Anomalous ultrafast dynamics of hot plasmonic electrons in nanostructures with hot spots

Harutyunyan, Hayk; Martinson, Alex B. F.; Rosenmann, Daniel; Khorashad, Larousse Khosravi; Besteiro, Lucas V.; Govorov, Alexander O.; Wiederrecht, Gary P.

doi:10.1038/NNANO.2015.165

Anomalous ultrafast dynamics of hot plasmonic electrons in nanostructures with hot spots

Journal Article · Mon Aug 03 00:00:00 EDT 2015 · Nature Nanotechnology

DOI:https://doi.org/10.1038/NNANO.2015.165· OSTI ID:1354829

Harutyunyan, Hayk ^[1]; Martinson, Alex B. F. ^[2]; Rosenmann, Daniel ^[2]; Khorashad, Larousse Khosravi ^[3]; Besteiro, Lucas V. ^[3]; Govorov, Alexander O. ^[3]; Wiederrecht, Gary P. ^[2]

Argonne National Lab. (ANL), Argonne, IL (United States); Emory Univ., Atlanta, GA (United States)
Argonne National Lab. (ANL), Argonne, IL (United States)
Ohio Univ., Athens, OH (United States)

The interaction of light and matter in metallic nanosystems is mediated by the collective oscillation of surface electrons, called plasmons. After excitation, plasmons are absorbed by the metal electrons through inter- and intraband transitions, creating a highly non-thermal distribution of electrons. The electron population then decays through electron-electron interactions, creating a hot electron distribution within a few hundred femtoseconds, followed by a further relaxation via electron-phonon scattering on the timescale of a few pico-seconds. In the spectral domain, hot plasmonic electrons induce changes to the plasmonic resonance of the nanostructure by modifying the dielectric constant of the metal. Here, we report on the observation of anomalously strong changes to the ultrafast temporal and spectral responses of these excited hot plasmonic electrons in hybrid metal/oxide nanostructures as a result of varying the geometry and composition of the nanostructure and the excitation wavelength. In particular, we show a large ultrafast, pulsewidth-limited contribution to the excited electron decay signal in hybrid nanostructures containing hot spots. The intensity of this contribution correlates with the efficiency of the generation of highly excited surface electrons. Using theoretical models, we attribute this effect to the generation of hot plasmonic electrons from hot spots. Finally, we then develop general principles to enhance the generation of energetic electrons through specifically designed plasmonic nanostructures that could be used in applications where hot electron generation is beneficial, such as in solar photocatalysis, photodetectors and nonlinear devices.

View Accepted Manuscript (DOE)

Research Organization:: Argonne National Lab. (ANL), Argonne, IL (United States)

Sponsoring Organization:: Scientific User Facilities Division; USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)

Grant/Contract Number:: AC02-06CH11357

OSTI ID:: 1354829

Alternate ID(s):: OSTI ID: 1370800
OSTI ID: 1386272

Journal Information:: Nature Nanotechnology, Journal Name: Nature Nanotechnology Journal Issue: 9 Vol. 10; ISSN 1748-3387

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

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