AI Article Synopsis
- The emission spectrum of a dye is influenced by the energy of radiative transitions and can be modified using optical nanoantennas that alter the decay rates of emitters.
- DNA origami is utilized to position a dye near a gold nanorod, showing how placement affects the emission spectrum, leading to varying enhancements or suppressions of transitions depending on their overlap with the nanorod's resonance.
- The significant changes in fluorescence observed may indicate violations of Kasha's rule, pointing to a complex interaction between the dye's emissions and the nanostructure.
Article Abstract
The emission spectrum of a dye is given by the energy of all of the possible radiative transitions weighted by their probability. This spectrum can be altered with optical nanoantennas that are able to manipulate the decay rate of nearby emitters by modifying the local density of photonic states. Here, we make use of DNA origami to precisely place an individual dye at different positions around a gold nanorod and show how this affects the emission spectrum of the dye. In particular, we observe a strong suppression or enhancement of the transitions to different vibrational levels of the excitonic ground state, depending on the spectral overlap with the nanorod resonance. This reshaping can be used to experimentally extract the spectral dependence of the radiative decay rate enhancement. Furthermore, for some cases, we argue that the drastic alteration of the fluorescence spectrum could arise from the violation of Kasha's rule.
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| http://dx.doi.org/10.1021/acs.nanolett.3c01818 | DOI Listing |
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