TY - UNPB
T1 - Eppur si riscalda -- and yet, it (just) heats up
T2 - Further Comments on "Quantifying hot carrier and thermal contributions in plasmonic photocatalysis"
AU - Sivan, Yonatan
AU - Baraban, Joshua
AU - Dubi, Yonatan
PY - 2019/7
Y1 - 2019/7
N2 - Our Comment [Sivan et al., Science 2019] (as well as its longer version
[Dubi, Un, & Sivan, ArXiv 2019], and the supporting theoretical
studies [Dubi and Sivan, ArXiv 2018]) on recent attempts to distinguish
thermal and non-thermal ("hot carrier") contributions to
plasmon-assisted photocatalysis [Zhou et al., Science 2018] initiated a
re-evaluation process of previous literature on the topic within the
nano-plasmonics and chemistry communities. The Response of Zhou et al.
attempts to defend the claims of the original paper. In this manuscript,
we show that the Response presents additional data that further
validates our central criticism: inaccurately measured temperatures
(that are lower than the actual temperature of the catalyst) led Zhou et
al. 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 [Zhou et al., Science 2018]. We demonstrate that both the
Response and the original paper 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.
AB - Our Comment [Sivan et al., Science 2019] (as well as its longer version
[Dubi, Un, & Sivan, ArXiv 2019], and the supporting theoretical
studies [Dubi and Sivan, ArXiv 2018]) on recent attempts to distinguish
thermal and non-thermal ("hot carrier") contributions to
plasmon-assisted photocatalysis [Zhou et al., Science 2018] initiated a
re-evaluation process of previous literature on the topic within the
nano-plasmonics and chemistry communities. The Response of Zhou et al.
attempts to defend the claims of the original paper. In this manuscript,
we show that the Response presents additional data that further
validates our central criticism: inaccurately measured temperatures
(that are lower than the actual temperature of the catalyst) led Zhou et
al. 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 [Zhou et al., Science 2018]. We demonstrate that both the
Response and the original paper 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.
KW - Physics - Chemical Physics
U2 - 10.48550/arXiv.1907.04773
DO - 10.48550/arXiv.1907.04773
M3 - Preprint
BT - Eppur si riscalda -- and yet, it (just) heats up
ER -