Eppur Si Riscalda - and yet, It (Just) Heats Up: Further Comments on “Quantifying Hot Carrier and Thermal Contributions in Plasmonic Photocatalysis”

10 July 2019, Version 1
This content is a preprint and has not undergone peer review at the time of posting.

Abstract

Our Comment [1] on recent attempts to distinguish thermal and non-thermal (``hot carrier'') contributions to plasmon-assisted photocatalysis [2] initiated a re-evaluation process of previous literature on the topic within the nano-plasmonics and chemistry communities. The Response of Zhou et al [3] attempts to defend the claims of the original paper [2].

In this manuscript, we show that the Response [3] presents additional data that further validates our central criticism: inaccurately measured temperatures (that are lower than the actual temperature of the catalyst) led Zhou \etal to incorrectly claim conclusive evidence of non-thermal effects. We identify flaws in the experimental setup (e.g. the use of the default settings for the thermal camera and incorrect positioning of the thermometer) that may have led Zhou et al to make such claims. We further show that the Response contains several factual errors and does not address the technical problems we identified with the data acquisition in [2]. We demonstrate that both the Response [3] and the original paper [2] contain additional faults, for example, in the power determination and in the normalization of the rate to the catalyst volume, and exhibit misconceptions regarding the thermo-optic response of metal nanostructures. The burden of proof required by the proposal of a novel physical mechanism has simply not been met, especially when the existing data can be modeled exquisitely by conventional theory.
[1] Y. Sivan, J. Baraban, I. W. Un & Y. Dubi, Science Vol. 364, Issue 6439, eaaw9367. https://science.sciencemag.org/content/364/6439/eaaw9367.abstract

[2] https://science.sciencemag.org/content/362/6410/69

[3] https://science.sciencemag.org/content/364/6439/eaaw9545

Keywords

Plasmonic photocatalysis
hot electrons

Comments

Comments are not moderated before they are posted, but they can be removed by the site moderators if they are found to be in contravention of our Commenting Policy [opens in a new tab] - please read this policy before you post. Comments should be used for scholarly discussion of the content in question. You can find more information about how to use the commenting feature here [opens in a new tab] .
This site is protected by reCAPTCHA and the Google Privacy Policy [opens in a new tab] and Terms of Service [opens in a new tab] apply.