Monitoring plasmonic hot-carrier chemical reactions at the single particle level

TY - JOUR

T1 - Monitoring plasmonic hot-carrier chemical reactions at the single particle level

AU - Simoncelli, Sabrina

AU - Pensa, Evangelina L.

AU - Brick, Thomas

AU - Gargiulo, Julian

AU - Lauri, Alberto

AU - Cambiasso, Javier

AU - Li, Yi

AU - Maier, Stefan A.

AU - Cortés, Emiliano

PY - 2018/10/24

Y1 - 2018/10/24

N2 - Plasmon excitation in metal nanoparticles triggers the generation of highly energetic charge carriers that, when properly manipulated and exploited, can mediate chemical reactions. Single-particle techniques are key to unearthing the underlying mechanisms of hot-carrier generation, transport and injection, as well as to disentangling the role of the temperature increase and the enhanced near-field at the nanoparticle-molecule interface. Gaining nanoscopic insight into these processes and their interplay could aid in the rational design of plasmonic photocatalysts. Here, we present three different approaches to monitor hot-carrier reactivity at the single-particle level. We use a combination of dark-field microscopy and photoelectrochemistry to track a hot-hole driven reaction on a single Au nanoparticle. We image hot-electron reactivity with sub-particle spatial resolution using nanoscopy techniques. Finally, we push the limits by looking for a hot-electron induced chemical reaction that generates a fluorescent product, which should enable imaging plasmonic photocatalysis at the single-particle and single-molecule levels.

AB - Plasmon excitation in metal nanoparticles triggers the generation of highly energetic charge carriers that, when properly manipulated and exploited, can mediate chemical reactions. Single-particle techniques are key to unearthing the underlying mechanisms of hot-carrier generation, transport and injection, as well as to disentangling the role of the temperature increase and the enhanced near-field at the nanoparticle-molecule interface. Gaining nanoscopic insight into these processes and their interplay could aid in the rational design of plasmonic photocatalysts. Here, we present three different approaches to monitor hot-carrier reactivity at the single-particle level. We use a combination of dark-field microscopy and photoelectrochemistry to track a hot-hole driven reaction on a single Au nanoparticle. We image hot-electron reactivity with sub-particle spatial resolution using nanoscopy techniques. Finally, we push the limits by looking for a hot-electron induced chemical reaction that generates a fluorescent product, which should enable imaging plasmonic photocatalysis at the single-particle and single-molecule levels.

UR - http://www.scopus.com/inward/record.url?scp=85066476515&partnerID=8YFLogxK

U2 - 10.1039/c8fd00138c

DO - 10.1039/c8fd00138c

M3 - Article

AN - SCOPUS:85066476515

SN - 1359-6640

VL - 214

SP - 73

EP - 87

JO - Faraday Discussions

JF - Faraday Discussions

ER -