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Resonantly pumped bright-triplet exciton lasing in cesium lead bromide perovskites

Abstract:
The surprising recent observation of highly emissive triplet-states in lead halide perovskites accounts for their orders-of-magnitude brighter optical signals and high quantum efficiencies compared to other semiconductors. This makes them attractive for future optoelectronic applications, especially in bright low-threshold nanolasers. While nonresonantly pumped lasing from all-inorganic lead-halide perovskites is now well-established as an attractive pathway to scalable low-power laser sources for nano-optoelectronics, here we showcase a resonant optical pumping scheme on a fast triplet-state in CsPbBr<sub>3</sub> nanocrystals. The scheme allows us to realize a polarized triplet-laser source that dramatically enhances the coherent signal by 1 order of magnitude while suppressing noncoherent contributions. The result is a source with highly attractive technological characteristics, including a bright and polarized signal and a high stimulated-to-spontaneous emission signal contrast that can be filtered to enhance spectral purity. The emission is generated by pumping selectively on a weakly confined excitonic state with a Bohr radius ∼10 nm in the nanocrystals. The exciton fine-structure is revealed by the energy-splitting resulting from confinement in nanocrystals with tetragonal symmetry. We use a linear polarizer to resolve 2-fold nondegenerate sublevels in the triplet exciton and use photoluminescence excitation spectroscopy to determine the energy of the state before pumping it resonantly.
Publication status:
Published
Peer review status:
Peer reviewed

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Publisher copy:
10.1021/acsphotonics.1c00720

Authors


More by this author
Role:
Author
ORCID:
0000-0002-2393-9745
More by this author
Role:
Author
ORCID:
0000-0001-6566-0438


Publisher:
American Chemical Society
Journal:
ACS Photonics More from this journal
Volume:
8
Issue:
9
Pages:
2699-2704
Publication date:
2021-08-27
Acceptance date:
2021-08-20
DOI:
EISSN:
2330-4022
ISSN:
2330-4022
Pmid:
34557568


Language:
English
Keywords:
Pubs id:
1195948
Local pid:
pubs:1195948
Deposit date:
2021-11-23

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