Plasmonic Chirality and Circular Dichroism in Bioassembled and Nonbiological Systems: Theoretical Background and Recent Progress

Kong, Xiang‐Tian; Besteiro, Lucas V.; Wang, Zhiming; Govorov, Alexander O.

doi:10.1002/adma.201801790

Cited by 134 publications

(126 citation statements)

References 109 publications

(330 reference statements)

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“…Finally, during hot electron injection (3), carriers typically acquire low transmission probability because of considerable momentum mismatch and poor overlap of the electron wavefunctions between the metal and the semiconductor . While momentum conservation is broken when the dimension of the plasmonic component is much lower than the photon wavelength, as in the case of NPs, the overlap of electronic wavefunctions still strongly influences electron injection efficiency. In our photocatalytic system hot electrons produced in TiN have a stronger overlap of their wavefunctions with TiO 2 when compared to Au, since the density of states of conduction band is mainly characterized by Ti 3d wavefunctions for both TiN and TiO 2 .…”

Section: Resultsmentioning

confidence: 99%

“…This rate has the form

r_{s, high–energy} (θ, φ) = \frac{2}{π^{2}} \times \frac{e^{2} E_{normalF}^{2}}{ℏ} \frac{(ℏ ω - ϕ_{B})}{{(ℏ ω)}^{4}} {(||, E_{normalnormal} (θ, φ))}^{2}

where E normal (θ,ϕ) is the normal component of the internal electric field near the surface of the NP and E F is the Fermi energy of the metal. Using the above equations, we now arrive at the final expression for the total generation rate in a NP

\begin{matrix} {normalRate}_{high–energy} = \frac{2}{π^{2}} \times \frac{e^{2} E_{normalF}^{2}}{ℏ} \frac{ℏ ω - ϕ_{normalB}}{{(ℏ ω)}^{4}} \\ \times \int_{S_{NC}} {|E_{normal} (θ, φ)|}^{2} normald s \end{matrix}

…”

Section: Resultsmentioning

confidence: 99%

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Broadband Hot‐Electron Collection for Solar Water Splitting with Plasmonic Titanium Nitride

Naldoni

Guler

Wang

et al. 2017

Advanced Optical Materials

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283

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absorption. Although photocatalysis is already used in small-scale abatement of both indoor and outdoor pollution, the low efficiency (5%-10%) of solar-to-chemical energy conversion limits further breakthroughs in strategic applications such as hydrogen production and photovoltaics (PVs). [1,2] The engineering of composite interfaces for optimized operation is a key step to increase the solar absorption, electron-hole separation, and collection, and finally to provide high reaction yield. [3,4] The use of plasmonic nanostructures in energy conversion applications has been recently demonstrated with the enhanced performance of solar-to-fuels and solar-to-electricity devices. [5][6][7][8][9][10][11] Surface plasmons concentrate light into nanoscale volumes at the interface of a dielectric or a semiconductor providing intense electromagnetic field localization and improved scattering. The possibility to harness hot electrons generated from the surface plasmon decay [12,13] has shown to be a promising route toward selective nanocatalysis, [14][15][16][17][18][19][20] full-spectrum solar water splitting, [21][22][23] and ultrafast photodetection. [24][25][26][27] The nonradiative decay of surface plasmons, occurring in the 40-150 fs timescale, [12] produces a population of highly energetic (hot) electrons that are stabilized through injection into the semiconductor conduction band across a Schottky barrier. [28] Plasmonic nanoparticles (NPs) enable the efficient conversion of solar light into electrons with an energy well below the band gap of the semiconductor but limited to energies higher than the potential barrier (φ B ). As of yet, these demonstrations have been limited to NPs made of plasmonic noble metals such as Ag and Au. Despite their good optical performance, several challenges remain for noble metal NPs including high cost, poor chemical (Ag) and thermal stability (Au, Ag), diffusion into surrounding structures, and CMOS incompatibility, which hinders the practical implementation of conventional plasmonic structures.Aluminum nanocrystals are alternative plasmonic photocatalysts that provide efficient hot electron generation at low cost (i.e., high abundance of Al on the earth crust). [29][30][31][32][33][34] Nevertheless, issues for large-scale applications are related to Al NPs preparation, due to explosive reactivity of Al molecular The use of hot electrons generated from the decay of surface plasmons is a novel concept that promises to increase the conversion yield in solar energy technologies. Titanium nitride (TiN) is an emerging plasmonic material that offers compatibility with complementary metal-oxide-semiconductor (CMOS) technology, corrosion resistance, as well as mechanical strength and durability, thus outperforming noble metals in terms of cost, mechanical, chemical, and thermal stability. Here, it is shown that plasmonic TiN can inject into TiO 2 twice as many hot electrons as Au nanoparticles. TiO 2 nanowires decorated with TiN nanoparticles show higher photocurrent enhancement than decorat...

