Eppur si riscalda -- and yet，it（just）heats up：Further Comments on“Quantifying hot carrier and thermal contributions in plasmonic crystals”
Eppur si riscalda -- and yet, it (just) heats up: Further Comments on "Quantifying hot carrier and thermal contributions in plasmonic photocatalysis"
摘要：
我们的评论[Sivan等人，Science 2019]（以及其较长版本[Dubi，Un，& Sivan，ArXiv 2019]，以及支持理论研究[Dubi和Sivan，ArXiv 2018]）最近尝试区分热和非热（“热载流子”）对等离子体辅助的电子束的贡献[Zhou et al.，Science 2018]启动了对纳米等离子体和化学社区内有关该主题的先前文献的重新评估过程。Zhou等人的回应试图捍卫原始论文的主张。在这份手稿中，我们表明，回应提供了额外的数据，进一步证实了我们的核心批评：不准确的测量温度（低于催化剂的实际温度）导致Zhou等人错误地声称非热效应的确凿证据。我们确定了实验设置中的缺陷（例如，使用热成像相机的默认设置和温度计的不正确定位），这些缺陷可能导致Zhou等人做出这样的声明。我们进一步表明，回应包含几个事实错误，并且没有解决我们在[Zhou et al.，Science 2018]。我们表明，响应和原始文件包含额外的故障，例如，在功率确定和催化剂体积的速率的归一化，并表现出误解的热光响应的金属纳米结构。提出一种新的物理机制所需的举证责任根本没有得到满足，特别是当现有的数据可以通过传统理论进行精确建模时。
英文摘要：
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.
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