Hot electron-driven photocatalysis and transient absorption spectroscopy in plasmon resonant grating structures

Wang, Yi; Shen, Lang; Wang, Yu; Hou, Bingya; Gibson, George N.; Poudel, Nirakar; Chen, Jihan; Shi, Haotian; Guignon, Ernest; Cady, Nathaniel C.; Page, William D.; Pilar, Arturo; Dawlaty, Jahan M.; Cronin, Stephen B.

doi:10.1039/c8fd00141c

Cited by 18 publications

(19 citation statements)

References 16 publications

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“…Instead of varying the illumination power, varying the light beam diameter can also provide valuable information. As shown further on, this procedure applies only for reactions occurring at the surface of a solid catalyst, such as a substrate covered with nanoparticles 6,[38][39][40] or an optically thick pellet 41 . It does not apply for photochemical reactions occurring on nanoparticles suspended in a liquid 42 , where heat diffusion is more complex.…”

Section: Procedures # 2: Varying the Light Beam Diametermentioning

confidence: 99%

“…Thus, depending on how the illumination beam diameter is varied, the photochemical rate features radically different variations. Note that this reasoning makes no assumption on the sample thickness and, for this reason, applies not only for particles deposited on a flat substrate 6,[38][39][40] but also for thick samples, e.g., made of compacted powders or pellets 41 .…”

Section: Procedures # 2: Varying the Light Beam Diametermentioning

confidence: 99%

“…We noted above that this procedure could be applied for solid samples, typically catalysts and nanoparticles dispersed on a planar substrate 6,[38][39][40] or pellets 41 , in contact with a gas or a liquid phase, for which a heat source would remain twodimensional. Indeed, the case of nanoparticles and reactants suspended in solution is more complex and cannot be faithfully investigated using this procedure.…”

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confidence: 99%

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Simple experimental procedures to distinguish photothermal from hot-carrier processes in plasmonics

et al. 2020

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Light absorption and scattering of plasmonic metal nanoparticles can lead to non-equilibrium charge carriers, intense electromagnetic near-fields, and heat generation, with promising applications in a vast range of fields, from chemical and physical sensing to nanomedicine and photocatalysis for the sustainable production of fuels and chemicals. Disentangling the relative contribution of thermal and non-thermal contributions in plasmon-driven processes is, however, difficult. Nanoscale temperature measurements are technically challenging, and macroscale experiments are often characterized by collective heating effects, which tend to make the actual temperature increase unpredictable. This work is intended to help the reader experimentally detect and quantify photothermal effects in plasmon-driven chemical reactions, to discriminate their contribution from that due to photochemical processes and to cast a critical eye on the current literature. To this aim, we review, and in some cases propose, seven simple experimental procedures that do not require the use of complex or expensive thermal microscopy techniques. These proposed procedures are adaptable to a wide range of experiments and fields of research where photothermal effects need to be assessed, such as plasmonic-assisted chemistry, heterogeneous catalysis, photovoltaics, biosensing, and enhanced molecular spectroscopy.

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Section: Procedures # 2: Varying the Light Beam Diametermentioning

confidence: 99%

Section: Procedures # 2: Varying the Light Beam Diametermentioning

confidence: 99%

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confidence: 99%

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Simple experimental procedures to distinguish photothermal from hot-carrier processes in plasmonics

et al. 2020

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“…In order to investigate the mechanism of the enhanced photocatalytic performance of 6B-TiO 2 , the samples of bare TiO 2 and B doping TiO 2 were investigated by photocurrent response, EIS and PL spectrum, and the results are shown in Figure 3. It can be seen in Figure 3A that 6B-TiO 2 shows highest photocurrent response, indicating that more electrons can be generated in 6B-TiO 2 by visible light irradiation Murali et al, 2019;Wang et al, 2019). In the EIS analysis (Figure 3B), 6B-TiO 2 exhibits a semicircle of the EIS Nyquist plot with the smallest radius, indicating the smallest interfacial charge transference impedance as compared to those of bare TiO 2 and other B doping TiO 2 (Dai et al, 2015;Zou et al, 2016;Manwar et al, 2019).…”

Section: Characterization Of B Doping Tio 2 Samplesmentioning

confidence: 94%

Optimization of Boron Doped TiO2 as an Efficient Visible Light-Driven Photocatalyst for Organic Dye Degradation With High Reusability

Niu

Chen

et al. 2020

Front. Chem.

