TY - JOUR
T1 - Origin of plasmon lineshape and enhanced hot electron generation in metal nanoparticles
AU - You, Xinyuan
AU - Ramakrishna, S.
AU - Seideman, Tamar
N1 - Funding Information:
The authors thank the Atomic, Molecular, and Optics Sciences (AMOS) of the Department of Energy (Award Number DE-FG02-04ER15612/0013) and the National Science Foundation (Award Number CHE-1465201) for support.
Publisher Copyright:
© 2017 American Chemical Society.
PY - 2018/1/4
Y1 - 2018/1/4
N2 - Plasmon-generated hot carriers are currently being studied intensively for their role in enhancing the efficiency of photovoltaic and photocatalytic processes. Theoretical studies of the hot electrons subsystem have generated insight, but we show that a unified quantum-mechanical treatment of the plasmon and hot electrons reveals new physical phenomena. Instead of a unidirectional energy transfer process in Landau damping, back energy transfer is predicted in small metal nanoparticles (MNPs) within a model-Hamiltonian approach. As a result, the single Lorentzian plasmonic line shape is modulated by a multipeak structure, whose individual line width provides a direct way to probe the electronic dephasing. More importantly, the hot electron generation can be enhanced greatly by matching the incident energy to the peaks of the modulated line shape.
AB - Plasmon-generated hot carriers are currently being studied intensively for their role in enhancing the efficiency of photovoltaic and photocatalytic processes. Theoretical studies of the hot electrons subsystem have generated insight, but we show that a unified quantum-mechanical treatment of the plasmon and hot electrons reveals new physical phenomena. Instead of a unidirectional energy transfer process in Landau damping, back energy transfer is predicted in small metal nanoparticles (MNPs) within a model-Hamiltonian approach. As a result, the single Lorentzian plasmonic line shape is modulated by a multipeak structure, whose individual line width provides a direct way to probe the electronic dephasing. More importantly, the hot electron generation can be enhanced greatly by matching the incident energy to the peaks of the modulated line shape.
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U2 - 10.1021/acs.jpclett.7b03126
DO - 10.1021/acs.jpclett.7b03126
M3 - Article
C2 - 29256610
AN - SCOPUS:85040104077
VL - 9
SP - 141
EP - 145
JO - Journal of Physical Chemistry Letters
JF - Journal of Physical Chemistry Letters
SN - 1948-7185
IS - 1
ER -
