectroscopic signals. We show how direct (Coulomb) and exchange coupling to the bath give rise to distinct spectral signatures and discuss mathematical limits on inverting spectral signatures to extract the background density of states.
Keywords: coherent nonlinear spectroscopy; excitation-induced dephasing; many-body effects in quantum dynamics; quantum stochastic calculus.
Similar articles
-
Stochastic scattering theory for excitation-induced dephasing: Comparison to the Anderson-Kubo lineshape.J Chem Phys. 2020 Oct 21;153(15):154115. doi: 10.1063/5.0026467. J Chem Phys. 2020. PMID: 33092361
-
Stochastic scattering theory for excitation-induced dephasing: Time-dependent nonlinear coherent exciton lineshapes.J Chem Phys. 2020 Oct 28;153(16):164706. doi: 10.1063/5.0026351. J Chem Phys. 2020. PMID: 33138398
-
Many-Exciton Quantum Dynamics in a Ruddlesden-Popper Tin Iodide.J Phys Chem C Nanomater Interfaces. 2023 Oct 25;127(43):21194-21203. doi: 10.1021/acs.jpcc.3c04896. eCollection 2023 Nov 2. J Phys Chem C Nanomater Interfaces. 2023. PMID: 37937156 Free PMC article.
-
Exciton-Scattering-Induced Dephasing in Two-Dimensional Semiconductors.Phys Rev Lett. 2020 Jun 26;124(25):257402. doi: 10.1103/PhysRevLett.124.257402. Phys Rev Lett. 2020. PMID: 32639791
-
Semiconductor excitons in new light.Nat Mater. 2006 Jul;5(7):523-31. doi: 10.1038/nmat1658. Nat Mater. 2006. PMID: 16819475 Review.
Cited by
-
Unveiling Multiquantum Excitonic Correlations in Push-Pull Polymer Semiconductors.J Phys Chem Lett. 2024 Apr 11;15(14):3705-3712. doi: 10.1021/acs.jpclett.4c00065. Epub 2024 Mar 28. J Phys Chem Lett. 2024. PMID: 38546242 Free PMC article.
Publication types
LinkOut - more resources
Full Text Sources