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Section: Resultsmentioning

confidence: 99%

“…This rate has the form

r_{s, high–energy} (θ, φ) = \frac{2}{π^{2}} \times \frac{e^{2} E_{normalF}^{2}}{ℏ} \frac{(ℏ ω - ϕ_{B})}{{(ℏ ω)}^{4}} {(||, E_{normalnormal} (θ, φ))}^{2}

\begin{matrix} {normalRate}_{high–energy} = \frac{2}{π^{2}} \times \frac{e^{2} E_{normalF}^{2}}{ℏ} \frac{ℏ ω - ϕ_{normalB}}{{(ℏ ω)}^{4}} \\ \times \int_{S_{NC}} {|E_{normal} (θ, φ)|}^{2} normald s \end{matrix}

…”

Section: Resultsmentioning

confidence: 99%

Broadband Hot‐Electron Collection for Solar Water Splitting with Plasmonic Titanium Nitride

Naldoni

Guler

Wang

et al. 2017

Advanced Optical Materials

Self Cite

283

204

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“…In other words, the semiconductor is intrinsically active at the LSPR wavelength. On the other hand, the “hot spots” formed at the interface between plasmonic metal nanoparticles and the semiconductor can facilitate the photogeneration of electron–hole pairs and their subsequent separation, therefore reducing their recombination rate . We have recently synthesized BiOCl that has rich oxygen vacancies and is decorated with Au nanospheres for selective benzyl alcohol oxidation .…”

Section: Localized Surface Plasmon Resonancementioning

confidence: 99%

Emerging Applications of Plasmons in Driving CO₂ Reduction and N₂ Fixation

et al. 2018

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The photochemical production of fuels using sunlight is an innovative way for meeting the quickly increasing energy demands. One of the largest challenges is to develop high-performance photocatalysts that can meet the requirements of practical applications. Owing to their intriguing localized surface plasmon resonances, noble metal nanoparticles and nanostructures show a great potential for enhancing the photocatalytic efficiency and thereby have attracted rapidly growing interest recently. Here, for the first time, the latest achievements in the utilization of plasmons in driving CO reduction and N fixation into high-value products are comprehensively described. The involved plasmonic enhancement mechanisms in the two types of reactions are fully illustrated. A particular emphasis is given to the outlook on the direction and prospects for future work in this topic.

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“…Along these lines, the extent of such a photosensitization process is inversely proportional to the space separating both species . Moreover, the magnitude of the electromagnetic field enhancement created by the plasmonic component at the metal–semiconductor interface is another parameter of paramount importance to increase the efficiency of hot‐electron transfer . In other possible mechanisms, the ability of plasmonic nanoparticles to focalize the incoming light is used as a means to couple the plasmonic near‐field to the semiconductor, thus increasing the effective absorption cross section of the latter (antenna effect) .…”

Section: Methodsmentioning

confidence: 99%

“…b) Rate of hot‐electron injection as a function of the gap (averaged over orientations) calculated by using the surface rate formalism from Ref. . c) Calculated electromagnetic field enhancement as a function of the gap formed between two Au NRs in a tip‐to‐tip configuration.…”

Section: Methodsmentioning

confidence: 99%

Traveling Hot Spots in Plasmonic Photocatalysis: Manipulating Interparticle Spacing for Real‐Time Control of Electron Injection

et al. 2018

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Herein, we introduce a novel approach to achieve real‐time control over the hot‐electron injection process in metal–semiconductor photocatalysts. Such functionality is attained through the design of a hybrid nanocomposite in which plasmonic Au nanorods and TiO2 nanoparticles are synergistically integrated with a thermoresponsive polymer. In this manner, modifying the temperature of the system allows 1) precise regulation of the interparticle distance between the catalyst and the plasmonic component and 2) the reversible formation of plasmonic hot spots on the semiconductor. Both features can be simultaneously exploited to modulate the injection of hot electrons, thus boosting/inhibiting at will the photocatalytic activity of these heterostructures. This innovative conception enables dynamically adjustable performance of semiconductors, hence opening the door to the development of a new generation of plasmon‐operated photocatalytic devices.

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Plasmonic Chirality and Circular Dichroism in Bioassembled and Nonbiological Systems: Theoretical Background and Recent Progress

Cited by 134 publications

References 109 publications

Broadband Hot‐Electron Collection for Solar Water Splitting with Plasmonic Titanium Nitride

Broadband Hot‐Electron Collection for Solar Water Splitting with Plasmonic Titanium Nitride

Emerging Applications of Plasmons in Driving CO₂ Reduction and N₂ Fixation

Traveling Hot Spots in Plasmonic Photocatalysis: Manipulating Interparticle Spacing for Real‐Time Control of Electron Injection

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Plasmonic Chirality and Circular Dichroism in Bioassembled and Nonbiological Systems: Theoretical Background and Recent Progress

Cited by 134 publications

References 109 publications

Broadband Hot‐Electron Collection for Solar Water Splitting with Plasmonic Titanium Nitride

Broadband Hot‐Electron Collection for Solar Water Splitting with Plasmonic Titanium Nitride

Emerging Applications of Plasmons in Driving CO2 Reduction and N2 Fixation

Traveling Hot Spots in Plasmonic Photocatalysis: Manipulating Interparticle Spacing for Real‐Time Control of Electron Injection

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Emerging Applications of Plasmons in Driving CO₂ Reduction and N₂ Fixation