Abstract
One of the key phenomena that determine the fluorescence of nanocrystals is the nonradiative Auger-Meitner recombination of excitons. This nonradiative rate affects the nanocrystals’ fluorescence intensity, excited state lifetime, and quantum yield. Whereas most of the above properties can be directly measured, the quantum yield is the most difficult to assess. Here we place semiconductor nanocrystals inside a tunable plasmonic nanocavity with subwavelength spacing and modulate their radiative de-excitation rate by changing the cavity size. This allows us to determine absolute values of their fluorescence quantum yield under specific excitation conditions. Moreover, as expected considering the enhanced Auger-Meitner rate for higher multiple excited states, increasing the excitation rate reduces the quantum yield of the nanocrystals.
| Original language | English |
|---|---|
| Pages (from-to) | 2702-2707 |
| Number of pages | 6 |
| Journal | Journal of Physical Chemistry Letters |
| Volume | 14 |
| Issue number | 10 |
| DOIs | |
| State | Published - 16 Mar 2023 |
Bibliographical note
Publisher Copyright:© 2023 The Authors. Published by American Chemical Society.
Funding
This work was supported by the Deutsche Forschungsgemeinschaft (DFG, German Research Foundation) under Germany’s Excellence Strategy─EXC 2067/1-390729940. S.G. and A.I.C. are grateful to the Deutsche Forschungsgemeinschaft (DFG, German Research Foundation) for financial support through project 431012826. J.E. and S.G. are grateful to the European Research Council (ERC) via project “smMIET” (Grant Agreement No. 884488) under the European Union’s Horizon 2020 research and innovation program. This research was also supported by DARPA Fund No. D14PC00141, by the European Research Council (ERC) advanced grant NVS 669941, by the Human Frontier Science Program (HFSP) research grant RGP0061/2015, and by the BER program of the Department of Energy Office of Science, grant DE-FC03-02ER63421. Work at the Molecular Foundry was supported by the Office of Science, Office of Basic Energy Sciences, of the U.S. Department of Energy under Contract No. DE-AC02-05CH11231. This work was also supported by STROBE: A National Science Foundation Science & Technology Center under Grant No. DMR 1548924.
| Funders | Funder number |
|---|---|
| U.S. Department of Energy | DE-AC02-05CH11231 |
| Defense Advanced Research Projects Agency | NVS 669941, D14PC00141 |
| Office of Science | DE-FC03-02ER63421 |
| Basic Energy Sciences | |
| Horizon 2020 Framework Programme | |
| BioXFEL Science and Technology Center | DMR 1548924 |
| European Commission | 884488 |
| Human Frontier Science Program | RGP0061/2015 |
| Deutsche Forschungsgemeinschaft | EXC 2067/1-390729940, 431012826 |