Quantifying Wavelength-Dependent Plasmonic Hot Carrier Energy Distributions at Metal/Semiconductor Interfaces

ACS Nano
Yun YuKatherine A Willets

Abstract

Hot carriers generated from the nonradiative decay of localized surface plasmons are capable of driving charge-transfer reactions at the surfaces of metal nanostructures. Photocatalytic devices utilizing plasmonic hot carriers are often based on metal nanoparticle/semiconductor heterostructures owing to their efficient electron-hole separation ability. The rapid thermalization of hot carriers generated at the metal nanoparticles yields a distribution of carrier energies that determines the capability of the photocatalytic device to drive redox reactions. Here, we quantify the thermalized hot carrier energy distribution generated at Au/TiO2 nanostructures using wavelength-dependent scanning electrochemical microscopy and a series of molecular probes with different redox potentials. We determine the quantum efficiencies and oxidizing power of the hot carriers from wavelength-dependent reaction rates and photocurrent across the metal/semiconductor interface. The wavelength-dependent reaction efficiency tracks the surface plasmon resonance spectrum of the Au nanoparticles, showing that the reaction is facilitated by plasmon excitation, while the responses from molecules with different redox potentials shed light on the energy distr...Continue Reading

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Citations

Apr 1, 2020·Nanoscale Horizons : the Home for Rapid Reports of Exceptional Significance in Nanoscience and Nanotechnolgy·Tetsu Tatsuma, Hiroyasu Nishi
Jun 15, 2020·The Journal of Chemical Physics·Haibin TangNianqiang Wu
Dec 3, 2020·Nanomaterials·Ruben F HamansAndrea Baldi
May 12, 2021·Proceedings of the National Academy of Sciences of the United States of America·Linan ZhouNaomi J Halas
May 13, 2021·Advanced Materials·Yuchao ZhangWei David Wei
Jul 29, 2021·Physical Chemistry Chemical Physics : PCCP·Amanu Lakachew Nigusie, Masaki Ujihara
Aug 21, 2019·Accounts of Chemical Research·Julian GargiuloEmiliano Cortés
Jul 31, 2019·ACS Nano·Ujjal BhattacharjeeDavid J Masiello
Feb 7, 2020·Journal of the American Chemical Society·Larousse Khosravi KhorashadAlexander O Govorov
Jul 4, 2020·Journal of the American Chemical Society·Yue QiRichard P Van Duyne
May 7, 2020·Nano Letters·Yawei LiuTianquan Lian
Dec 10, 2020·ACS Nano·James L BrooksRenee R Frontiera
Dec 15, 2020·ACS Nano·Emiliano CortésPrineha Narang
Sep 4, 2021·ACS Applied Materials & Interfaces·Ehsan VahidzadehKarthik Shankar
Sep 18, 2021·Chemical Society Reviews·Jian ZhaoJinghong Li

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