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No visible light activity is the bottle neck for wide application of TiO 2 , and Boron doping is one of the effective way to broaden the adsorption edge of TiO 2 . In this study, several Boron doped TiO 2 materials were prepared via a facile co-precipitation and calcination process. The B doping amounts were optimized by the degradation of rhodamine B (Rh B) under visible light irradiation, which indicated that when the mass fraction of boron is 6% (denoted as 6B-TiO 2 ), the boron doped TiO 2 materials exhibited the highest activity. In order to investigate the enhanced mechanism, the difference between B-doped TiO 2 and bare TiO 2 including visible light harvesting abilities, separation efficiencies of photo-generated electron-hole pairs, photo-induced electrons generation abilities, photo-induced charges transferring speed were studied and compared in details. h + and · O − 2 were determined to be the two main responsible active species in the photocatalytic oxidation process. Besides the high degradation efficiency, 6B-TiO 2 also exhibited high reusability in the photocatalysis, which could be reused at least 5 cycles with almost no active reduction. The results indicate that 6B-TiO 2 has high photocatalytic degradation ability toward organic dye of rhodamine B under visible light irradiation, which is a highly potential photocatalyst to cope with organic pollution.

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“…More recently, corrugated metallic grating nanostructures have emerged as an effective platform for generating plasmon-enhanced hot carriers in the visible range [13][14][15]. These gratings are fabricated by depositing a plasmonic metal on a corrugated silicon substrate.…”

Section: Introductionmentioning

confidence: 99%

Hot Electron Plasmon-Resonant Grating Structures for Enhanced Photochemistry: A Theoretical Study

et al. 2021

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Metallic grating structures have been shown to provide an effective platform for generating hot electrons and driving electrochemical reactions. Here, we present a systematic theoretical study of the surface plasmon resonance in different corrugated metallic grating structures using computational electromagnetic tools (i.e., the finite difference time domain (FDTD) method). We identify the corrugation parameters that produce maximum resonant field enhancement at commonly used wavelengths for photocatalytic applications (633 nm and 785 nm) in different material systems, including Ag, Au, Cu, Al, and Pt. The absorption spectra of each grating structure have been fitted with the analytical equation obtained from Coupled Mode Theory. We then extracted the absorptive and radiative loss rates. The field enhancement can be maximized by matching the absorption and radiation losses via tuning the geometric parameters. We could improve the average field enhancement of 633 nm and 785 nm modes by a factor of 1.8× and 3.8× for Ag, 1.4× and 3.6× for Au, and 1.2× and 2.6× for Cu. The optimum structures are found to be shallower for Ag, Au, and Cu; deeper for Pt; and to almost remain the same for Al. The gratings become flat for all the metals for increasing the average field enhancement. Overall, Ag and Au were found to be the best in terms of overall field enhancement while Pt had the worst performance.

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Hot electron-driven photocatalysis and transient absorption spectroscopy in plasmon resonant grating structures

Abstract: We have developed a method to measure photocurrents produced by photoexcited hot electrons and holes in bulk metal films.

Cited by 18 publications

References 16 publications

Simple experimental procedures to distinguish photothermal from hot-carrier processes in plasmonics

Simple experimental procedures to distinguish photothermal from hot-carrier processes in plasmonics

Optimization of Boron Doped TiO2 as an Efficient Visible Light-Driven Photocatalyst for Organic Dye Degradation With High Reusability

Hot Electron Plasmon-Resonant Grating Structures for Enhanced Photochemistry: A Theoretical Study

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