Even-Parity Self-Trapped Excitons Lead to Magnetic
Dipole Radiation in Two-Dimensional
Lead Halide Perovskites
Version 2 2022-04-19, 18:04
Version 1 2020-07-15, 14:36
Posted on 2022-04-19 - 18:04
Recently, unconventional bright magnetic dipole (MD) radiation
was observed from two-dimensional (2D) hybrid organic–inorganic
perovskites (HOIPs). According to commonly accepted HOIP band structure
calculations, such MD light emission from the ground-state exciton
should be strictly symmetry forbidden. These results suggest that
MD emission arises in conjunction with an as-yet unidentified symmetry-breaking
mechanism. In this paper, we show that MD light emission originates
from a self-trapped p-like exciton stabilized at energies below the
primary electric dipole (ED)-emitting 1s exciton. Using suitable combinations
of sample and collection geometries, we isolate the distinct temperature-dependent
properties of the ED and MD photoluminescence (PL). We show that the
ED emission wavelength is nearly constant with temperature, whereas
the MD emission wavelength exhibits substantial red shifts with heating.
To explain these results, we derive a microscopic model comprising
two distinct parity exciton states coupled to lattice distortions.
The model explains many experimental observations, including the thermal
red shift, the difference in emission wavelengths, and the relative
intensities of the ED and MD emission. Thermodynamic analysis of temperature-dependent
PL reveals that the MD emission originates from a locally distorted
structure. Finally, we demonstrate unusual hysteresis effects of the
MD-emitting state near structural phase transitions. We hypothesize
that this is another manifestation of the local distortions, indicating
that they are insensitive to phase changes in the equilibrium lattice
structure.
CITE THIS COLLECTION
DataCite
3 Biotech
3D Printing in Medicine
3D Research
3D-Printed Materials and Systems
4OR
AAPG Bulletin
AAPS Open
AAPS PharmSciTech
Abhandlungen aus dem Mathematischen Seminar der Universität Hamburg
ABI Technik (German)
Academic Medicine
Academic Pediatrics
Academic Psychiatry
Academic Questions
Academy of Management Discoveries
Academy of Management Journal
Academy of Management Learning and Education
Academy of Management Perspectives
Academy of Management Proceedings
Academy of Management Review
DeCrescent, Ryan A.; Du, Xinhong; Kennard, Rhiannon M.; Venkatesan, Naveen R.; Dahlman, Clayton J.; Chabinyc, Michael L.; et al. (2020). Even-Parity Self-Trapped Excitons Lead to Magnetic
Dipole Radiation in Two-Dimensional
Lead Halide Perovskites. ACS Publications. Collection. https://doi.org/10.1021/acsnano.0c03783
or
Select your citation style and then place your mouse over the citation text to select it.
SHARE
Usage metrics
Read the peer-reviewed publication
AUTHORS (7)
RD
Ryan A. DeCrescent
XD
Xinhong Du
RK
Rhiannon M. Kennard
NV
Naveen R. Venkatesan
CD
Clayton J. Dahlman
MC
Michael L. Chabinyc
JS
Jon A. Schuller
KEYWORDS
yet unidentified symmetryusing suitable combinationsthermal red shiftstrictly symmetry forbiddenprimary electric dipolelocally distorted structuretrapped excitons leadlike exciton stabilizedequilibrium lattice structuremd light emissionmd emission originatesmd emission arisesmagnetic dipole radiationdependent pl revealsed emission wavelengthmd emissionemission wavelengthstrapped pstate excitonpl ).lattice distortionsdependent propertiesmd photoluminescencethermodynamic analysisrelative intensitiesphase changesnearly constantlocal distortionshoips ).collection geometriesbreaking mechanismanother manifestation