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Cocina, A.* ; Brechbühler, R.* ; Vonk, S.J.W.* ; Cui, J. ; Rossinelli, A.A.* ; Rojo, H.* ; Rabouw, F.T.* ; Norris, D.J.*

Nanophotonic approach to study excited-state dynamics in semiconductor nanocrystals.

J. Phys. Chem. Lett. 13, 4145-4151 (2022)
Postprint DOI PMC
Open Access Green
In semiconductor nanocrystals, excited electrons relax through multiple radiative and nonradiative pathways. This complexity complicates characterization of their decay processes with standard time- and temperature-dependent photoluminescence studies. Here, we exploit a simple nanophotonic approach to augment such measurements and to address open questions related to nanocrystal emission. We place nanocrystals at different distances from a gold reflector to affect radiative rates through variations in the local density of optical states. We apply this approach to spherical CdSe-based nanocrystals to probe the radiative efficiency and polarization properties of the lowest dark and bright excitons by analyzing temperature-dependent emission dynamics. For CdSe-based nanoplatelets, we identify the charge-carrier trapping mechanism responsible for strongly delayed emission. Our method, when combined with careful modeling of the influence of the nanophotonic environment on the relaxation dynamics, offers a versatile strategy to disentangle the complex excited-state decay pathways present in fluorescent nanocrystals as well as other emitters.
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Publication type Article: Journal article
Document type Scientific Article
Corresponding Author
e-ISSN 1948-7185
Journal Journal of Physical Chemistry Letters, The
Quellenangaben Volume: 13, Issue: 18, Pages: 4145-4151 Article Number: , Supplement: ,
Publisher American Chemical Society (ACS)
Non-patent literature Publications
Reviewing status Peer reviewed
Institute(s) Helmholtz Pioneer Campus (HPC)
Grants Nederlandse Organisatie voor Wetenschappelijk onderzoek
Schweizerischer Nationalfonds zur Forderung der Wissenschaftlichen Forschung
European Research Council
Seventh Framework Programme