Recently we published an article
in Journal of Physical Chemistry Letters titled “Strong
Plasmon Enhancement of the Saturation Photon Count Rate of Single
Molecules” (DOI: 10.1021/acs.jpclett.0c00155; publication date:
February 19, 2020). Unfortunately, it recently came to our attention
that there is a typographical error in the discussion of Figure 6.Following the comments by one of the referees we modified the manuscript
regarding the triplet state modifications, but we mistakenly state
that the ratio γisc/γT might be
at the origin of the mismatch we find in Isat. Obviously, if PCRmax matches the expectation, the ratio
γisc/γT also matches the expectation.
The text should therefore read that not the ratio γisc/γT but the absolute value of γisc is at the origin of the mismatch. If possible we would also like
broaden the argument and include one sentence that an overestimation
of the particle–fluorophore spacing might contribute as well
because γnr scales more strongly with distance than
γr.The paragraph containing the above-mentioned
additions and corrections
should read as follows:In the simulations we have treated the
term appearing in
both eq 3 and 4 as unity,
following Ebbesen et al.[1] Considering the
fact that the PCRmax enhancement closely follows the prediction
this could indicate stronger than expected plasmonic modification
of γtot, which contains contributions of γnr and γisc. First, a particle–fluorophore
spacing smaller than expected by only 0.5 nm causes a 2-fold
increase in Isat, whereas PCRmax increases by only 10%. This is caused by the fact that γnr depends more strongly on particle–fluorophore spacing
than γr. Second, modification of γisc might also play a role in the higher Isat. Modification of γisc has also been reported, but
experimental studies are limited to a select number of cases[2−6] that indeed report modest modifications. A quantitative investigation
of triplet modifications requires a temporal resolution that is not
accessible in our current camera-based setup but could be further
investigated using, for example, fluorescence correlation spectroscopy
(FCS).[6−8]