Observation and Analysis of Incoherent Second-Harmonic Generation in Gold Nanoclusters with Six Atoms
2020
We
report the first-hyperpolarizability, β(−2ω;ω,ω), of gold nanoclusters
Au6(GSH)2(MPA)2 having six gold atoms
capped by 3-mercaptopropionic acid and glutathione (GSH) that is unprecedented.
Here, we used the concentration of 2.1 × 1016 nanoclusters/mL
in experiments to determine β(−2ω;ω,ω),
applying the hyper-Rayleigh scattering technique by using a 1064 nm
laser and analyzing the scattered light at 532 nm. The measured hyperpolarizability
is found to be β(−2ω;ω,ω) = 760 ×
10–30 esu. The static hyperpolarizability, β(0)
= 300 × 10–30 esu, was determined by using
a two-level model approximation. The large β(−2ω;ω,ω)
is attributed to the quantum confinement effect and the geometry of
the nanoclusters that have no inversion symmetry. Computer calculations
based on the density functional theory method were performed, and
the numerical results present the same order of magnitude than the
experimental values.
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