The
nonlinear optical (NLO) properties of π-conjugated polydiacetylene
(PDA) nanotubes (NTs) were enhanced by the localized surface plasmon
resonance (LSPR) effect from gold (Au) nanoparticles (NPs). Three
types of PDA NTs hybridized with Au NPs have been fabricated successfully,
i.e., Au NPs deposited on the outer surface (outer type), on both
outer and inner surfaces (outer/inner type), and on the inner surface
(inner type). Third-order NLO susceptibility, χ(3)(ω), has been evaluated by transient transmission spectroscopy
and spectroscopic ellipsometry, and then structural correlations of
these optical data were discussed in detail. χ(3)(ω) was compared by newly proposing a figure of merit (FOM),
which may reflect the generation efficiency for χ(3)(ω) based on the intensity of the excitonic absorption peak
in PDA NTs because the NLO properties of PDA were originated from
excitons. As a result, the outer/inner type has numerically provided
the maximum of FOM by a factor of about 5 compared with original PDA
NTs. The gap mode effect in a metal–insulator–metal-like
nanostructure as well as the LSPR effect would be responsible for
the increase in the FOM of the outer/inner type. Consequently, hybridized
PDA NTs would open a new field toward all-optical and photonic device
applications.