Plasmon-induced dynamics of H2 splitting on a silver atomic chain

Yan, Lei; Ding, Zijing; Song, Peng; Wang, Fangwei; Meng, Sheng

doi:10.1063/1.4929611

Cited by 32 publications

(37 citation statements)

References 37 publications

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“…Namely, increasing laser intensity results in increased charge transfer from Au NP to water, and subsequent rate enhancement for water splitting. In addition, below a critical laser fluence, no charge transfer occurs, and water does not split . We also examined the time-dependent charge density at the Fermi level E F (Figure c).…”

Section: Resultsmentioning

confidence: 99%

Quantum Mode Selectivity of Plasmon-Induced Water Splitting on Gold Nanoparticles

2016

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Plasmon induced water splitting is a promising research area with the potential for efficient conversion of solar to chemical energy, yet its atomic mechanism is not well understood. Here, ultrafast electron-nuclear dynamics of water splitting on gold nanoparticles upon exposure to femtosecond laser pulses was directly simulated using real time time-dependent density functional theory (TDDFT). Strong correlation between laser intensity, hot electron transfer, and reaction rates has been identified. The rate of water splitting is dependent not only on respective optical absorption strength, but also on the quantum oscillation mode of plasmonic excitation. Odd modes are more efficient than even modes, owing to faster decaying into hot electrons whose energy matches well the antibonding orbital of water. This finding suggests photocatalytic activity can be manipulated by adjusting the energy level of plasmon-induced hot carriers, through altering the cluster size and laser parameter, to better overlap adsorbate unoccupied level in plasmon-assisted photochemistry.

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Section: Resultsmentioning

confidence: 99%

Quantum Mode Selectivity of Plasmon-Induced Water Splitting on Gold Nanoparticles

2016

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“…Plasmon-driven photochemistry has received increasing attention in recent years for its potential for overcoming the intrinsic limitations of conventional semiconductor photocatalysis. Recent studies have shown that the generated hot carriers in plasmonic structures can be transferred to adjacent electron acceptors, inducing such photochemical processes as H 2 , O 2 , and N 2 dissociation, − water splitting, − artificial photosynthesis, and hydrocarbon conversion . The unique feature that the optical properties of metallic nanoparticles (NPs) are tunable over a wide range of the spectrum via size, shape, and composition makes the NPs an ideal candidate for plasmon-induced chemistry .…”

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confidence: 99%

Plasmonic Hot-Carrier-Mediated Tunable Photochemical Reactions

et al. 2018

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Hot-carrier generation from surface plasmon decay has found applications in many branches of physics, chemistry, materials science, and energy science. Recent reports demonstrated that the hot carriers generated from plasmon decay in nanoparticles can transfer to attached molecules and drive photochemistry which was thought impossible previously. In this work, we have computationally explored the atomic-scale mechanism of a plasmonic hot-carrier-mediated chemical process, H dissociation. Numerical simulations demonstrate that, after photoexcitation, hot carriers transfer to the antibonding state of the H molecule from the nanoparticle, resulting in a repulsive-potential-energy surface and H dissociation. This process occurs when the molecule is close to a single nanoparticle. However, if the molecule is located at the center of the gap in a plasmonic dimer, dissociation is suppressed due to sequential charge transfer, which efficiently reduces occupation in the antibonding state and, in turn, reduces dissociation. An asymmetric displacement of the molecule in the gap breaks the symmetry and restores dissociation when the additional charge transfer is significantly suppressed. Thus, these models demonstrate the possibility of structurally tunable photochemistry via plasmonic hot carriers.

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“…Similar results can be obtained by the same analysis, as shown in Figures 4B , 5B ,C, that is, the HOMO-1 and HOMO levels make a dominant contribution to the excitation to the LUMO and LUMO+1 state, where the corresponding wave functions are mainly distributed on the metal nanoparticle. Therefore, the channels of indirect charge transfer can be open via inelastic electron tunneling ( Christopher et al, 2011 ; Brongersma et al, 2015 ; Linic et al, 2015 ; Thrall et al, 2013 ; Mukherjee et al, 2013 ; Mukherjee et al, 2014 ; Zhang et al, 2018 ; Yan et al, 2015 ). Second, there is a significant charge transfer from the HOMO-8 to LUMO+11 states, as shown in Figure 5D .…”

Section: Resultsmentioning

confidence: 99%

Plasmon-Induced Water Splitting on Ag-Alloyed Pt Single-Atom Catalysts

et al. 2021

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A promising route to realize solar-to-chemical energy conversion resorts to water splitting using plasmon photocatalysis. However, the ultrafast carrier dynamics and underlying mechanism in such processes has seldom been investigated, especially when the single-atom catalyst is introduced. Here, from the perspective of quantum dynamics at the atomic length scale and femtosecond time scale, we probe the carrier and structural dynamics of plasmon-assisted water splitting on an Ag-alloyed Pt single-atom catalyst, represented by the Ag19Pt nanocluster. The substitution of an Ag atom by the Pt atom at the tip of the tetrahedron Ag20 enhances the interaction between water and the nanoparticle. The excitation of localized surface plasmons in the Ag19Pt cluster strengthens the charge separation and electron transfer upon illumination. These facts cooperatively turn on more than one charge transfer channels and give rise to enhanced charge transfer from the metal nanoparticle to the water molecule, resulting in rapid plasmon-induced water splitting. These results provide atomistic insights and guidelines for the design of efficient single-atom photocatalysts for plasmon-assisted water splitting.

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Plasmon-induced dynamics of H2 splitting on a silver atomic chain

Cited by 32 publications

References 37 publications

Quantum Mode Selectivity of Plasmon-Induced Water Splitting on Gold Nanoparticles

Quantum Mode Selectivity of Plasmon-Induced Water Splitting on Gold Nanoparticles

Plasmonic Hot-Carrier-Mediated Tunable Photochemical Reactions

Plasmon-Induced Water Splitting on Ag-Alloyed Pt Single-Atom Catalysts

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