Direct Observation of a Plasmon-Induced Hot Electron Flow in a Multimetallic Nanostructure
(2020) In Nano Letters p.8220-8228- Abstract
Plasmon hot carriers are interesting for photoredox chemical synthesis but their direct utilization is limited by their ultrafast thermalization. Therefore, they are often transferred to suitable accepting materials that expedite their lifetime. Solid-state photocatalysts are technologically more suitable than their molecular counterparts, but their photophysical processes are harder to follow due to the absence of clear optical fingerprints. Herein, the journey of hot electrons in a solid-state multimetallic photocatalyst is revealed by a combination of ultrafast visible and infrared spectroscopy. Dynamics showed that electrons formed upon silver plasmonic excitation reach the gold catalytic site within 700 fs and the electron flow... (More)
Plasmon hot carriers are interesting for photoredox chemical synthesis but their direct utilization is limited by their ultrafast thermalization. Therefore, they are often transferred to suitable accepting materials that expedite their lifetime. Solid-state photocatalysts are technologically more suitable than their molecular counterparts, but their photophysical processes are harder to follow due to the absence of clear optical fingerprints. Herein, the journey of hot electrons in a solid-state multimetallic photocatalyst is revealed by a combination of ultrafast visible and infrared spectroscopy. Dynamics showed that electrons formed upon silver plasmonic excitation reach the gold catalytic site within 700 fs and the electron flow could also be reversed. Gold is the preferred site until saturation of its 5d band occurs. Silver-plasmon hot electrons increased the rate of nitrophenol reduction 16-fold, confirming the preponderant role of hot electrons in the overall catalytic activity and the importance to follow hot carriers' journeys in solid-state photosystems.
(Less)
- author
- Van Turnhout, Lars ; Hattori, Yocefu ; Meng, Jie ; Zheng, Kaibo LU and Sá, Jacinto
- organization
- publishing date
- 2020
- type
- Contribution to journal
- publication status
- published
- subject
- keywords
- hot-electron, multimetallic system, photocatalysis, Plasmon, ultrafast dynamics
- in
- Nano Letters
- pages
- 8220 - 8228
- publisher
- The American Chemical Society (ACS)
- external identifiers
-
- pmid:33095592
- scopus:85095832230
- ISSN
- 1530-6984
- DOI
- 10.1021/acs.nanolett.0c03344
- language
- English
- LU publication?
- yes
- id
- 672861f5-6e45-4c75-a2af-029bc6cc2568
- date added to LUP
- 2020-11-27 08:27:18
- date last changed
- 2024-08-23 06:47:05
@article{672861f5-6e45-4c75-a2af-029bc6cc2568,
abstract = {{<p>Plasmon hot carriers are interesting for photoredox chemical synthesis but their direct utilization is limited by their ultrafast thermalization. Therefore, they are often transferred to suitable accepting materials that expedite their lifetime. Solid-state photocatalysts are technologically more suitable than their molecular counterparts, but their photophysical processes are harder to follow due to the absence of clear optical fingerprints. Herein, the journey of hot electrons in a solid-state multimetallic photocatalyst is revealed by a combination of ultrafast visible and infrared spectroscopy. Dynamics showed that electrons formed upon silver plasmonic excitation reach the gold catalytic site within 700 fs and the electron flow could also be reversed. Gold is the preferred site until saturation of its 5d band occurs. Silver-plasmon hot electrons increased the rate of nitrophenol reduction 16-fold, confirming the preponderant role of hot electrons in the overall catalytic activity and the importance to follow hot carriers' journeys in solid-state photosystems. </p>}},
author = {{Van Turnhout, Lars and Hattori, Yocefu and Meng, Jie and Zheng, Kaibo and Sá, Jacinto}},
issn = {{1530-6984}},
keywords = {{hot-electron; multimetallic system; photocatalysis; Plasmon; ultrafast dynamics}},
language = {{eng}},
pages = {{8220--8228}},
publisher = {{The American Chemical Society (ACS)}},
series = {{Nano Letters}},
title = {{Direct Observation of a Plasmon-Induced Hot Electron Flow in a Multimetallic Nanostructure}},
url = {{http://dx.doi.org/10.1021/acs.nanolett.0c03344}},
doi = {{10.1021/acs.nanolett.0c03344}},
year = {{2020}},
}