Phonon-Bottleneck Enhanced Exciton Emission in 2D Perovskites
Journal article, 2024
Layered halide perovskites exhibit remarkable optoelectronic properties and technological promise, driven by strongly bound excitons. The interplay of spin-orbit and exchange coupling creates a rich excitonic landscape, determining their optical signatures and exciton dynamics. Despite the dark excitonic ground state, surprisingly efficient emission from higher-energy bright states has puzzled the scientific community, sparking debates on relaxation mechanisms. Combining low-temperature magneto-optical measurements with sophisticated many-particle theory, the origin of the bright exciton emission in perovskites is elucidated by tracking the thermalization of dark and bright excitons under a magnetic field. The unexpectedly high emission is clearly attributed to a pronounced phonon-bottleneck effect, considerably slowing down the relaxation toward the energetically lowest dark states. It is demonstrated that this bottleneck can be tuned by manipulating the bright-dark energy splitting and optical phonon energies, offering valuable insights and strategies for controlling exciton emission in layered perovskite materials that is crucial for optoelectronics applications.
exciton dynamics
phonons
layered perovskite
excitons
Author
J. J.P. Thompson
Philipps University Marburg
University of Cambridge
Mateusz Dyksik
Wrocław University of Science and Technology
Paulina Peksa
LCMI Laboratoire des Champs Magnetiques Intenses
Wrocław University of Science and Technology
Katarzyna Posmyk
Wrocław University of Science and Technology
LCMI Laboratoire des Champs Magnetiques Intenses
Ambjörn Joki
Chalmers, Microtechnology and Nanoscience (MC2), Applied Quantum Physics
Raul Perea Causin
Chalmers, Physics, Condensed Matter and Materials Theory
Paul Erhart
Chalmers, Physics, Condensed Matter and Materials Theory
M Baranowski
Wrocław University of Science and Technology
M. A. Loi
University of Groningen
Paulina Plochocka
LCMI Laboratoire des Champs Magnetiques Intenses
Wrocław University of Science and Technology
Ermin Malic
Philipps University Marburg
Advanced Energy Materials
1614-6832 (ISSN) 1614-6840 (eISSN)
Vol. 14 20 2304343Subject Categories
Atom and Molecular Physics and Optics
Condensed Matter Physics
DOI
10.1002/aenm.202304343