Quantifying hot carrier and thermal contributions in plasmonic photocatalysis

Zhou, Linan; Swearer, Dayne F.; Zhang, Chao; Robatjazi, Hossein; Zhao, Hangqi; Henderson, Luke A.; Dong, Liangliang; Christopher, Phillip; Carter, Emily A.; Nordlander, Peter; Halas, Naomi J.

doi:10.1126/science.aat6967

Cited by 891 publications

(1,067 citation statements)

References 45 publications

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“…At this time a large body of work has been accumulated on the process of charge transfer of hot carriers from the plasmonic metals into semiconductors or dielectrics [27][28][29][30][31][32][33][34][35][36][37][38]. The results (in terms of the injection efficiency) have varied between the different groups, sometimes by orders of magnitude and more.…”

Section: Introductionmentioning

confidence: 99%

Fundamental limits of hot carrier injection from metal in nanoplasmonics

2019

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Evolution of the non-equilibrium carriers excited in the process of decay of surface plasmon polaritons (SPPs) in metal is described for each step -from the carrier generation to their extraction from the metal. The relative importance of various carrier generating mechanism is discussed. It is shown that both carrier generation and their decay are inherently quantum processes as for realistic illumination conditions no more than a single SPP per nanoparticle exists at a given time. As a result, the distribution of nonequilibrium carriers cannot be described by a single temperature. It is also shown that the originally excited carriers that have not undergone a single electron-electron scattering event, are practically the only ones that contribute to the injection. The role of the momentum conservation in the carrier extraction is discussed and it is shown that if all the momentum conservation rules are relaxed, it is the density of states in the semiconductor/dielectric that determines the ultimate injection efficiency. A set of recommendations aimed at improving the efficiency of plasmonic-assisted photodetection and (to a lesser degree) photocatalysis is made in the end.

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Section: Introductionmentioning

confidence: 99%

Fundamental limits of hot carrier injection from metal in nanoplasmonics

2019

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“…It is also worthy to mention that, in agreement with our previous results, laser‐induced thermal damage of the sample did not occur under weak laser intensity (30 µW). We do not observe any signs of thermal damage from local thermal contribution, such as broad carbon peaks. Figure b shows that the oxidized/reduced ratio varies less with temperature (22–26%) than it does with the distance (21–47%).…”

Section: Resultsmentioning

confidence: 55%

Nanoscale Surface Redox Chemistry Triggered by Plasmon‐Generated Hot Carriers

Yin

Lan

Goubert

et al. 2019

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Direct photoexcitation of charges at a plasmonic metal hotspot produces energetic carriers that are capable of performing photocatalysis in the visible spectrum. However, the mechanisms of generation and transport of hot carriers are still not fully understood and under intense investigation because of their potential technological importance. Here, spectroscopic evidence proves that the reduction of dye molecules tethered to a Au(111) surface can be triggered by plasmonic carriers via a tunneling mechanism, which results in anomalous Raman intensity fluctuations. Tip‐enhanced Raman spectroscopy (TERS) helps to correlate Raman intensity fluctuations with temperature and with properties of the molecular spacer. In combination with electrochemical surface‐enhanced Raman spectroscopy, TERS results show that plasmon‐induced energetic carriers can directly tunnel to the dye through the spacer. This organic spacer chemically isolates the adsorbate from the metal but does not block photo‐induced redox reactions, which offers new possibilities for optimizing plasmon‐induced photocatalytic systems.

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“…[1][2][3] Photo-electrochemical (PEC) water splitting has been regarded as one of the promising approaches for sustainable energy conversion, mimicking natural photosynthesis. [1][2][3] Photo-electrochemical (PEC) water splitting has been regarded as one of the promising approaches for sustainable energy conversion, mimicking natural photosynthesis.…”

Section: Introductionmentioning

confidence: 99%

3D Porous Pyramid Heterostructure Array Realizing Efficient Photo‐Electrochemical Performance

Cao

Hou

et al. 2019

Advanced Energy Materials

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Direct photo‐electrochemical (PEC) water splitting is of great practical interest for developing a sustainable energy systems, but remains a big challenge owing to sluggish charge separation, low efficiency, and poor stability. Herein, a 3D porous In2O3/In2S3 pyramid heterostructure array on a fluorine‐doped tin oxide substrate is fabricated by an ion exchange–induced synthesis strategy. Based on the synergistic structural and electronic modulations from density functional theory calculations and experimental observations, 3D porous In2O3/In2S3 photoanode by the protective layer delivers a low onset potential of ≈0.02 V versus reversible hydrogen electrode (RHE), the highest photocurrent density of 8.2 mA cm−2 at 1.23 V versus RHE among all the In2S3 photoanodes reported to date, an incident photon‐to‐current efficiency of 76% at 400 nm, and high stability over 20 h for PEC water splitting are reported. This work provides an alternative promising prototype for the design and construction of novel heterostructures in robust PEC water splitting applications.

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Quantifying hot carrier and thermal contributions in plasmonic photocatalysis

Cited by 891 publications

References 45 publications

Fundamental limits of hot carrier injection from metal in nanoplasmonics

Fundamental limits of hot carrier injection from metal in nanoplasmonics

Nanoscale Surface Redox Chemistry Triggered by Plasmon‐Generated Hot Carriers

3D Porous Pyramid Heterostructure Array Realizing Efficient Photo‐Electrochemical Performance

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