TY - JOUR
KW - Surfaces, Coatings and Films
KW - Physical and Theoretical Chemistry
KW - General Energy
KW - Electronic, Optical and Magnetic Materials
AU - Jacob Pettine
AU - David Nesbitt
AB - Concentrated optical fields in plasmonic metal nanostructures generate high densities of excited charge carriers, which can be extracted or emitted into surrounding media for a variety of physical, chemical, and biological applications. However, the detailed geometry- and field-dependent photoexcitation mechanisms determining the spatial, temporal, vector momentum, and energy distributions of these carriers in nanoplasmonic systems are still under investigation. Gathering insights from recent studies with nanoscale spatial, femtosecond temporal, and/or angle-resolved momentum resolution, we survey several emerging methods for geometrical design and active optical control of nanoplasmonic hot carrier excitation and emission distributions. Uniform dielectric coatings, for example, provide a means of blocking or regulating hot carrier emission, while nonuniform coatings can provide nanoscale spatial selectivity. Nanoscale site selectivity can also be actively controlled on ultrafast time scales by optically addressing different polarization- and/or frequency-sensitive hot spots, particularly with sharp nanocathode geometries such as nanostars. Furthermore, the nanoplasmonic geometry and the corresponding internal vs surface electric field distributions significantly influence the fundamental bulk- vs surface-like photoexcitation mechanisms, with dramatic effects on the excited carrier distributions and dynamics. Finally, energy-resolved pump–probe photoemission studies clarify the tens-of-femtosecond time scales relevant for hot carrier extraction.
BT - The Journal of Physical Chemistry C
DA - 2022-08
DO - 10.1021/acs.jpcc.2c03425
N2 - Concentrated optical fields in plasmonic metal nanostructures generate high densities of excited charge carriers, which can be extracted or emitted into surrounding media for a variety of physical, chemical, and biological applications. However, the detailed geometry- and field-dependent photoexcitation mechanisms determining the spatial, temporal, vector momentum, and energy distributions of these carriers in nanoplasmonic systems are still under investigation. Gathering insights from recent studies with nanoscale spatial, femtosecond temporal, and/or angle-resolved momentum resolution, we survey several emerging methods for geometrical design and active optical control of nanoplasmonic hot carrier excitation and emission distributions. Uniform dielectric coatings, for example, provide a means of blocking or regulating hot carrier emission, while nonuniform coatings can provide nanoscale spatial selectivity. Nanoscale site selectivity can also be actively controlled on ultrafast time scales by optically addressing different polarization- and/or frequency-sensitive hot spots, particularly with sharp nanocathode geometries such as nanostars. Furthermore, the nanoplasmonic geometry and the corresponding internal vs surface electric field distributions significantly influence the fundamental bulk- vs surface-like photoexcitation mechanisms, with dramatic effects on the excited carrier distributions and dynamics. Finally, energy-resolved pump–probe photoemission studies clarify the tens-of-femtosecond time scales relevant for hot carrier extraction.
PB - American Chemical Society (ACS)
PY - 2022
T2 - The Journal of Physical Chemistry C
TI - Emerging Methods for Controlling Hot Carrier Excitation and Emission Distributions in Nanoplasmonic Systems
SN - 1932-7447, 1932-7455
ER -