Plasmonic substrates comprising gold nanostars efficiently regenerate cofactor molecules

Sánchez‐Iglesias, Ana; Barroso, Javier; Solís, Diego M.; Taboada, J. M.; Obelleiro, F.; Pavlov, Valeri; Grzelczak, Marek

doi:10.1039/c6ta01770c

Cited by 31 publications

(37 citation statements)

References 54 publications

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“…In particular, we will look at spherical NPs, NRs, and NSTs. The NSTs are especially interesting for the plasmonic effects since they have multiple hot spots at the tips . It was also shown experimentally and theoretically in refs.…”

Section: Electromagnetic Models Of Nanocrystals and Quantum Formalismmentioning

confidence: 71%

“…It was also shown experimentally and theoretically in refs. that the geometrical parameters of the tips in the NSTs strongly influence the positions of plasmonic resonances in such NCs. In our study, we first calculate classical optical properties of nanocrystals using the COMSOL software and the empirical dielectric constants of metals (gold and silver) .…”

Section: Electromagnetic Models Of Nanocrystals and Quantum Formalismmentioning

confidence: 99%

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Plasmonic Nanostars with Hot Spots for Efficient Generation of Hot Electrons under Solar Illumination

Kong

Wang

Govorov

2016

Advanced Optical Materials

153

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to the resonant plasmonic effect. It was also observed [24,26,27] and calculated [25] that the plasmonic hot spots in metal nanostructures can generate large numbers of energetic electrons. The design of a plasmonic nanocrystal is crucial to create plasmonic hot spots that generate efficiently energetic electrons. In this study, we will address this problem of hot spots and energetic electrons.Here we investigate theoretically the process of generation of hot electrons in nanocrystals with various shapes, such as nanostars (NSTs), nanorods (NRs), and spherical nanoparticles (NPs). The focus will be on the role of plasmonic hot spots in such NCs. In this study, we show that plasmonic NSTs with multiple hot spots are very efficient for generation of energetic electrons. We also compare NSTs with NRs and NPs and discuss two material systems, gold and silver. Silver NCs exhibit much larger rates of generation since the plasmon enhancement in such silver NCs is much stronger than that in the case of gold. The physical reason for the high rates of generation of hot carriers in the silver NCs are the following: (1) The long mean free path of electrons and (2) the narrow and intensive plasmonic resonances. The effect of generation of hot electrons is an essentially quantum effect and comes from the optical absorption processes near the surfaces of a NC. Such surface absorption is, of course, efficient only in relatively small NCs. We, therefore, examine the quantum efficiencies and the quantum plasmonic parameter for NCs of various sizes and shapes. Using such calculations, we show the quantum nature of the generation of energetic carriers in NCs in general.We also should note that the formalism of the paper focuses on the quantum intraband transitions in the NCs made of gold and silver. Such intraband transitions dominate the optical responses of the plasmonic NCs in the spectral intervals λ > 500 nm (gold) and λ > 400 nm (silver). Simultaneously, these spectral intervals are most interesting for the plasmonic effects since the plasmonic peaks in these spectral regions appear to be narrow and strong. [23] Regarding the role of the interband transitions and generation of hot holes in the d-band, one can look into recent review papers (e.g., ref.[23]).Theoretically, the problem of hot electrons has been addressed using several methods: Density matrix formalism combined with time-dependent DFT, perturbative approach for the injection currents, Fermi's golden rule, nonequilibrium Nanostars (NSTs) are spiky nanocrystals (NCs) with plasmonic hot spots. In this study, it is shown that strong electromagnetic fields localized in the NST tips are able to generate large numbers of energetic (hot) electrons, which can be used for photochemistry. To compute plasmonic NCs with complex shapes, a quantum approach based on the effect of surface generation of hot electrons is developed. This approach is then applied to NSTs, nanorods (NRs) and nanospheres. It is found that the plasmonic NSTs with multiple hot spots have the best charact...

