The interaction between light and metal nanoparticles enables investigations of microscopic phenomena on nanometer length and ultrashort time scales, benefiting from strong confinement and enhancement of the optical field. However, the ultrafast dynamics of these nanoparticles are primarily investigated by multiphoton photoluminescence on picoseconds or photoemission on femtoseconds independently. Here, we presented two-photon photoluminescence (TPPL) measurements on individual Au nanobipyramids (AuNP) to reveal their ultrafast dynamics by two-pulse excitation on a global time scale ranging from sub-femtosecond to tens of picoseconds. Two-orders-of-magnitude photoluminescence enhancement, namely super interference fringes, has been demonstrated on tens of femtoseconds. Power-dependent measurements uncovered the transform of the nonlinearity from 1 to 2 when the interpulse delay varied from tens of femtoseconds to tens of picoseconds. We proved that the real intermediate state plays a critical role in the observed phenomena, supported by numerical simulations with a three eigenstates model and further experiments on Au nanospheres with different diameters. The crucial parameters, including the dephasing time, the radiative rate, and the coupling between different states, have been estimated using numerical simulations. Our results provide insight into the role of intermediate states in the ultrafast dynamics of noble metal nanoparticles. The giant photoluminescence in super interference fringes enables potential practical applications in imaging, sensing, and nanophotonics.
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