Temporal dynamics of confined optical fields can provide valuable insights into light–matter interactions in complex optical systems, going beyond their frequency-domain description. Here, we present a new experimental approach based on interferometric autocorrelation (IAC) that reveals the dynamics of optical near-fields enhanced by collective resonances in periodic metasurfaces. We focus on probing the resonances known as waveguide-plasmon polaritons, which are supported by plasmonic nanoparticle arrays coupled to a slab waveguide. To probe the resonant near-field enhancement, our IAC measurements make use of enhanced two-photon excited luminescence (TPEL) from semiconductor quantum dots deposited on the nanoparticle arrays. Thanks to the incoherent character of TPEL, the measurements are only sensitive to the fundamental optical fields and therefore can reveal clear signatures of their coherent temporal dynamics. In particular, we show that the excitation of a high-Q collective resonance gives rise to interference fringes at time delays as large as 500 fs, much greater than the incident pulse duration (150 fs). Based on these signatures, the basic characteristics of the resonances can be determined, including their Q factors, which are found to exceed 200. Furthermore, the measurements also reveal temporal beating between two different resonances, providing information on their frequencies and their relative contribution to the field enhancement. Finally, we present an approach to enhance the visibility of the resonances hidden in the IAC curves by converting them into spectrograms, which greatly facilitates the analysis and interpretation of the results. Our findings open up new perspectives on time-resolved studies of collective resonances in metasurfaces and other multiresonant systems.

Monocrystalline materials are essential for optoelectronic devices such as solar cells, LEDs, lasers, and transistors to reach the highest performance. Advances in synthetic chemistry now allow for high quality monocrystalline nanomaterials to be grown at low temperature in solution for many materials; however, the realization of extended structures with control over the final 3D geometry still remains elusive. Here, a new paradigm is presented, which relies on epitaxy between monocrystalline nanocube building blocks. The nanocubes are assembled in a predefined pattern and then epitaxially connected at the atomic level by chemical growth in solution, to form monocrystalline nanopatterns on arbitrary substrates. As a first demonstration, it is shown that monocrystalline silver structures obtained with such a process have optical properties and conductivity comparable to single-crystalline silver. This flexible multiscale process may ultimately enable the implementation of monocrystalline materials in optoelectronic devices, raising performance to the ultimate limit.