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Section: Electromagnetic Models Of Nanocrystals and Quantum Formalismmentioning

confidence: 71%

Section: Electromagnetic Models Of Nanocrystals and Quantum Formalismmentioning

confidence: 99%

Plasmonic Nanostars with Hot Spots for Efficient Generation of Hot Electrons under Solar Illumination

Kong

Wang

Govorov

2016

Advanced Optical Materials

153

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“…The first successful example of plasmonic cofactor photoregenerator was reported for gold nanorods coated with Pt domains on their tips (Figure 8B), thereby representing a previously defined plasmonic photocatalyst containing a heterojunction that combines a plasmonic structure (Au NRs) and a catalytic active site (Pt) to successfully carry out the regeneration (reduction) of NADH cofactor molecules [85]. A subsequent study carried out by the same authors determined an even more remarkable photo-response of gold nanostars with epitaxially grown Pt domains that was associated to the major light harvesting capacity of the star-shaped plasmonic structures (see Figure 8A) [84,85]. The potential combination of these plasmonic heterojunctions with other semiconductors represents a very promising alternative to obtain suitable mediators that can help to modulate multiple biochemical processes via light-induced inputs.…”

Section: Alternativementioning

confidence: 97%

“…A brief overview of the current state of the art in this field devoted to regular semiconductors has been recently published elsewhere [83].More recent studies involving the use of plasmonic materials have been reported by Sanchez-Iglesias et al Their studies focused on the evaluation of multiple gold-shaped plasmonic nanostructures (see Figure 8) and their effect on the effective photoregeneration of nicotinamide adenine dinucleotide (NADH) molecules. These latter molecules are extremely important in natural biochemical routes as mediating cofactors in many enzymes [84,85]. Moreover, cofactor molecules are necessary, for instance, in the photosynthesis process as light harvesters and intervening in the reduction-oxidation balances involved in respiration [86].…”

Section: Photobiocatalysismentioning

confidence: 99%

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Plasmonics Devoted to Photocatalytic Applications in Liquid, Gas, and Biological Environments

Bueno-Alejo¹,

Arca-Ramos²,

Hueso³

2017

Nanoplasmonics - Fundamentals and Applications

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Plasmonic nanomaterials have emerged in the last years as a very interesting option for many photocatalytic processes. Their localized surface plasmon resonance (LSPR) brings in some unique properties that overcome some of the drawbacks associated with traditional photocatalysis based on semiconductors. Even when in its infancy, many advances have been made in the field, mainly related to the synthesis of new structures with the capabilities of light absorption in the whole solar spectrum. A great number of reactions have been attempted using nanoplasmonic materials. In this chapter, we present the most recent advances made in the field of plasmonic photocatalysis comprising an introductory section to define the main types of plasmonic nanomaterials available, including the most recently labeled alternatives. Following with the major areas of catalytic application, a second section of the chapter has been devoted to liquid-phase reactions for the treatment of pollutants and a selection of organic reactions to render added-value to chemicals under mild conditions. The third part of the chapter addresses two specific applications of nanoplasmonic photocatalysts in gas-phase reactions involving the remediation of volatile organic compounds and the transformation of carbon dioxide into valuable energy-related chemicals. Finally, a fourth section of the chapter introduces the most recent applications of plasmonics in biochemical processes involving the regulation of cofactor molecules and their mimetic behavior as potential enzyme-like surrogates.

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Plasmonic Photocatalysis: Activating Chemical Bonds through Light and Plasmon

Jain

Kashyap

Pillai

2022

Advanced Optical Materials

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Plasmonic substrates comprising gold nanostars efficiently regenerate cofactor molecules

Abstract: Gold nanostars as a photocatalyst perform better than rods and cubes.

Cited by 31 publications

References 54 publications

Plasmonic Nanostars with Hot Spots for Efficient Generation of Hot Electrons under Solar Illumination

Plasmonic Nanostars with Hot Spots for Efficient Generation of Hot Electrons under Solar Illumination

Plasmonics Devoted to Photocatalytic Applications in Liquid, Gas, and Biological Environments

Plasmonic Photocatalysis: Activating Chemical Bonds through Light and Plasmon

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