Journal
NANO LETTERS
Volume 21, Issue 18, Pages 7512-7518Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acs.nanolett.1c01639
Keywords
Electrochromism; localized surface plasmon resonance; plasmonic nanocubes; quantum capacitance; Fermi energy
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Funding
- National Research Foundation of Korea (NRF) - Korea government (MSIT) [NRF-2021R1A2C3010083, NRF-2017R1A5A1015365]
- BioNano Health-Guard Research Center - Ministry of Science and ICT (MSIT) of Korea as Global Frontier Project [HGUARD_2013M3A6B2078947]
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This study observed three distinct electrochromic behaviors of gold nanocubes with a wide potential range through in situ dark-field electrospectroscopy, with the nanocubes showing a faster frequency shift under highly negative potential. This unexpected phenomenon opens up the possibility of largely tunable electrochromic LSPR shifts, and is attributed to the material-specific quantum mechanical electronic structures of the plasmonic materials.
Plasmonic electrochromism, a change in the localized surface plasmon resonance (LSPR) with an applied electric potential, has been attracting increasing attention for the development of spectroscopic tools or optoelectronic systems. There is a consensus on the mechanism of plasmonic electrochromism based on the classical capacitor and the Drude model. However, the electrochromic behaviors of metallic nanoparticles in narrow optical windows have been demonstrated only with small monotonic LSPR shifts, which limits the use of the electrochromism. Here, we observed three distinct electrochromic behaviors of gold nanocubes with a wide potential range through in situ dark-field electrospectroscopy. Interestingly, the nanocubes show a faster frequency shift under the highly negative potential, and this opens the possibility of largely tunable electrochromic LSPR shifts. The reversibility of the electrochemical switching with these cubes are also shown. We attribute this unexpected change beyond classical understandings to the material-specific quantum mechanical electronic structures of the plasmonic materials.
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