Electron heating and thermal relaxation of gold nanorods revealed by two-dimensional electronic spectroscopy

Aude Lietard, Cho Shuen Hsieh, Hanju Rhee, Minhaeng Cho

Research output: Contribution to journalArticlepeer-review

21 Citations (Scopus)

Abstract

To elucidate the complex interplay between the size and shape of gold nanorods and their electronic, photothermal, and optical properties for molecular imaging, photothermal therapy, and optoelectronic devices, it is a prerequisite to characterize ultrafast electron dynamics in gold nanorods. Time-resolved transient absorption (TA) studies of plasmonic electrons in various nanostructures have revealed the time scales for electron heating, lattice vibrational excitation, and phonon relaxation processes in condensed phases. However, because linear spectroscopic and time-resolved TA signals are vulnerable to inhomogeneous line-broadening, pure dephasing and direct electron heating effects are difficult to observe. Here we show that femtosecond two-dimensional electronic spectroscopy, with its unprecedented time resolution and phase sensitivity, can be used to collect direct experimental evidence for ultrafast electron heating, anomalously strong coherent and transient electronic plasmonic responses, and homogenous dephasing processes resulting from electron-vibration couplings even for polydisperse gold nanorods.

Original languageEnglish
Article number891
JournalNature communications
Volume9
Issue number1
DOIs
Publication statusPublished - 2018 Dec 1

Bibliographical note

Funding Information:
This work was supported by IBS-R023-D1. H.R. thanks financial support from IBS CMSD (PB2016005) and KBSI (E37300). The 2DES experimental data presented here were measured using the Femtosecond Multi-dimensional Laser Spectroscopic System (FMLS) at the Korea Basic Science Institute (KBSI). We thank Heejeong Kim, Dr. Jongbok Seo, and Dr. Chiyong Eom for providing LHC chromatophores of photosynthetic bacteria whose 2DES spectra are used to compare with those of AuNRs in the Supplementary Information.

Publisher Copyright:
© 2018 The Author(s) 2018.

ASJC Scopus subject areas

  • General
  • General Physics and Astronomy
  • General Chemistry
  • General Biochemistry,Genetics and Molecular Biology

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